Articles | Volume 11, issue 1
https://doi.org/10.5194/amt-11-49-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-11-49-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
08 Jan 2018
Research article |
| 08 Jan 2018
| 08 Jan 2018
A reference data set for validating vapor pressure measurement techniques: homologous series of polyethylene glycols
Ulrich K. Krieger
CORRESPONDING AUTHOR
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Franziska Siegrist
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Claudia Marcolli
Institute for Atmospheric and Climate Science, ETH Zürich, 8092 Zürich, Switzerland
Eva U. Emanuelsson
Department of Chemistry, Aarhus University, 8000 Aarhus, Denmark
Freya M. Gøbel
Department of Chemistry, Aarhus University, 8000 Aarhus, Denmark
Merete Bilde
Department of Chemistry, Aarhus University, 8000 Aarhus, Denmark
Aleksandra Marsh
School of Chemistry, University of Bristol, BS8 1TS Bristol, UK
Jonathan P. Reid
School of Chemistry, University of Bristol, BS8 1TS Bristol, UK
Andrew J. Huisman
Chemistry Department, Union College, Schenectady, NY 12308, USA
Ilona Riipinen
Department of Environmental Science and Analytical Chemistry, Stockholm University, 106 91 Stockholm, Sweden
Noora Hyttinen
Department of Chemistry, University of Helsinki, 00014 Helsinki, Finland
Nanna Myllys
Department of Physics, University of Helsinki, 00014 Helsinki, Finland
Theo Kurtén
Department of Chemistry, University of Helsinki, 00014 Helsinki, Finland
Thomas Bannan
Centre for Atmospheric Sciences, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
Carl J. Percival
Centre for Atmospheric Sciences, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
David Topping
Centre for Atmospheric Sciences, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
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The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remain below an hour for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
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Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
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Mehrnoush M. Fard, Ulrich K. Krieger, and Thomas Peter
Atmos. Chem. Phys., 18, 13511–13530, https://doi.org/10.5194/acp-18-13511-2018, https://doi.org/10.5194/acp-18-13511-2018, 2018
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Atmospheric aerosol particles may undergo liquid–liquid phase separation (LLPS) when exposed to varying relative humidity, with an aqueous organic phase enclosing an aqueous inorganic phase below a threshold of relative humidity. Brown carbon (BrC) compounds will redistribute to the organic phase upon LLPS. We use numerical modeling to study the shortwave radiative impact of LLPS containing BrC and conclude that it is not significant for atmospheric aerosol.
Adam W. Birdsall, Ulrich K. Krieger, and Frank N. Keutsch
Atmos. Meas. Tech., 11, 33–47, https://doi.org/10.5194/amt-11-33-2018, https://doi.org/10.5194/amt-11-33-2018, 2018
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Sandra Bastelberger, Ulrich K. Krieger, Beiping Luo, and Thomas Peter
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We present quantitative condensed-phase diffusivity measurements of a volatile organic (tetraethylene glycol) in highly viscous single aerosol particles (aqueous sucrose). The condensed-phase diffusivity exhibits a strong temperature and humidity dependence. Our results suggest that diffusion limitations of volatile organics in highly viscous organic aerosol may severely impact gas–particle partitioning under cold and dry conditions.
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Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Erika Kienast-Sjögren, Christian Rolf, Patric Seifert, Ulrich K. Krieger, Bei P. Luo, Martina Krämer, and Thomas Peter
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D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
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S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
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G. Ganbavale, C. Marcolli, U. K. Krieger, A. Zuend, G. Stratmann, and T. Peter
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A. Cirisan, B. P. Luo, I. Engel, F. G. Wienhold, M. Sprenger, U. K. Krieger, U. Weers, G. Romanens, G. Levrat, P. Jeannet, D. Ruffieux, R. Philipona, B. Calpini, P. Spichtinger, and T. Peter
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A. J. Huisman, U. K. Krieger, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 13, 6647–6662, https://doi.org/10.5194/acp-13-6647-2013, https://doi.org/10.5194/acp-13-6647-2013, 2013
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
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Anna J. Miller, Christopher Fuchs, Fabiola Ramelli, Huiying Zhang, Nadja Omanovic, Robert Spirig, Claudia Marcolli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
EGUsphere, https://doi.org/10.5194/egusphere-2024-3230, https://doi.org/10.5194/egusphere-2024-3230, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We analyzed the ability of silver iodide particles to form ice crystals in naturally-occurring liquid clouds below 0 °C and found that ≈0.1−1 % of particles nucleate ice, with a negative dependence on temperature. Contextualizing our results with previous laboratory studies, we help to bridge the gap between laboratory and field experiments and which also helps to inform future cloud seeding projects.
Yuanyuan Luo, Lauri Franzon, Jiangyi Zhang, Nina Sarnela, Neil M. Donahue, Theo Kurtén, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2024-3323, https://doi.org/10.5194/egusphere-2024-3323, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study explores the formation of accretion products from reactions involving highly reactive compounds, Criegee intermediates. We focused on three types of terpenes, common in nature, and their reactions with specific acids. Our findings reveal that these reactions efficiently produce expected compounds. This research enhances our understanding of how these reactions affect air quality and climate by contributing to aerosol formation, crucial for atmospheric chemistry.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Zijun Li, Angela Buchholz, and Noora Hyttinen
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Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2838, https://doi.org/10.5194/egusphere-2024-2838, 2024
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We model the CCN activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updrafts.
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
Atmos. Chem. Phys., 24, 9459–9473, https://doi.org/10.5194/acp-24-9459-2024, https://doi.org/10.5194/acp-24-9459-2024, 2024
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∆3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecule (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and their potential to impact atmospheric aerosols.
Olivia Mae Jackson, Aristeidis Voliotis, Thomas J. Bannan, Simon P. O'Meara, Gordon McFiggans, Dave Johnson, and Hugh Coe
EGUsphere, https://doi.org/10.5194/egusphere-2024-2380, https://doi.org/10.5194/egusphere-2024-2380, 2024
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The paper details a method of measuring volatility of pesticides using chemical ionisation mass spectrometry (CIMS) to calculate vapour pressure. This was then compared to current literature values and commonly used models. The exact nature of the literature values often remain uncertain due to being hidden in industrial reports. The results show that the method used primarily matches current literature values and any difference can be explained by method differences either in the methodology.
Sebastian Diez, Stuart Lacy, Hugh Coe, Josefina Urquiza, Max Priestman, Michael Flynn, Nicholas Marsden, Nicholas A. Martin, Stefan Gillott, Thomas Bannan, and Pete M. Edwards
Atmos. Meas. Tech., 17, 3809–3827, https://doi.org/10.5194/amt-17-3809-2024, https://doi.org/10.5194/amt-17-3809-2024, 2024
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In this paper we present an overview of the QUANT project, which to our knowledge is one of the largest evaluations of commercial sensors to date. The objective was to evaluate the performance of a range of commercial products and also to nourish the different applications in which these technologies can offer relevant information.
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
EGUsphere, https://doi.org/10.5194/egusphere-2024-1459, https://doi.org/10.5194/egusphere-2024-1459, 2024
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The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remain below an hour for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
Liine Heikkinen, Daniel G. Partridge, Sara Blichner, Wei Huang, Rahul Ranjan, Paul Bowen, Emanuele Tovazzi, Tuukka Petäjä, Claudia Mohr, and Ilona Riipinen
Atmos. Chem. Phys., 24, 5117–5147, https://doi.org/10.5194/acp-24-5117-2024, https://doi.org/10.5194/acp-24-5117-2024, 2024
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The organic vapor condensation with water vapor (co-condensation) in rising air below clouds is modeled in this work over the boreal forest because the forest air is rich in organic vapors. We show that the number of cloud droplets can increase by 20 % if considering co-condensation. The enhancements are even larger if the air contains many small, naturally produced aerosol particles. Such conditions are most frequently met in spring in the boreal forest.
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
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Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Dominic Heslin-Rees, Peter Tunved, Johan Ström, Roxana Cremer, Paul Zieger, Ilona Riipinen, Annica M. L. Ekman, Konstantinos Eleftheriadis, and Radovan Krejci
Atmos. Chem. Phys., 24, 2059–2075, https://doi.org/10.5194/acp-24-2059-2024, https://doi.org/10.5194/acp-24-2059-2024, 2024
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Light-absorbing atmospheric particles (e.g. black carbon – BC) exert a warming effect on the Arctic climate. We show that the amount of particle light absorption decreased from 2002 to 2023. We conclude that in addition to reductions in emissions of BC, wet removal plays a role in the long-term reduction of BC in the Arctic, given the increase in surface precipitation experienced by air masses arriving at the site. The potential impact of biomass burning events is shown to have increased.
Alexander T. Archibald, Bablu Sinha, Maria Russo, Emily Matthews, Freya Squires, N. Luke Abraham, Stephane Bauguitte, Thomas Bannan, Thomas Bell, David Berry, Lucy Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Ben I. Moat, Katie Read, Chris Reed, Malcolm Roberts, Reinhard Schiemann, David Schroeder, Tim Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Ming-Xi Yang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-405, https://doi.org/10.5194/essd-2023-405, 2024
Revised manuscript accepted for ESSD
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Here we present an overview of the data generated as part of the North Atlantic Climate System Integrated Studies (ACSIS) programme which are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA, www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC, bodc.ac.uk). ACSIS data cover the full North Atlantic System comprising: the North Atlantic Ocean, the atmosphere above it including its composition, Arctic Sea Ice and the Greenland Ice Sheet.
Markku Kulmala, Anna Lintunen, Hanna Lappalainen, Annele Virtanen, Chao Yan, Ekaterina Ezhova, Tuomo Nieminen, Ilona Riipinen, Risto Makkonen, Johanna Tamminen, Anu-Maija Sundström, Antti Arola, Armin Hansel, Kari Lehtinen, Timo Vesala, Tuukka Petäjä, Jaana Bäck, Tom Kokkonen, and Veli-Matti Kerminen
Atmos. Chem. Phys., 23, 14949–14971, https://doi.org/10.5194/acp-23-14949-2023, https://doi.org/10.5194/acp-23-14949-2023, 2023
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To be able to meet global grand challenges, we need comprehensive open data with proper metadata. In this opinion paper, we describe the SMEAR (Station for Measuring Earth surface – Atmosphere Relations) concept and include several examples (cases), such as new particle formation and growth, feedback loops and the effect of COVID-19, and what has been learned from these investigations. The future needs and the potential of comprehensive observations of the environment are summarized.
Noora Hyttinen
Atmos. Chem. Phys., 23, 13809–13817, https://doi.org/10.5194/acp-23-13809-2023, https://doi.org/10.5194/acp-23-13809-2023, 2023
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Water activity in aerosol particles describes how particles respond to variations in relative humidity. Here, water activities were calculated for a set of 80 salts that may be present in aerosol particles using a state-of-the-art quantum-chemistry-based method. The effect of the dissociated salt on water activity varies with both the cation and anion. Most of the studied salts increase water uptake compared to pure water-soluble organic particles.
Dimitri Castarède, Zoé Brasseur, Yusheng Wu, Zamin A. Kanji, Markus Hartmann, Lauri Ahonen, Merete Bilde, Markku Kulmala, Tuukka Petäjä, Jan B. C. Pettersson, Berko Sierau, Olaf Stetzer, Frank Stratmann, Birgitta Svenningsson, Erik Swietlicki, Quynh Thu Nguyen, Jonathan Duplissy, and Erik S. Thomson
Atmos. Meas. Tech., 16, 3881–3899, https://doi.org/10.5194/amt-16-3881-2023, https://doi.org/10.5194/amt-16-3881-2023, 2023
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Clouds play a key role in Earth’s climate by influencing the surface energy budget. Certain types of atmospheric aerosols, called ice-nucleating particles (INPs), induce the formation of ice in clouds and, thus, often initiate precipitation formation. The Portable Ice Nucleation Chamber 2 (PINCii) is a new instrument developed to study ice formation and to conduct ambient measurements of INPs, allowing us to investigate the sources and properties of the atmospheric aerosols that can act as INPs.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362, https://doi.org/10.5194/acp-23-7347-2023, https://doi.org/10.5194/acp-23-7347-2023, 2023
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
Zijun Li, Noora Hyttinen, Miika Vainikka, Olli-Pekka Tikkasalo, Siegfried Schobesberger, and Taina Yli-Juuti
Atmos. Chem. Phys., 23, 6863–6877, https://doi.org/10.5194/acp-23-6863-2023, https://doi.org/10.5194/acp-23-6863-2023, 2023
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The saturation vapor pressure (psat) of low-volatility organic compounds (LVOCs) governs their partitioning between the gas and particle phases. To estimate the psat of selected LVOCs, we performed particle evaporation measurements in a residence time chamber at a temperature setting relevant to atmospheric aerosol formation and conducted state-of-the-art computational calculations. We found good agreement between the experimentally measured and model-estimated psat values for most LVOCs.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023, https://doi.org/10.5194/acp-23-5993-2023, 2023
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We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Anand Kumar, Kristian Klumpp, Chen Barak, Giora Rytwo, Michael Plötze, Thomas Peter, and Claudia Marcolli
Atmos. Chem. Phys., 23, 4881–4902, https://doi.org/10.5194/acp-23-4881-2023, https://doi.org/10.5194/acp-23-4881-2023, 2023
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Smectites are a major class of clay minerals that are ice nucleation (IN) active. They form platelets that swell or even delaminate in water by intercalation of water between their layers. We hypothesize that at least three smectite layers need to be stacked together to host a critical ice embryo on clay mineral edges and that the larger the surface edge area is, the higher the freezing temperature. Edge sites on such clay particles play a crucial role in imparting IN ability to such particles.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
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Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Kristian Klumpp, Claudia Marcolli, Ana Alonso-Hellweg, Christopher H. Dreimol, and Thomas Peter
Atmos. Chem. Phys., 23, 1579–1598, https://doi.org/10.5194/acp-23-1579-2023, https://doi.org/10.5194/acp-23-1579-2023, 2023
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The prerequisites of a particle surface for efficient ice nucleation are still poorly understood. This study compares the ice nucleation activity of two chemically identical but morphologically different minerals (kaolinite and halloysite). We observe, on average, not only higher ice nucleation activities for halloysite than kaolinite but also higher diversity between individual samples. We identify the particle edges as being the most likely site for ice nucleation.
Nikou Hamzehpour, Claudia Marcolli, Sara Pashai, Kristian Klumpp, and Thomas Peter
Atmos. Chem. Phys., 22, 14905–14930, https://doi.org/10.5194/acp-22-14905-2022, https://doi.org/10.5194/acp-22-14905-2022, 2022
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Playa surfaces in Iran that emerged through Lake Urmia (LU) desiccation have become a relevant dust source of regional relevance. Here, we identify highly erodible LU playa surfaces and determine their physicochemical properties and mineralogical composition and perform emulsion-freezing experiments with them. We find high ice nucleation activities (up to 250 K) that correlate positively with organic matter and clay content and negatively with pH, salinity, K-feldspars, and quartz.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
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Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
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Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
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Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Mao Du, Aristeidis Voliotis, Yunqi Shao, Yu Wang, Thomas J. Bannan, Kelly L. Pereira, Jacqueline F. Hamilton, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Meas. Tech., 15, 4385–4406, https://doi.org/10.5194/amt-15-4385-2022, https://doi.org/10.5194/amt-15-4385-2022, 2022
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Atmospheric chemistry plays a key role in the understanding of aerosol formation and air pollution. We designed chamber experiments for the characterization of secondary organic aerosol (SOA) from a biogenic precursor with inorganic seed. Our results highlight the advantages of a combination of online FIGAERO-CIMS and offline LC-Orbitrap MS analytical techniques to characterize the chemical composition of SOA in chamber studies.
Sebastian Diez, Stuart E. Lacy, Thomas J. Bannan, Michael Flynn, Tom Gardiner, David Harrison, Nicholas Marsden, Nicholas A. Martin, Katie Read, and Pete M. Edwards
Atmos. Meas. Tech., 15, 4091–4105, https://doi.org/10.5194/amt-15-4091-2022, https://doi.org/10.5194/amt-15-4091-2022, 2022
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Regardless of the cost of the measuring instrument, there are no perfect measurements. For this reason, we compare the quality of the information provided by cheap devices when they are used to measure air pollutants and we try to emphasise that before judging the potential usefulness of the devices, the user must specify his own needs. Since commonly used performance indices/metrics can be misleading in qualifying this, we propose complementary visual analysis to the more commonly used metrics.
Matthias Karl, Liisa Pirjola, Tiia Grönholm, Mona Kurppa, Srinivasan Anand, Xiaole Zhang, Andreas Held, Rolf Sander, Miikka Dal Maso, David Topping, Shuai Jiang, Leena Kangas, and Jaakko Kukkonen
Geosci. Model Dev., 15, 3969–4026, https://doi.org/10.5194/gmd-15-3969-2022, https://doi.org/10.5194/gmd-15-3969-2022, 2022
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The community aerosol dynamics model MAFOR includes several advanced features: coupling with an up-to-date chemistry mechanism for volatile organic compounds, a revised Brownian coagulation kernel that takes into account the fractal geometry of soot particles, a multitude of nucleation parameterizations, size-resolved partitioning of semi-volatile inorganics, and a hybrid method for the formation of secondary organic aerosols within the framework of condensation and evaporation.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
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Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Kristian Klumpp, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 22, 3655–3673, https://doi.org/10.5194/acp-22-3655-2022, https://doi.org/10.5194/acp-22-3655-2022, 2022
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Surface interactions with solutes can significantly alter the ice nucleation activity of mineral dust. Past studies revealed the sensitivity of microcline, one of the most ice-active types of dust in the atmosphere, to inorganic solutes. This study focuses on the interaction of microcline with bio-organic substances and the resulting effects on its ice nucleation activity. We observe strongly hampered ice nucleation activity due to the presence of carboxylic and amino acids but not for polyols.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
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Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Dina Alfaouri, Monica Passananti, Tommaso Zanca, Lauri Ahonen, Juha Kangasluoma, Jakub Kubečka, Nanna Myllys, and Hanna Vehkamäki
Atmos. Meas. Tech., 15, 11–19, https://doi.org/10.5194/amt-15-11-2022, https://doi.org/10.5194/amt-15-11-2022, 2022
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To study what is happening in the atmosphere, it is important to be able to measure the molecules and clusters present in it. In our work, we studied an artifact that happens inside a mass spectrometer, in particular the fragmentation of clusters. We were able to quantify the fragmentation and retrieve the correct concentration and composition of the clusters using our dual (experimental and theoretical) approach.
Bernd Kärcher and Claudia Marcolli
Atmos. Chem. Phys., 21, 15213–15220, https://doi.org/10.5194/acp-21-15213-2021, https://doi.org/10.5194/acp-21-15213-2021, 2021
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Aerosol–cloud interactions play an important role in climate change. Simulations of the competition between homogeneous solution droplet freezing and heterogeneous ice nucleation can be compromised by the misapplication of ice-active particle fractions frequently derived from laboratory measurements or parametrizations. Our study frames the problem and establishes a solution that is easy to implement in cloud models.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
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The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys., 21, 11637–11654, https://doi.org/10.5194/acp-21-11637-2021, https://doi.org/10.5194/acp-21-11637-2021, 2021
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We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Zainab Bibi, Hugh Coe, James Brooks, Paul I. Williams, Ernesto Reyes-Villegas, Michael Priestley, Carl J. Percival, and James D. Allan
Atmos. Chem. Phys., 21, 10763–10777, https://doi.org/10.5194/acp-21-10763-2021, https://doi.org/10.5194/acp-21-10763-2021, 2021
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We are presenting a new method to apportion black carbon/soot into multiple sources through the inclusion of fullerene and metal data into HR-SP-AMS factorisation. While this itself would be considered a technical development, we can present a budget of contributions to measured BC during the event studied, including the conclusion that fireworks contributed little compared to the bonfire, traffic, and domestic wood-burning emissions.
Robin Wollesen de Jonge, Jonas Elm, Bernadette Rosati, Sigurd Christiansen, Noora Hyttinen, Dana Lüdemann, Merete Bilde, and Pontus Roldin
Atmos. Chem. Phys., 21, 9955–9976, https://doi.org/10.5194/acp-21-9955-2021, https://doi.org/10.5194/acp-21-9955-2021, 2021
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This study presents a detailed analysis of the OH-initiated oxidation of dimethyl sulfide (DMS) based on experiments performed in the Aarhus University Research on Aerosol (AURA) smog chamber and the gas- and particle-phase chemistry kinetic multilayer model (ADCHAM). We capture the formation, growth and chemical composition of aerosols in the chamber setup by an improved multiphase oxidation mechanism and utilize our results to reproduce the important role of DMS in the marine boundary layer.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Claudia Marcolli, Fabian Mahrt, and Bernd Kärcher
Atmos. Chem. Phys., 21, 7791–7843, https://doi.org/10.5194/acp-21-7791-2021, https://doi.org/10.5194/acp-21-7791-2021, 2021
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Pores are aerosol particle features that trigger ice nucleation, as they take up water by capillary condensation below water saturation that freezes at low temperatures. The pore ice can then grow into macroscopic ice crystals making up cirrus clouds. Here, we investigate the pores in soot aggregates responsible for pore condensation and freezing (PCF). Moreover, we present a framework to parameterize soot PCF that is able to predict the ice nucleation activity based on soot properties.
Langwen Huang and David Topping
Geosci. Model Dev., 14, 2187–2203, https://doi.org/10.5194/gmd-14-2187-2021, https://doi.org/10.5194/gmd-14-2187-2021, 2021
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As our knowledge and understanding of atmospheric aerosol particle evolution and impact grows, designing community mechanistic models requires an ability to capture increasing chemical, physical and therefore numerical complexity. As the landscape of computing software and hardware evolves, it is important to profile the usefulness of emerging platforms in tackling this complexity. With this in mind we present JlBox v1.1, written in Julia.
Ines Bulatovic, Adele L. Igel, Caroline Leck, Jost Heintzenberg, Ilona Riipinen, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 3871–3897, https://doi.org/10.5194/acp-21-3871-2021, https://doi.org/10.5194/acp-21-3871-2021, 2021
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We use detailed numerical modelling to show that small aerosol particles (diameters ~25–80 nm; so-called Aitken mode particles) significantly influence low-level cloud properties in the clean summertime high Arctic. The small particles can help sustain clouds when the concentration of larger particles is low (<10–20 cm-3). Measurements from four different observational campaigns in the high Arctic support the modelling results as they indicate that Aitken mode aerosols are frequently activated.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
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This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Simon Patrick O'Meara, Shuxuan Xu, David Topping, M. Rami Alfarra, Gerard Capes, Douglas Lowe, Yunqi Shao, and Gordon McFiggans
Geosci. Model Dev., 14, 675–702, https://doi.org/10.5194/gmd-14-675-2021, https://doi.org/10.5194/gmd-14-675-2021, 2021
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User-friendly and open-source software for simulating aerosol chambers is a valuable tool for research scientists in designing and analysing their experiments. This paper describes a new version of such software and will therefore provide a useful reference for those applying it. Central to the paper is an assessment of the software's accuracy through comparison against previously published simulations.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
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Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Anna Shcherbacheva, Tracey Balehowsky, Jakub Kubečka, Tinja Olenius, Tapio Helin, Heikki Haario, Marko Laine, Theo Kurtén, and Hanna Vehkamäki
Atmos. Chem. Phys., 20, 15867–15906, https://doi.org/10.5194/acp-20-15867-2020, https://doi.org/10.5194/acp-20-15867-2020, 2020
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Atmospheric new particle formation and cluster growth to aerosol particles is an important field of research, in particular due to the climate change phenomenon. Evaporation rates are very difficult to account for but they are important to explain the formation and growth of particles. Different quantum chemistry (QC) methods produce substantially different values for the evaporation rates. We propose a novel approach for inferring evaporation rates of clusters from available measurements.
Patrick A. Barker, Grant Allen, Martin Gallagher, Joseph R. Pitt, Rebecca E. Fisher, Thomas Bannan, Euan G. Nisbet, Stéphane J.-B. Bauguitte, Dominika Pasternak, Samuel Cliff, Marina B. Schimpf, Archit Mehra, Keith N. Bower, James D. Lee, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 20, 15443–15459, https://doi.org/10.5194/acp-20-15443-2020, https://doi.org/10.5194/acp-20-15443-2020, 2020
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Africa is estimated to account for approximately 52 % of global biomass burning (BB) carbon emissions. Despite this, there has been little previous in situ study of African BB emissions. This work presents BB emission factors for various atmospheric trace gases sampled from an aircraft in two distinct areas of Africa (Senegal and Uganda). Intracontinental variability in biomass burning methane emission is identified, which is attributed to difference in the specific fuel mixtures burnt.
Douglas Morrison, Ian Crawford, Nicholas Marsden, Michael Flynn, Katie Read, Luis Neves, Virginia Foot, Paul Kaye, Warren Stanley, Hugh Coe, David Topping, and Martin Gallagher
Atmos. Chem. Phys., 20, 14473–14490, https://doi.org/10.5194/acp-20-14473-2020, https://doi.org/10.5194/acp-20-14473-2020, 2020
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We provide conservative estimates of the concentrations of bacteria within transatlantic dust clouds, originating from the African continent. We observe significant seasonal differences in the overall concentrations of particles but no seasonal variation in the ratio between bacteria and dust. With bacteria contributing to ice formation at warmer temperatures than dust, our observations should improve the accuracy of climate models.
Noora Hyttinen, Reyhaneh Heshmatnezhad, Jonas Elm, Theo Kurtén, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 13131–13143, https://doi.org/10.5194/acp-20-13131-2020, https://doi.org/10.5194/acp-20-13131-2020, 2020
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We present aqueous solubilities and activity coefficients of mono- and dicarboxylic acids (C1–C6 and C2–C8, respectively) estimated using the COSMOtherm program. In addition, we have calculated effective equilibrium constants of dimerization and hydration of the same acids in the condensed phase. We were also able to improve the agreement between experimental and estimated properties of monocarboxylic acids in aqueous solutions by including clustering reactions in COSMOtherm calculations.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
David Topping, David Watts, Hugh Coe, James Evans, Thomas J. Bannan, Douglas Lowe, Caroline Jay, and Jonathan W. Taylor
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-270, https://doi.org/10.5194/gmd-2020-270, 2020
Publication in GMD not foreseen
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Time-series forecasting methods have often been used to mitigate some of the challenges associated with deploying chemical transport models. In this study we deploy and evaluate Facebook’s Prophetmodel v0.6 in predicting hourly concentrations of Nitrogen Dioxide [NO2]. et. Overall we find the Prophet model offers a relatively effective and simple way to make predictions about NO2 at local levels.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Robert O. David, Jonas Fahrni, Claudia Marcolli, Fabian Mahrt, Dominik Brühwiler, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 9419–9440, https://doi.org/10.5194/acp-20-9419-2020, https://doi.org/10.5194/acp-20-9419-2020, 2020
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Ice crystal formation plays an important role in controlling the Earth's climate. However, the mechanisms responsible for ice formation in the atmosphere are still uncertain. Here we use surrogates for atmospherically relevant porous particles to determine the role of pore diameter and wettability on the ability of porous particles to nucleate ice in the atmosphere. Our results are consistent with the pore condensation and freeing mechanism.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Tommaso Zanca, Jakub Kubečka, Evgeni Zapadinsky, Monica Passananti, Theo Kurtén, and Hanna Vehkamäki
Atmos. Meas. Tech., 13, 3581–3593, https://doi.org/10.5194/amt-13-3581-2020, https://doi.org/10.5194/amt-13-3581-2020, 2020
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In this paper we quantify (using a statistical model) the probability of decomposition of a representative class of HOM clusters in an APi-TOF mass spectrometer. This is important because it quantifies the systematic error of measurements in a APi-TOF MS due to cluster decomposition. The results (specific for our selected clusters) show that decomposition is negligible, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Nir Bluvshtein, Ulrich K. Krieger, and Thomas Peter
Atmos. Meas. Tech., 13, 3191–3203, https://doi.org/10.5194/amt-13-3191-2020, https://doi.org/10.5194/amt-13-3191-2020, 2020
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Light-absorbing organic particles undergo transformations during their exposure in the atmosphere. The role these particles play in the global radiative balance is uncertain. This study describes high-sensitivity and high-precision measurements of light absorption by a single particle levitated in an electrodynamic balance. This high level of sensitivity enables future studies to explore the major processes responsible for changes to the particle's light absorptivity.
Noora Hyttinen, Jonas Elm, Jussi Malila, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 5679–5696, https://doi.org/10.5194/acp-20-5679-2020, https://doi.org/10.5194/acp-20-5679-2020, 2020
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Organosulfates have been identified in atmospheric secondary organic aerosol (SOA). The thermodynamic properties of SOA constituents, such as organosulfates, affect the stability and atmospheric impact of the SOA. Here we present estimated solubility, activity, pKa, saturation vapor pressure and Henry's law solubility values for several atmospherically relevant monoterpene- and isoprene-derived organosulfate compounds. These properties can be used, for example, in aerosol process modeling.
María Cascajo-Castresana, Robert O. David, Maiara A. Iriarte-Alonso, Alexander M. Bittner, and Claudia Marcolli
Atmos. Chem. Phys., 20, 3291–3315, https://doi.org/10.5194/acp-20-3291-2020, https://doi.org/10.5194/acp-20-3291-2020, 2020
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Atmospheric ice-nucleating particles are rare but relevant for cloud glaciation. A source of particles that nucleate ice above −15 °C is biological material including some proteins. Here we show that proteins of very diverse functions and structures can nucleate ice. Among these, the iron storage protein apoferritin stands out, with activity up to −4 °C. We show that its activity does not stem from correctly assembled proteins but from misfolded protein monomers or oligomers and aggregates.
Claudia Marcolli
Atmos. Chem. Phys., 20, 3209–3230, https://doi.org/10.5194/acp-20-3209-2020, https://doi.org/10.5194/acp-20-3209-2020, 2020
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Pore condensation and freezing (PCF) is an ice nucleation mechanism explaining ice formation at low ice supersaturation. It is assumed that liquid water condenses in pores of solid aerosol particles below water saturation followed by ice nucleation within the pores. This study discusses conditions of pore filling, homogeneous ice nucleation within the volume of porewater, and growth of ice out of the pores, taking the effect of negative pressure within pores below water saturation into account.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
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Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Parya Broomandi, Xueyu Geng, Weisi Guo, Jong Ryeol Kim, Alessio Pagani, and David Topping
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2019-342, https://doi.org/10.5194/gmd-2019-342, 2020
Revised manuscript not accepted
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As a result of our novel graph-based reduced modeling, we are able to represent high-dimensional knowledge into a causal inference and stability framework.
Kathryn Fowler, Paul Connolly, and David Topping
Atmos. Chem. Phys., 20, 683–698, https://doi.org/10.5194/acp-20-683-2020, https://doi.org/10.5194/acp-20-683-2020, 2020
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Observations of low–temperature cirrus clouds have found unexpectedly low ice crystal numbers and high supersaturations, suggesting an incomplete understanding of the freezing mechanisms under these conditions. The existence of viscous organic aerosol has offered alternative ice nucleation pathways, which have been observed in laboratory studies. We have developed the first cloud parcel model to investigate the effect of viscosity on ice nucleation.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Robert O. David, Maria Cascajo-Castresana, Killian P. Brennan, Michael Rösch, Nora Els, Julia Werz, Vera Weichlinger, Lin S. Boynton, Sophie Bogler, Nadine Borduas-Dedekind, Claudia Marcolli, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 6865–6888, https://doi.org/10.5194/amt-12-6865-2019, https://doi.org/10.5194/amt-12-6865-2019, 2019
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Here we present the development and applicability of the DRoplet Ice Nuclei Counter Zurich (DRINCZ). DRINCZ allows for ice nuclei in the immersion mode to be quantified between 0 and -25 °C with an uncertainty of ±0.9 °C. Furthermore, we present a new method for assessing biases in drop-freezing apparatuses and cumulative ice-nucleating-particle concentrations from snow samples collected in the Austrian Alps at the Sonnblick Observatory.
Leigh R. Crilley, Louisa J. Kramer, Bin Ouyang, Jun Duan, Wenqian Zhang, Shengrui Tong, Maofa Ge, Ke Tang, Min Qin, Pinhua Xie, Marvin D. Shaw, Alastair C. Lewis, Archit Mehra, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Hugh Coe, James Allan, Carl J. Percival, Olalekan A. M. Popoola, Roderic L. Jones, and William J. Bloss
Atmos. Meas. Tech., 12, 6449–6463, https://doi.org/10.5194/amt-12-6449-2019, https://doi.org/10.5194/amt-12-6449-2019, 2019
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Nitrous acid (HONO) is key species for understanding tropospheric chemistry, yet accurate and precise measurements are challenging. Here we report an inter–comparison exercise of a number of instruments that measured HONO in a highly polluted location (Beijing). All instruments agreed on the temporal trends yet displayed divergence in absolute concentrations. The cause of this divergence was unclear, but it may in part be due to spatial variability in instrument location.
Roope Halonen, Evgeni Zapadinsky, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 19, 13355–13366, https://doi.org/10.5194/acp-19-13355-2019, https://doi.org/10.5194/acp-19-13355-2019, 2019
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The rate of collisions between molecules or clusters is used to determine particle formation in the atmosphere. The basic approach is to treat the colliding particles as noninteracting hard spheres. By using atomistic simulations with a realistic force field and theoretical approaches, we showed that the actual collision rate of two sulfuric acid molecules is more than twice as high as that for hard spheres. The results of this study will improve models of atmospheric particle growth.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Kelly L. Pereira, Grazia Rovelli, Young C. Song, Alfred W. Mayhew, Jonathan P. Reid, and Jacqueline F. Hamilton
Atmos. Meas. Tech., 12, 4519–4541, https://doi.org/10.5194/amt-12-4519-2019, https://doi.org/10.5194/amt-12-4519-2019, 2019
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We present the design and operation of a newly built continuous-flow reactor (CFR), which can be used as a tool to gain considerable insights into the composition and physical state of secondary organic aerosol (SOA). The CFR was used to generate large quantities of SOA mass, allowing the use of highly accurate techniques that are not usually accessible. We demonstrate how this unique approach can be used to investigate the relationship between SOA formation and physiochemical properties.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Nanna Myllys, Jakub Kubečka, Vitus Besel, Dina Alfaouri, Tinja Olenius, James Norman Smith, and Monica Passananti
Atmos. Chem. Phys., 19, 9753–9768, https://doi.org/10.5194/acp-19-9753-2019, https://doi.org/10.5194/acp-19-9753-2019, 2019
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In atmospheric sulfuric-acid-driven particle formation, bases are able to stabilize the initial molecular clusters and thus enhance particle formation. We have investigated the enhancing potential of different bases in atmospheric particle formation. We show that strong bases with low abundance are likely to dominate electrically neutral particle formation, whereas weak bases with high abundance have a larger role in ion-mediated particle formation.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
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We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Lauriane L. J. Quéléver, Kasper Kristensen, Louise Normann Jensen, Bernadette Rosati, Ricky Teiwes, Kaspar R. Daellenbach, Otso Peräkylä, Pontus Roldin, Rossana Bossi, Henrik B. Pedersen, Marianne Glasius, Merete Bilde, and Mikael Ehn
Atmos. Chem. Phys., 19, 7609–7625, https://doi.org/10.5194/acp-19-7609-2019, https://doi.org/10.5194/acp-19-7609-2019, 2019
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Highly oxygenated organic molecules (HOMs) form rapidly in oxidation of monoterpenes and have been shown to be crucial for secondary organic aerosol formation. We studied the formation of HOMs under different temperatures, finding a strong dependence on their yields. As temperatures decrease, the isomerization reactions that allow rapid oxidation by molecular oxygen slow down, and competing reaction pathways can suppress the HOM formation almost completely, especially at high VOC loadings.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6035–6058, https://doi.org/10.5194/acp-19-6035-2019, https://doi.org/10.5194/acp-19-6035-2019, 2019
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This paper not only interests the atmospheric science community but has a potential to cater to a broader audience. We discuss both long- and
short-term effects of various
atmospherically relevantchemical species on a fairly abundant mineral surface
Quartz. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6059–6084, https://doi.org/10.5194/acp-19-6059-2019, https://doi.org/10.5194/acp-19-6059-2019, 2019
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This paper not only interests the Atmospheric Science community but has a potential to cater to a broader audience. We discuss both long- and short-term effects of various
atmospherically relevantchemical species on fairly abundant mineral surfaces like feldspars and clays. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
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The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Elizabeth Forde, Martin Gallagher, Virginia Foot, Roland Sarda-Esteve, Ian Crawford, Paul Kaye, Warren Stanley, and David Topping
Atmos. Chem. Phys., 19, 1665–1684, https://doi.org/10.5194/acp-19-1665-2019, https://doi.org/10.5194/acp-19-1665-2019, 2019
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The abundance and diversity of airborne biological particles in different environments remains poorly constrained. Measurements of such particles were conducted at four sites in the United Kingdom, using real-time fluorescence instrumentation. Using local land cover types, sources of suspected particle types were identified and compared. Most sites exhibited a wet-discharged fungal spore dominance, with the exception of one site, which was inferred to be influenced by a local dairy farm.
Theo Kurtén, Noora Hyttinen, Emma Louise D'Ambro, Joel Thornton, and Nønne Lyng Prisle
Atmos. Chem. Phys., 18, 17589–17600, https://doi.org/10.5194/acp-18-17589-2018, https://doi.org/10.5194/acp-18-17589-2018, 2018
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We use COSMO-RS to compute saturation vapor pressures for two products of isoprene photo-oxidation and compare the results to measurements. COSMO-RS is an attractive option for calculating properties of molecules, as it is based on quantum mechanics and requires few fitting parameters. However, we show that the default implementation of this method suffers from errors related to both conformational sampling and intramolecular hydrogen bonding. We propose solutions to these problems.
Simon Ruske, David O. Topping, Virginia E. Foot, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 11, 6203–6230, https://doi.org/10.5194/amt-11-6203-2018, https://doi.org/10.5194/amt-11-6203-2018, 2018
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Pollen, bacteria and fungal spores are common in the environment, can have very important implications for public health and may influence the weather. Biological sensors potentially could be used to monitor quantities of these types of particles. However, it is important to transform the measurements from these instruments into counts of these biological particles. The paper tests a variety of approaches for achieving this aim on data collected in a laboratory.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937, https://doi.org/10.5194/acp-18-14925-2018, https://doi.org/10.5194/acp-18-14925-2018, 2018
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Co-condensation of inorganic or organic vapours on growing droplets could significantly enhance both CCN and cloud droplet number concentration, thereby influencing climate. Until now, there has been very few direct observational evidence of this process. We exposed involatile inorganic particles to a moist atmosphere containing a controlled amount of an organic semi-volatile vapour. We measured a much greater growth of the particles than if they had only been exposed to water vapour.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
Jenni Kontkanen, Tinja Olenius, Markku Kulmala, and Ilona Riipinen
Atmos. Chem. Phys., 18, 13733–13754, https://doi.org/10.5194/acp-18-13733-2018, https://doi.org/10.5194/acp-18-13733-2018, 2018
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New particle formation involving sulfuric acid, bases and organic compounds is an important source of atmospheric aerosol particles. We investigate the capability of nano-Köhler theory to describe this process by simulating the dynamics of atmospheric molecular clusters. We find that nano-Köhler-type behavior occurs in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations are in a suitable range.
Mehrnoush M. Fard, Ulrich K. Krieger, and Thomas Peter
Atmos. Chem. Phys., 18, 13511–13530, https://doi.org/10.5194/acp-18-13511-2018, https://doi.org/10.5194/acp-18-13511-2018, 2018
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Atmospheric aerosol particles may undergo liquid–liquid phase separation (LLPS) when exposed to varying relative humidity, with an aqueous organic phase enclosing an aqueous inorganic phase below a threshold of relative humidity. Brown carbon (BrC) compounds will redistribute to the organic phase upon LLPS. We use numerical modeling to study the shortwave radiative impact of LLPS containing BrC and conclude that it is not significant for atmospheric aerosol.
Michael Priestley, Michael le Breton, Thomas J. Bannan, Stephen D. Worrall, Asan Bacak, Andrew R. D. Smedley, Ernesto Reyes-Villegas, Archit Mehra, James Allan, Ann R. Webb, Dudley E. Shallcross, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 18, 13481–13493, https://doi.org/10.5194/acp-18-13481-2018, https://doi.org/10.5194/acp-18-13481-2018, 2018
Fabian Mahrt, Claudia Marcolli, Robert O. David, Philippe Grönquist, Eszter J. Barthazy Meier, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 13363–13392, https://doi.org/10.5194/acp-18-13363-2018, https://doi.org/10.5194/acp-18-13363-2018, 2018
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The ice nucleation ability of different soot particles in the cirrus and mixed-phase cloud temperature regime is presented. The impact of aerosol particle size, particle morphology, organic matter and hydrophilicity on ice nucleation is examined. We propose ice nucleation proceeds via a pore condensation freezing mechanism for soot particles with the necessary physicochemical properties that nucleated ice well below water saturation.
Michael Le Breton, Åsa M. Hallquist, Ravi Kant Pathak, David Simpson, Yujue Wang, John Johansson, Jing Zheng, Yudong Yang, Dongjie Shang, Haichao Wang, Qianyun Liu, Chak Chan, Tao Wang, Thomas J. Bannan, Michael Priestley, Carl J. Percival, Dudley E. Shallcross, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 13013–13030, https://doi.org/10.5194/acp-18-13013-2018, https://doi.org/10.5194/acp-18-13013-2018, 2018
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We apply state-of-the-art chemical characterization to determine the chloride radical production in Beijing via measurement of inorganic halogens at a semi-rural site. The high concentration of inorganic halogens, namely nitryl chloride, enables the production of chlorinated volatile organic compounds which are measured in both the gas and particle phases simultaneously. This enables the secondary production of aerosols via chlorine oxidation to be directly observed in ambient air.
Maryam Dalirian, Arttu Ylisirniö, Angela Buchholz, Daniel Schlesinger, Johan Ström, Annele Virtanen, and Ilona Riipinen
Atmos. Chem. Phys., 18, 12477–12489, https://doi.org/10.5194/acp-18-12477-2018, https://doi.org/10.5194/acp-18-12477-2018, 2018
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Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect is, however, still uncertain. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC particles, in pure state or coated by various organic species. Our results show that existing theories have potential in describing the CCN activation of atmospheric BC mixed with soluble pollutants.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Yangxi Chu, Erin Evoy, Saeid Kamal, Young Chul Song, Jonathan P. Reid, Chak K. Chan, and Allan K. Bertram
Atmos. Meas. Tech., 11, 4809–4822, https://doi.org/10.5194/amt-11-4809-2018, https://doi.org/10.5194/amt-11-4809-2018, 2018
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The viscosity of erythritol, a tetrol found in aerosol particles, is highly uncertain. To help resolve this uncertainty, we measured the viscosities of
erythritol–water particles using rectangular-area fluorescence recovery after photobleaching and aerosol optical tweezers techniques. These results
should help improve the understanding of the viscosity of secondary organic aerosol particles. In addition, we present an intercomparison of techniques
for measuring the viscosity of particles.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Michael Le Breton, Yujue Wang, Åsa M. Hallquist, Ravi Kant Pathak, Jing Zheng, Yudong Yang, Dongjie Shang, Marianne Glasius, Thomas J. Bannan, Qianyun Liu, Chak K. Chan, Carl J. Percival, Wenfei Zhu, Shengrong Lou, David Topping, Yuchen Wang, Jianzhen Yu, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 10355–10371, https://doi.org/10.5194/acp-18-10355-2018, https://doi.org/10.5194/acp-18-10355-2018, 2018
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This paper utilizes a chemical ionisation mass spectrometer measuring gas and particle-phase organosulfates (OS) simultaneously during a field campaign in Beijing, China, and highlights how high time frequency online measurements enable a detailed analysis of dominant production mechanisms. We find that high aerosol acidity, organic precursor concentration and relative humidity promote the production of OS. The thermogram desorption reveals the potential for semi-volatile gas-phase OS.
Ru-Jin Huang, Junji Cao, Yang Chen, Lu Yang, Jincan Shen, Qihua You, Kai Wang, Chunshui Lin, Wei Xu, Bo Gao, Yongjie Li, Qi Chen, Thorsten Hoffmann, Colin D. O'Dowd, Merete Bilde, and Marianne Glasius
Atmos. Meas. Tech., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, https://doi.org/10.5194/amt-11-3447-2018, 2018
Quentin Bourgeois, Annica M. L. Ekman, Jean-Baptiste Renard, Radovan Krejci, Abhay Devasthale, Frida A.-M. Bender, Ilona Riipinen, Gwenaël Berthet, and Jason L. Tackett
Atmos. Chem. Phys., 18, 7709–7720, https://doi.org/10.5194/acp-18-7709-2018, https://doi.org/10.5194/acp-18-7709-2018, 2018
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The altitude of aerosols is crucial as they can impact cloud formation and radiation. In this study, satellite observations have been used to characterize the global aerosol optical depth (AOD) in the boundary layer and the free troposphere. The free troposphere contributes 39 % to the global AOD during daytime. Overall, the results have implications for the description of budgets, sources, sinks and transport of aerosol particles as presently described in the atmospheric model.
Anand Kumar, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 18, 7057–7079, https://doi.org/10.5194/acp-18-7057-2018, https://doi.org/10.5194/acp-18-7057-2018, 2018
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We have performed immersion freezing experiments with microcline (most active ice nucleation, IN, K-feldspar polymorph) and investigated the effect of ammonium and non-ammonium solutes on its IN efficiency. We report increased IN efficiency of microcline in dilute ammonia- or ammonium-containing solutions, which opens up a pathway for condensation freezing occurring at a warmer temperature than immersion freezing.
Ernesto Reyes-Villegas, Michael Priestley, Yu-Chieh Ting, Sophie Haslett, Thomas Bannan, Michael Le Breton, Paul I. Williams, Asan Bacak, Michael J. Flynn, Hugh Coe, Carl Percival, and James D. Allan
Atmos. Chem. Phys., 18, 4093–4111, https://doi.org/10.5194/acp-18-4093-2018, https://doi.org/10.5194/acp-18-4093-2018, 2018
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This work presents the analysis of a special event with high biomass burning emissions, named Bonfire Night. Nitrogen chemistry was observed and it was possible to study the night time chemistry. It was possible to quantify particulate organic oxides of nitrogen (PON) concentrations of 2.8 µg m−3 using 46 : 30 ratios from aerosol mass spectrometry measurements. The use of the receptor model positive matrix factorization (PMF) allowed to separate organic aerosols into different sources.
Stefano Decesari, Simona Kovarich, Manuela Pavan, Arianna Bassan, Andrea Ciacci, and David Topping
Atmos. Chem. Phys., 18, 2329–2340, https://doi.org/10.5194/acp-18-2329-2018, https://doi.org/10.5194/acp-18-2329-2018, 2018
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Particulate matter (PM) chemical composition includes thousands of individual organic compounds that have never been tested for their toxicological potential. Computational (in silico) screenings represent a promising approach to identify new target compounds for more in-depth toxicological analyses. We provide here a proof-of-concept evaluation based on ca. 100 aerosol organic compounds. Reliable toxicological predictions were obtained for more than 80 % of them.
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara
Atmos. Chem. Phys., 18, 1629–1642, https://doi.org/10.5194/acp-18-1629-2018, https://doi.org/10.5194/acp-18-1629-2018, 2018
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This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
Adam W. Birdsall, Ulrich K. Krieger, and Frank N. Keutsch
Atmos. Meas. Tech., 11, 33–47, https://doi.org/10.5194/amt-11-33-2018, https://doi.org/10.5194/amt-11-33-2018, 2018
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We have developed a laboratory system that provides mass spectra of individual particles, roughly 20 microns in diameter, after they have been levitated in an electric field. Measured evaporation of polyethylene glycol particles was found to agree with a kinetic model. The system can be used to study fundamental chemical and physical processes involving particles that are difficult to isolate and study with other techniques, and hence improve our understanding of atmospheric particles.
Simon O'Meara, David O. Topping, Rahul A. Zaveri, and Gordon McFiggans
Atmos. Chem. Phys., 17, 10477–10494, https://doi.org/10.5194/acp-17-10477-2017, https://doi.org/10.5194/acp-17-10477-2017, 2017
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To simulate particle-phase diffusion, an analytical expression is desired because it takes less calculation time than a differential equation. Here a correction is found for the analytical solution for when diffusivity is dependent on composition, thereby making it more widely applicable than before. Consequently, we are able to more realistically evaluate the rate limitation (if any) imposed by particle-phase diffusion on component partitioning between the gas and particle phase.
Michael I. Cotterell, Rose E. Willoughby, Bryan R. Bzdek, Andrew J. Orr-Ewing, and Jonathan P. Reid
Atmos. Chem. Phys., 17, 9837–9851, https://doi.org/10.5194/acp-17-9837-2017, https://doi.org/10.5194/acp-17-9837-2017, 2017
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The optical properties of aerosols are required to analyse measurements of aerosol properties, estimate radiative forcing and interpret remote sensing retrievals. We provide comprehensive data sets of the refractive indices of the most important inorganic aerosol constituents, reporting parameterisations for the wavelength and relative humidity dependencies for each system. We assess the accuracy of this study, made on single trapped particles, against previous less comprehensive data sets.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Sandra Bastelberger, Ulrich K. Krieger, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 8453–8471, https://doi.org/10.5194/acp-17-8453-2017, https://doi.org/10.5194/acp-17-8453-2017, 2017
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We present quantitative condensed-phase diffusivity measurements of a volatile organic (tetraethylene glycol) in highly viscous single aerosol particles (aqueous sucrose). The condensed-phase diffusivity exhibits a strong temperature and humidity dependence. Our results suggest that diffusion limitations of volatile organics in highly viscous organic aerosol may severely impact gas–particle partitioning under cold and dry conditions.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Aleksandra Marsh, Rachael E. H. Miles, Grazia Rovelli, Alexander G. Cowling, Lucy Nandy, Cari S. Dutcher, and Jonathan P. Reid
Atmos. Chem. Phys., 17, 5583–5599, https://doi.org/10.5194/acp-17-5583-2017, https://doi.org/10.5194/acp-17-5583-2017, 2017
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The response of aerosol particles to changes in relative humidity (RH) is dependent on the hygroscopicity of the constituent chemical components. We present accurate measurements of the hygroscopic response of aerosols over a wide range in RH, extending up to the saturation RH. The chemical compounds studied include dicarboxylic acids, amino acids, sugars and polyols. These data provide a comprehensive source of data to help improve functional group activity models of aerosol hygroscopicity.
Lisa Stirnweis, Claudia Marcolli, Josef Dommen, Peter Barmet, Carla Frege, Stephen M. Platt, Emily A. Bruns, Manuel Krapf, Jay G. Slowik, Robert Wolf, Andre S. H. Prévôt, Urs Baltensperger, and Imad El-Haddad
Atmos. Chem. Phys., 17, 5035–5061, https://doi.org/10.5194/acp-17-5035-2017, https://doi.org/10.5194/acp-17-5035-2017, 2017
Grazia Rovelli, Rachael E. H. Miles, Jonathan P. Reid, and Simon L. Clegg
Atmos. Chem. Phys., 17, 4369–4385, https://doi.org/10.5194/acp-17-4369-2017, https://doi.org/10.5194/acp-17-4369-2017, 2017
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The response of airborne particles to relative humidity (RH) in the atmosphere, referred to as their hygroscopicity, is a key property that determines their water content. The hygroscopicity depends on the chemical species that make up the particle. Here, we investigate the growth in particle size and composition that occurs with increasing RH for particles containing a series of amine compounds and sulfuric acid, typical atmospheric components, providing a comprehensive and accurate data set.
Lukas Kaufmann, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 3525–3552, https://doi.org/10.5194/acp-17-3525-2017, https://doi.org/10.5194/acp-17-3525-2017, 2017
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To improve the understanding of heterogeneous ice nucleation, we have subjected different ice nuclei to repeated freezing cycles and evaluated the freezing temperatures with different parameterizations of classical nucleation theory. It was found that two fit parameters were necessary to describe the temperature dependence of the nucleation rate.
Simon Ruske, David O. Topping, Virginia E. Foot, Paul H. Kaye, Warren R. Stanley, Ian Crawford, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 10, 695–708, https://doi.org/10.5194/amt-10-695-2017, https://doi.org/10.5194/amt-10-695-2017, 2017
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Particles such as bacteria, pollen and fungal spores have important implications within the environment and public health sectors. Here we evaluate the performance of various different methods for distinguishing between these different types of particles using a new instrument. We demonstrate that there may be better alternatives to the currently used methods which can be further investigated in future research.
Claudia Marcolli
Atmos. Chem. Phys., 17, 1595–1622, https://doi.org/10.5194/acp-17-1595-2017, https://doi.org/10.5194/acp-17-1595-2017, 2017
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Laboratory studies from the last century have shown that some types of particles are susceptible to pre-activation, i.e. they are able to develop macroscopic ice at warmer temperatures or lower relative humidities after they had been involved in an ice nucleation event before. This review analyses these works under the presumption that pre-activation occurs by ice preserved in pores, and it discusses atmospheric scenarios for which pre-activation might be important.
Eleonora Aruffo, Fabio Biancofiore, Piero Di Carlo, Marcella Busilacchio, Marco Verdecchia, Barbara Tomassetti, Cesare Dari-Salisburgo, Franco Giammaria, Stephane Bauguitte, James Lee, Sarah Moller, James Hopkins, Shalini Punjabi, Stephen J. Andrews, Alistair C. Lewis, Paul I. Palmer, Edward Hyer, Michael Le Breton, and Carl Percival
Atmos. Meas. Tech., 9, 5591–5606, https://doi.org/10.5194/amt-9-5591-2016, https://doi.org/10.5194/amt-9-5591-2016, 2016
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During the BORTAS aircraft campaign, we measured NO2 and their oxidtation products (as peroxy nitrates) with a custom laser-induced fluorescence instrument. Because of the high correlation between known pyrogenic tracers (i.e., carbon monoxide) and peroxy nitrates, we provide two methods to use these species for the identification of biomass burning (BB) plumes. Using an artifical neural network, we improved the BB identification taking into account of a meteorological parameter (pressure).
Hanna K. Lappalainen, Veli-Matti Kerminen, Tuukka Petäjä, Theo Kurten, Aleksander Baklanov, Anatoly Shvidenko, Jaana Bäck, Timo Vihma, Pavel Alekseychik, Meinrat O. Andreae, Stephen R. Arnold, Mikhail Arshinov, Eija Asmi, Boris Belan, Leonid Bobylev, Sergey Chalov, Yafang Cheng, Natalia Chubarova, Gerrit de Leeuw, Aijun Ding, Sergey Dobrolyubov, Sergei Dubtsov, Egor Dyukarev, Nikolai Elansky, Kostas Eleftheriadis, Igor Esau, Nikolay Filatov, Mikhail Flint, Congbin Fu, Olga Glezer, Aleksander Gliko, Martin Heimann, Albert A. M. Holtslag, Urmas Hõrrak, Juha Janhunen, Sirkku Juhola, Leena Järvi, Heikki Järvinen, Anna Kanukhina, Pavel Konstantinov, Vladimir Kotlyakov, Antti-Jussi Kieloaho, Alexander S. Komarov, Joni Kujansuu, Ilmo Kukkonen, Ella-Maria Duplissy, Ari Laaksonen, Tuomas Laurila, Heikki Lihavainen, Alexander Lisitzin, Alexsander Mahura, Alexander Makshtas, Evgeny Mareev, Stephany Mazon, Dmitry Matishov, Vladimir Melnikov, Eugene Mikhailov, Dmitri Moisseev, Robert Nigmatulin, Steffen M. Noe, Anne Ojala, Mari Pihlatie, Olga Popovicheva, Jukka Pumpanen, Tatjana Regerand, Irina Repina, Aleksei Shcherbinin, Vladimir Shevchenko, Mikko Sipilä, Andrey Skorokhod, Dominick V. Spracklen, Hang Su, Dmitry A. Subetto, Junying Sun, Arkady Y. Terzhevik, Yuri Timofeyev, Yuliya Troitskaya, Veli-Pekka Tynkkynen, Viacheslav I. Kharuk, Nina Zaytseva, Jiahua Zhang, Yrjö Viisanen, Timo Vesala, Pertti Hari, Hans Christen Hansson, Gennady G. Matvienko, Nikolai S. Kasimov, Huadong Guo, Valery Bondur, Sergej Zilitinkevich, and Markku Kulmala
Atmos. Chem. Phys., 16, 14421–14461, https://doi.org/10.5194/acp-16-14421-2016, https://doi.org/10.5194/acp-16-14421-2016, 2016
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After kick off in 2012, the Pan-Eurasian Experiment (PEEX) program has expanded fast and today the multi-disciplinary research community covers ca. 80 institutes and a network of ca. 500 scientists from Europe, Russia, and China. Here we introduce scientific topics relevant in this context. This is one of the first multi-disciplinary overviews crossing scientific boundaries, from atmospheric sciences to socio-economics and social sciences.
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
François Benduhn, Graham W. Mann, Kirsty J. Pringle, David O. Topping, Gordon McFiggans, and Kenneth S. Carslaw
Geosci. Model Dev., 9, 3875–3906, https://doi.org/10.5194/gmd-9-3875-2016, https://doi.org/10.5194/gmd-9-3875-2016, 2016
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We present a new mathematical formalism that serves to represent exchanges of inorganic matter between the atmosphere gas phase and the aerosol aqueous phase. In a global modelling framework, taking into account these processes may help represent many important features more accurately, such as the formation of cloud droplets or the radiative properties of the atmosphere. The formalism strives to keep an appropriate balance between accuracy and computation efficiency requirements.
Matthew Crooks, Paul Connolly, David Topping, and Gordon McFiggans
Geosci. Model Dev., 9, 3617–3637, https://doi.org/10.5194/gmd-9-3617-2016, https://doi.org/10.5194/gmd-9-3617-2016, 2016
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Semi-volatile compounds, like water, can exist in both vapour phases and condensed phases within a system. This paper presents a method of calculating the condensed and vapour phases of semi-volatile compounds at equilibrium, in particular, when the condensed mass occurs within particles of different sizes and chemical composition. The applications of interest to the authors are those of atmospheric importance such as cloud droplet formation and reflection or absorption of solar radiation.
Lukas Kaufmann, Claudia Marcolli, Julian Hofer, Valeria Pinti, Christopher R. Hoyle, and Thomas Peter
Atmos. Chem. Phys., 16, 11177–11206, https://doi.org/10.5194/acp-16-11177-2016, https://doi.org/10.5194/acp-16-11177-2016, 2016
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We investigated dust samples from dust source regions all over the globe with respect to their ice nucleation activity and their mineralogical composition. Stones of reference minerals were milled and investigated the same way as the natural dust samples. We found that the mineralogical composition is a major determinant of ice nucleation ability. Natural samples consist of mixtures of minerals with remarkably similar ice nucleation ability.
Samuel Lowe, Daniel G. Partridge, David Topping, and Philip Stier
Atmos. Chem. Phys., 16, 10941–10963, https://doi.org/10.5194/acp-16-10941-2016, https://doi.org/10.5194/acp-16-10941-2016, 2016
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A novel inverse modelling framework is developed for analysing the sensitivity of cloud condensation nuclei (CCN) concentrations to simultaneous perturbations in multiple model parameters at atmospherically relevant humidities. Many parameter interactions are identified and CCN concentrations are found to be relatively insensitive to bulk–surface partitioning, while aerosol concentration, surface tension, composition and solution ideality exhibit a higher degree of sensitivity.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
Claudia Marcolli, Baban Nagare, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8915–8937, https://doi.org/10.5194/acp-16-8915-2016, https://doi.org/10.5194/acp-16-8915-2016, 2016
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Silver iodide is one of the best-investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Nevertheless, many open questions remain. This paper gives an overview of silver iodide as an ice nucleus and tries to identify the factors that influence the ice nucleation ability of silver iodide.
Lindsay Renbaum-Wolff, Mijung Song, Claudia Marcolli, Yue Zhang, Pengfei F. Liu, James W. Grayson, Franz M. Geiger, Scot T. Martin, and Allan K. Bertram
Atmos. Chem. Phys., 16, 7969–7979, https://doi.org/10.5194/acp-16-7969-2016, https://doi.org/10.5194/acp-16-7969-2016, 2016
Erika Kienast-Sjögren, Christian Rolf, Patric Seifert, Ulrich K. Krieger, Bei P. Luo, Martina Krämer, and Thomas Peter
Atmos. Chem. Phys., 16, 7605–7621, https://doi.org/10.5194/acp-16-7605-2016, https://doi.org/10.5194/acp-16-7605-2016, 2016
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We present a climatology of mid-latitude cirrus cloud properties based on 13 000 hours of automatically analyzed lidar measurements at three different sites. Jungfraujoch,
situated at 3580 m a.s.l., is found to be ideal to measure high and optically thin
cirrus. We use our retrieved optical properties together with a radiation model and
estimate the radiative forcing by mid-latitude cirrus.
All cirrus clouds detected here have a positive net radiative effect.
Simon O'Meara, David O. Topping, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, https://doi.org/10.5194/acp-16-5299-2016, 2016
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To understand the effect of atmospheric particulate matter on climate and human health we need to know how it evolves. We investigate how best to estimate diffusion of components through particles by comparing diffusion times from three approaches to solving Fick's Law and find that they agree. This means that scientists can simulate Fickian diffusion through atmospheric particles using the approach best suited to their requirements and have confidence that their model is mathematically sound.
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
David Topping, Mark Barley, Michael K. Bane, Nicholas Higham, Bernard Aumont, Nicholas Dingle, and Gordon McFiggans
Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, https://doi.org/10.5194/gmd-9-899-2016, 2016
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In this paper we describe the development and application of a new web-based and open-source facility, UManSysProp (http://umansysprop .seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
J. R. Pitt, M. Le Breton, G. Allen, C. J. Percival, M. W. Gallagher, S. J.-B. Bauguitte, S. J. O'Shea, J. B. A. Muller, M. S. Zahniser, J. Pyle, and P. I. Palmer
Atmos. Meas. Tech., 9, 63–77, https://doi.org/10.5194/amt-9-63-2016, https://doi.org/10.5194/amt-9-63-2016, 2016
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We present details of an Aerodyne quantum cascade laser absorption spectrometer (QCLAS) used to make airborne measurements of N2O and CH4, including its configuration for use on board an aircraft. Two different methods to correct for the influence of water vapour on the measurements are evaluated. We diagnose a sensitivity of the instrument to changes in pressure, introduce a new calibration procedure to account for this effect, and assess its performance.
B. Nagare, C. Marcolli, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 15, 13759–13776, https://doi.org/10.5194/acp-15-13759-2015, https://doi.org/10.5194/acp-15-13759-2015, 2015
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We determined collision efficiencies of cloud droplets with aerosol particles experimentally and found that they were around 1 order of magnitude higher than theoretical formulations that include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This is most probably due to uncertainties and inaccuracies in the theoretical formulations of thermophoretic and diffusiophoretic processes.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
I. Crawford, S. Ruske, D. O. Topping, and M. W. Gallagher
Atmos. Meas. Tech., 8, 4979–4991, https://doi.org/10.5194/amt-8-4979-2015, https://doi.org/10.5194/amt-8-4979-2015, 2015
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HCA analysis methods were evaluated for the purpose of identifying primary biological aerosol sampled with a WIBS. The ward linkage with z-score normalisation could discriminate between five test particles with 98% accuracy. We applied these methods to a previously studied ambient data set, where both methods produced similar results with some minor differences in cluster partitioning. Finally we compared to previous approaches and found our new method offered improved quantification of PBA.
M. Kulmala, H. K. Lappalainen, T. Petäjä, T. Kurten, V.-M. Kerminen, Y. Viisanen, P. Hari, S. Sorvari, J. Bäck, V. Bondur, N. Kasimov, V. Kotlyakov, G. Matvienko, A. Baklanov, H. D. Guo, A. Ding, H.-C. Hansson, and S. Zilitinkevich
Atmos. Chem. Phys., 15, 13085–13096, https://doi.org/10.5194/acp-15-13085-2015, https://doi.org/10.5194/acp-15-13085-2015, 2015
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The Pan-European Experiment (PEEX) is introduced. PEEX is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. This paper outlines the mission, vision and objectives of PEEX and introduces its main components, including the research agenda, research infrastructure, knowledge transfer and potential impacts on society. The paper also summarizes the main scientific questions that PEEX is going to tackle in the future.
M. E. Salter, P. Zieger, J. C. Acosta Navarro, H. Grythe, A. Kirkevåg, B. Rosati, I. Riipinen, and E. D. Nilsson
Atmos. Chem. Phys., 15, 11047–11066, https://doi.org/10.5194/acp-15-11047-2015, https://doi.org/10.5194/acp-15-11047-2015, 2015
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We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The sea spray source function was implemented in a Lagrangian particle dispersion model and showed good skill in predicting measurements of Na+ concentration at a number of field sites, underlining its validity.
E. Hammer, N. Bukowiecki, B. P. Luo, U. Lohmann, C. Marcolli, E. Weingartner, U. Baltensperger, and C. R. Hoyle
Atmos. Chem. Phys., 15, 10309–10323, https://doi.org/10.5194/acp-15-10309-2015, https://doi.org/10.5194/acp-15-10309-2015, 2015
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An important quantity which determines aerosol activation and cloud formation is the effective peak supersaturation. The box model ZOMM was used to simulate the effective peak supersaturation experienced by an air parcel approaching a high-alpine research station in Switzerland. With the box model the sensitivity of the effective peak supersaturation to key aerosol and dynamical parameters was investigated.
K. Ruusuvuori, P. Hietala, O. Kupiainen-Määttä, T. Jokinen, H. Junninen, M. Sipilä, T. Kurtén, and H. Vehkamäki
Atmos. Meas. Tech., 8, 2577–2588, https://doi.org/10.5194/amt-8-2577-2015, https://doi.org/10.5194/amt-8-2577-2015, 2015
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Ionization reagents suitable for accurate measurements of the atmospheric gas-phase amine vapour concentrations are needed. Based on computational results, acetone is a viable option for use as an ionization reagent in CI-APi-TOF measurements on atmospheric dimethylamine. However, comparison between the computational and experimental results revealed notable discrepancies. Further study is still required before the acetone CI-APi-TOF can be considered a viable option in practice.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
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Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
G. Ganbavale, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 15, 447–493, https://doi.org/10.5194/acp-15-447-2015, https://doi.org/10.5194/acp-15-447-2015, 2015
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This study presents a new, improved parameterisation of the temperature dependence of activity coefficients implemented in the AIOMFAC group-contribution model. The AIOMFAC model with the improved parameterisation is applicable for a large variety of aqueous organic as well as water-free organic solutions of relevance for atmospheric aerosols. The new model parameters were determined based on published and new thermodynamic equilibrium data covering a temperature range from ~190 to 440 K.
J. W. Taylor, J. D. Allan, G. Allen, H. Coe, P. I. Williams, M. J. Flynn, M. Le Breton, J. B. A. Muller, C. J. Percival, D. Oram, G. Forster, J. D. Lee, A. R. Rickard, M. Parrington, and P. I. Palmer
Atmos. Chem. Phys., 14, 13755–13771, https://doi.org/10.5194/acp-14-13755-2014, https://doi.org/10.5194/acp-14-13755-2014, 2014
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We present a case study of BC wet removal by examining aerosol properties in three biomass burning plumes, one of which passed through a precipitating cloud. Nucleation scavenging preferentially removed the largest and most coated BC-containing particles. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume.
G. Allen, S. M. Illingworth, S. J. O'Shea, S. Newman, A. Vance, S. J.-B. Bauguitte, F. Marenco, J. Kent, K. Bower, M. W. Gallagher, J. Muller, C. J. Percival, C. Harlow, J. Lee, and J. P. Taylor
Atmos. Meas. Tech., 7, 4401–4416, https://doi.org/10.5194/amt-7-4401-2014, https://doi.org/10.5194/amt-7-4401-2014, 2014
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This paper presents a validated method and data set for new retrievals of trace gas concentrations and temperature from the ARIES infrared spectrometer instrument on the UK Atmospheric Research Aircraft (www.faam.ac.uk). This new capability for the aircraft will allow new science to be done because of the way it can sense information about the atmosphere without having to physically pass through it (remote sensing). This will allow us to better understand the make-up of the lower atmosphere.
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
G. Ganbavale, C. Marcolli, U. K. Krieger, A. Zuend, G. Stratmann, and T. Peter
Atmos. Chem. Phys., 14, 9993–10012, https://doi.org/10.5194/acp-14-9993-2014, https://doi.org/10.5194/acp-14-9993-2014, 2014
I. K. Ortega, T. Olenius, O. Kupiainen-Määttä, V. Loukonen, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 14, 7995–8007, https://doi.org/10.5194/acp-14-7995-2014, https://doi.org/10.5194/acp-14-7995-2014, 2014
A. Cirisan, B. P. Luo, I. Engel, F. G. Wienhold, M. Sprenger, U. K. Krieger, U. Weers, G. Romanens, G. Levrat, P. Jeannet, D. Ruffieux, R. Philipona, B. Calpini, P. Spichtinger, and T. Peter
Atmos. Chem. Phys., 14, 7341–7365, https://doi.org/10.5194/acp-14-7341-2014, https://doi.org/10.5194/acp-14-7341-2014, 2014
J. Hong, S. A. K. Häkkinen, M. Paramonov, M. Äijälä, J. Hakala, T. Nieminen, J. Mikkilä, N. L. Prisle, M. Kulmala, I. Riipinen, M. Bilde, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 4733–4748, https://doi.org/10.5194/acp-14-4733-2014, https://doi.org/10.5194/acp-14-4733-2014, 2014
P. J. Connolly, D. O. Topping, F. Malavelle, and G. McFiggans
Atmos. Chem. Phys., 14, 2289–2302, https://doi.org/10.5194/acp-14-2289-2014, https://doi.org/10.5194/acp-14-2289-2014, 2014
C. Marcolli
Atmos. Chem. Phys., 14, 2071–2104, https://doi.org/10.5194/acp-14-2071-2014, https://doi.org/10.5194/acp-14-2071-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, S. J.-B. Bauguitte, S. M. Illingworth, M. Le Breton, J. B. A. Muller, C. J. Percival, A. T. Archibald, D. E. Oram, M. Parrington, P. I. Palmer, and A. C. Lewis
Atmos. Chem. Phys., 13, 12451–12467, https://doi.org/10.5194/acp-13-12451-2013, https://doi.org/10.5194/acp-13-12451-2013, 2013
S. Bezantakos, K. Barmpounis, M. Giamarelou, E. Bossioli, M. Tombrou, N. Mihalopoulos, K. Eleftheriadis, J. Kalogiros, J. D. Allan, A. Bacak, C. J. Percival, H. Coe, and G. Biskos
Atmos. Chem. Phys., 13, 11595–11608, https://doi.org/10.5194/acp-13-11595-2013, https://doi.org/10.5194/acp-13-11595-2013, 2013
S. D. D'Andrea, S. A. K. Häkkinen, D. M. Westervelt, C. Kuang, E. J. T. Levin, V. P. Kanawade, W. R. Leaitch, D. V. Spracklen, I. Riipinen, and J. R. Pierce
Atmos. Chem. Phys., 13, 11519–11534, https://doi.org/10.5194/acp-13-11519-2013, https://doi.org/10.5194/acp-13-11519-2013, 2013
K. Ruusuvuori, T. Kurtén, I. K. Ortega, J. Faust, and H. Vehkamäki
Atmos. Chem. Phys., 13, 10397–10404, https://doi.org/10.5194/acp-13-10397-2013, https://doi.org/10.5194/acp-13-10397-2013, 2013
M. Le Breton, A. Bacak, J. B. A. Muller, S. J. O'Shea, P. Xiao, M. N. R. Ashfold, M. C. Cooke, R. Batt, D. E. Shallcross, D. E. Oram, G. Forster, S. J.-B. Bauguitte, P. I. Palmer, M. Parrington, A. C. Lewis, J. D. Lee, and C. J. Percival
Atmos. Chem. Phys., 13, 9217–9232, https://doi.org/10.5194/acp-13-9217-2013, https://doi.org/10.5194/acp-13-9217-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
A. J. Huisman, U. K. Krieger, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 13, 6647–6662, https://doi.org/10.5194/acp-13-6647-2013, https://doi.org/10.5194/acp-13-6647-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
S. J. O'Shea, S. J.-B. Bauguitte, M. W. Gallagher, D. Lowry, and C. J. Percival
Atmos. Meas. Tech., 6, 1095–1109, https://doi.org/10.5194/amt-6-1095-2013, https://doi.org/10.5194/amt-6-1095-2013, 2013
K. Kristensen, K. L. Enggrob, S. M. King, D. R. Worton, S. M. Platt, R. Mortensen, T. Rosenoern, J. D. Surratt, M. Bilde, A. H. Goldstein, and M. Glasius
Atmos. Chem. Phys., 13, 3763–3776, https://doi.org/10.5194/acp-13-3763-2013, https://doi.org/10.5194/acp-13-3763-2013, 2013
N. Bork, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 13, 3695–3703, https://doi.org/10.5194/acp-13-3695-2013, https://doi.org/10.5194/acp-13-3695-2013, 2013
E. U. Emanuelsson, M. Hallquist, K. Kristensen, M. Glasius, B. Bohn, H. Fuchs, B. Kammer, A. Kiendler-Scharr, S. Nehr, F. Rubach, R. Tillmann, A. Wahner, H.-C. Wu, and Th. F. Mentel
Atmos. Chem. Phys., 13, 2837–2855, https://doi.org/10.5194/acp-13-2837-2013, https://doi.org/10.5194/acp-13-2837-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
Related subject area
Subject: Aerosols | Technique: Laboratory Measurement | Topic: Validation and Intercomparisons
An interlaboratory comparison to quantify oxidative potential measurement in aerosol particles: challenges and recommendations for harmonisation
Quantifying the uncertainties in thermal–optical analysis of carbonaceous aircraft engine emissions: an interlaboratory study
Pressure-dependent performance of two CEN-specified condensation particle counters
Characterisation of a self-sustained, water-based condensation particle counter for aircraft cruising pressure level operation
Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations
Characterization of tandem aerosol classifiers for selecting particles: implication for eliminating the multiple charging effect
Impact of particle size, refractive index, and shape on the determination of the particle scattering coefficient – an optical closure study evaluating different nephelometer angular truncation and illumination corrections
Quantification of major particulate matter species from a single filter type using infrared spectroscopy – application to a large-scale monitoring network
Comparing black-carbon- and aerosol-absorption-measuring instruments – a new system using lab-generated soot coated with controlled amounts of secondary organic matter
Assessment of real-time bioaerosol particle counters using reference chamber experiments
Constraining the response factors of an extractive electrospray ionization mass spectrometer for near-molecular aerosol speciation
Application of the ECT9 protocol for radiocarbon-based source apportionment of carbonaceous aerosols
Intercomparison and characterization of 23 Aethalometers under laboratory and ambient air conditions: procedures and unit-to-unit variabilities
Determination of Aethalometer multiple-scattering enhancement parameters and impact on source apportionment during the winter 2017/18 EMEP/ACTRIS/COLOSSAL campaign in Milan
Laboratory validation of a compact single-scattering albedo (SSA) monitor
Facility for production of ambient-like model aerosols (PALMA) in the laboratory: application in the intercomparison of automated PM monitors with the reference gravimetric method
An interlaboratory comparison of aerosol inorganic ion measurements by ion chromatography: implications for aerosol pH estimate
Multifactor colorimetric analysis on pH-indicator papers: an optimized approach for direct determination of ambient aerosol pH
Highly oxygenated organic molecule cluster decomposition in atmospheric pressure interface time-of-flight mass spectrometers
Mass spectral characterization of primary emissions and implications in source apportionment of organic aerosol
Nitrate radical generation via continuous generation of dinitrogen pentoxide in a laminar flow reactor coupled to an oxidation flow reactor
Development of an antioxidant assay to study oxidative potential of airborne particulate matter
Determination of n-alkanes, polycyclic aromatic hydrocarbons and hopanes in atmospheric aerosol: evaluation and comparison of thermal desorption GC-MS and solvent extraction GC-MS approaches
Inter-comparison of elemental and organic carbon mass measurements from three North American national long-term monitoring networks at a co-located site
B3010: a boosted TSI 3010 condensation particle counter for airborne studies
Effect of dry or wet substrate deposition on the organic volume fraction of core–shell aerosol particles
Spectral Intensity Bioaerosol Sensor (SIBS): an instrument for spectrally resolved fluorescence detection of single particles in real time
HOx and NOx production in oxidation flow reactors via photolysis of isopropyl nitrite, isopropyl nitrite-d7, and 1,3-propyl dinitrite at λ = 254, 350, and 369 nm
Can ozone be used to calibrate aerosol photoacoustic spectrometers?
The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements
Viscosity of erythritol and erythritol–water particles as a function of water activity: new results and an intercomparison of techniques for measuring the viscosity of particles
Characterization of steady-state fluorescence properties of polystyrene latex spheres using off- and online spectroscopic methods
Organosulfates in atmospheric aerosol: synthesis and quantitative analysis of PM2.5 from Xi'an, northwestern China
Characterization of a catalyst-based conversion technique to measure total particulate nitrogen and organic carbon and comparison to a particle mass measurement instrument
On the accuracy of aerosol photoacoustic spectrometer calibrations using absorption by ozone
Evaluation of the new capture vapourizer for aerosol mass spectrometers (AMS) through laboratory studies of inorganic species
Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies
Characterization of three new condensation particle counters for sub-3 nm particle detection during the Helsinki CPC workshop: the ADI versatile water CPC, TSI 3777 nano enhancer and boosted TSI 3010
A novel single-cavity three-wavelength photoacoustic spectrometer for atmospheric aerosol research
Inter-comparison of NIOSH and IMPROVE protocols for OC and EC determination: implications for inter-protocol data conversion
Operation of the Airmodus A11 nano Condensation Nucleus Counter at various inlet pressures and various operation temperatures, and design of a new inlet system
Accuracy and precision of 14C-based source apportionment of organic and elemental carbon in aerosols using the Swiss_4S protocol
The charging of neutral dimethylamine and dimethylamine–sulfuric acid clusters using protonated acetone
Validation of the poke-flow technique combined with simulations of fluid flow for determining viscosities in samples with small volumes and high viscosities
Determination of atmospheric organosulfates using HILIC chromatography with MS detection
Characterisation and optimisation of a sample preparation method for the detection and quantification of atmospherically relevant carbonyl compounds in aqueous medium
Inter-comparison of laboratory smog chamber and flow reactor systems on organic aerosol yield and composition
ECOC comparison exercise with identical thermal protocols after temperature offset correction – instrument diagnostics by in-depth evaluation of operational parameters
An intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples
Refractory black carbon mass concentrations in snow and ice: method evaluation and inter-comparison with elemental carbon measurement
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian S. Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Aikaterina Seitanidi, Pourya Shahpoury, Eduardo J. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-107, https://doi.org/10.5194/amt-2024-107, 2024
Revised manuscript accepted for AMT
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In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP DTT assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardization in OP procedures.
Timothy A. Sipkens, Joel C. Corbin, Brett Smith, Stéphanie Gagné, Prem Lobo, Benjamin T. Brem, Mark P. Johnson, and Gregory J. Smallwood
Atmos. Meas. Tech., 17, 4291–4302, https://doi.org/10.5194/amt-17-4291-2024, https://doi.org/10.5194/amt-17-4291-2024, 2024
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Carbonaceous particles, such as soot, contribute to climate forcing, air pollution, and human health impacts. Thermal–optical analysis is a calibration standard used to measure these particles, but significant differences have been observed in the measurements across identical instruments. We report on the reproducibility of these measurements for aircraft emissions, which range from 8.0 % of the nominal value for organic carbon to 17 % for elemental carbon.
Paulus S. Bauer, Dorian Spät, Martina Eisenhut, Andreas Gattringer, and Bernadett Weinzierl
Atmos. Meas. Tech., 16, 4445–4460, https://doi.org/10.5194/amt-16-4445-2023, https://doi.org/10.5194/amt-16-4445-2023, 2023
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Particle number concentration is one of the most important parameters to quantify an aerosol. Aerosol number concentration in the nanometer range is commonly measured with condensation particle counters (CPCs). A CEN technical specification harmonizes the CPC specifications. However, it is not specified for low-pressure conditions as on high mountains or on airplanes. Here, we present the pressure-dependent performance of two different models of CEN CPCs, the Grimm 5410 CEN and the TSI 3772 CEN.
Patrick Weber, Oliver F. Bischof, Benedikt Fischer, Marcel Berg, Susanne Hering, Steven Spielman, Gregory Lewis, Andreas Petzold, and Ulrich Bundke
Atmos. Meas. Tech., 16, 3505–3514, https://doi.org/10.5194/amt-16-3505-2023, https://doi.org/10.5194/amt-16-3505-2023, 2023
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This study tests the new water condensation particle counter (MAGIC 210-LP) for deployment on passenger aircraft coordinated by the European research infrastructure IAGOS. We conducted a series of laboratory experiments for flight altitude conditions. We demonstrate that this water condensation particle counter model shows excellent agreement with a butanol-based instrument used in parallel and a Faraday cup electrometer as reference instrument at all tested pressure conditions.
Baseerat Romshoo, Mira Pöhlker, Alfred Wiedensohler, Sascha Pfeifer, Jorge Saturno, Andreas Nowak, Krzysztof Ciupek, Paul Quincey, Konstantina Vasilatou, Michaela N. Ess, Maria Gini, Konstantinos Eleftheriadis, Chris Robins, François Gaie-Levrel, and Thomas Müller
Atmos. Meas. Tech., 15, 6965–6989, https://doi.org/10.5194/amt-15-6965-2022, https://doi.org/10.5194/amt-15-6965-2022, 2022
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Black carbon (BC) is often assumed to be spherically shaped, causing uncertainties in its optical properties when modelled. This study investigates different modelling techniques for the optical properties of BC by comparing them to laboratory measurements. We provide experimental support for emphasizing the use of appropriate size representation (polydisperse size method) and morphological representation (aggregate morphology) for optical modelling and parameterization scheme development of BC.
Yao Song, Xiangyu Pei, Huichao Liu, Jiajia Zhou, and Zhibin Wang
Atmos. Meas. Tech., 15, 3513–3526, https://doi.org/10.5194/amt-15-3513-2022, https://doi.org/10.5194/amt-15-3513-2022, 2022
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Accurate particle classification is very important in aerosol studies. Differential mobility analyzers (DMAs), centrifugal particle mass analyzers (CPMAs), aerodynamic aerosol classifiers (AACs) and their tandem systems are commonly used. We demonstrated that DMA–CPMA is more susceptible to the multiple charging effect than DMA–AAC. It is not suggested to reduce the resolutions of the instruments, especially when selecting small-size soot particles.
Marilena Teri, Thomas Müller, Josef Gasteiger, Sara Valentini, Helmuth Horvath, Roberta Vecchi, Paulus Bauer, Adrian Walser, and Bernadett Weinzierl
Atmos. Meas. Tech., 15, 3161–3187, https://doi.org/10.5194/amt-15-3161-2022, https://doi.org/10.5194/amt-15-3161-2022, 2022
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We performed an extensive closure study including laboratory and simulated experiments to evaluate various angular corrections for the Aurora 4000 polar nephelometer, focusing on irregularly shaped aerosols such as mineral dust. We describe the impact of particle size, refractive index, and shape on the determination of the particle scattering coefficient and propose a guideline to establish the most appropriate angular correction depending on the aerosol type and the investigated size range.
Bruno Debus, Andrew T. Weakley, Satoshi Takahama, Kathryn M. George, Anahita Amiri-Farahani, Bret Schichtel, Scott Copeland, Anthony S. Wexler, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2685–2702, https://doi.org/10.5194/amt-15-2685-2022, https://doi.org/10.5194/amt-15-2685-2022, 2022
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In the US, routine particulate matter composition is measured on samples collected on three types of filter media and analyzed using several techniques. We propose an alternate approach that uses one analytical technique, Fourier transform-infrared spectroscopy (FT-IR), and one filter type to measure the chemical composition of particulate matter in a major US monitoring network. This method could be used to add low-cost sites to the network, fill-in missing data, or for quality control.
Daniel M. Kalbermatter, Griša Močnik, Luka Drinovec, Bradley Visser, Jannis Röhrbein, Matthias Oscity, Ernest Weingartner, Antti-Pekka Hyvärinen, and Konstantina Vasilatou
Atmos. Meas. Tech., 15, 561–572, https://doi.org/10.5194/amt-15-561-2022, https://doi.org/10.5194/amt-15-561-2022, 2022
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Soot particles with varying amounts of secondary organic matter coating were generated and used to compare a series of aerosol-absorption-measuring instruments: filter-based and photoacoustic instruments as well as photo-thermal interferometers. Significant deviations in the response of the instruments were observed depending on the amount of secondary organic coating. The system can be used for the inter-comparison and characterisation of instruments.
Gian Lieberherr, Kevin Auderset, Bertrand Calpini, Bernard Clot, Benoît Crouzy, Martin Gysel-Beer, Thomas Konzelmann, José Manzano, Andrea Mihajlovic, Alireza Moallemi, David O'Connor, Branko Sikoparija, Eric Sauvageat, Fiona Tummon, and Konstantina Vasilatou
Atmos. Meas. Tech., 14, 7693–7706, https://doi.org/10.5194/amt-14-7693-2021, https://doi.org/10.5194/amt-14-7693-2021, 2021
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Today there is no standard procedure to validate bioaerosol and pollen monitors. Three instruments were tested, focusing on detecting particles of different sizes. Only one instrument was able to detect the smallest particles (0.5 µm Ø), whereas the others performed best at the largest tested particles (10 µm Ø). These results are the first step towards a standardised validation procedure. The need for a reference counting method for larger particles (pollen grains: 10–200 µm Ø) was emphasised.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Lin Huang, Wendy Zhang, Guaciara M. Santos, Blanca T. Rodríguez, Sandra R. Holden, Vincent Vetro, and Claudia I. Czimczik
Atmos. Meas. Tech., 14, 3481–3500, https://doi.org/10.5194/amt-14-3481-2021, https://doi.org/10.5194/amt-14-3481-2021, 2021
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Radiocarbon (14C)-based source apportionment of aerosol carbon fractions requires the physical separation of OC from EC and minimizing of the incorporation of extraneous carbon. Using pure and mixed reference materials ranging in age from modern to fossil, we show that the ECT9 protocol effectively isolates OC and EC. This work expands existing opportunities for characterizing and monitoring sources of carbonaceous aerosols, including µg C-sized samples from the Arctic.
Andrea Cuesta-Mosquera, Griša Močnik, Luka Drinovec, Thomas Müller, Sascha Pfeifer, María Cruz Minguillón, Björn Briel, Paul Buckley, Vadimas Dudoitis, Javier Fernández-García, María Fernández-Amado, Joel Ferreira De Brito, Veronique Riffault, Harald Flentje, Eimear Heffernan, Nikolaos Kalivitis, Athina-Cerise Kalogridis, Hannes Keernik, Luminita Marmureanu, Krista Luoma, Angela Marinoni, Michael Pikridas, Gerhard Schauer, Norbert Serfozo, Henri Servomaa, Gloria Titos, Jesús Yus-Díez, Natalia Zioła, and Alfred Wiedensohler
Atmos. Meas. Tech., 14, 3195–3216, https://doi.org/10.5194/amt-14-3195-2021, https://doi.org/10.5194/amt-14-3195-2021, 2021
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Measurements of black carbon must be conducted with instruments operating in quality-checked and assured conditions to generate reliable and comparable data. Here, 23 Aethalometers monitoring black carbon mass concentrations in European networks were characterized and intercompared. The influence of different aerosol sources, maintenance activities, and the filter material on the instrumental variabilities were investigated. Good agreement and in general low deviations were seen.
Vera Bernardoni, Luca Ferrero, Ezio Bolzacchini, Alice Corina Forello, Asta Gregorič, Dario Massabò, Griša Močnik, Paolo Prati, Martin Rigler, Luca Santagostini, Francesca Soldan, Sara Valentini, Gianluigi Valli, and Roberta Vecchi
Atmos. Meas. Tech., 14, 2919–2940, https://doi.org/10.5194/amt-14-2919-2021, https://doi.org/10.5194/amt-14-2919-2021, 2021
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An instrument-dependent wavelength-independent parameter (C) is often used to face multiple-scattering issues affecting aerosol light absorption measurements by Aethalometers. Instead, we determined multi-wavelength C by comparison with absorption measurements of samples collected in parallel performed by an instrument developed in-house. Considering C wavelength dependence, harmonized results were obtained applying source and component apportionment models to data from different Aethalometers.
Julia Perim de Faria, Ulrich Bundke, Andrew Freedman, Timothy B. Onasch, and Andreas Petzold
Atmos. Meas. Tech., 14, 1635–1653, https://doi.org/10.5194/amt-14-1635-2021, https://doi.org/10.5194/amt-14-1635-2021, 2021
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An evaluation of the performance and accuracy of a Cavity Attenuated Phase-Shift Single Scattering Albedo Monitor (CAPS PMSSA; Aerodyne Research, Inc.) was conducted in an optical-closure study with proven technologies for aerosol particle optical-property measurements. This study demonstrates that the CAPS PMSSA is a robust and reliable instrument for the direct measurement of the particle scattering and extinction coefficients and thus single-scattering albedo.
Stefan Horender, Kevin Auderset, Paul Quincey, Stefan Seeger, Søren Nielsen Skov, Kai Dirscherl, Thomas O. M. Smith, Katie Williams, Camille C. Aegerter, Daniel M. Kalbermatter, François Gaie-Levrel, and Konstantina Vasilatou
Atmos. Meas. Tech., 14, 1225–1238, https://doi.org/10.5194/amt-14-1225-2021, https://doi.org/10.5194/amt-14-1225-2021, 2021
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A new facility has been developed which allows for the stable and reproducible generation of ambient-like model aerosols in the laboratory. The set-up consists of multiple aerosol generators, a custom-made flow tube homogeniser, isokinetic sampling probes, and a system to control aerosol temperature and humidity. The model aerosols, which contain fresh and aged soot, inorganic salt, and dust particles, can be used for the calibration of air quality monitoring instruments.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Guo Li, Hang Su, Nan Ma, Guangjie Zheng, Uwe Kuhn, Meng Li, Thomas Klimach, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 13, 6053–6065, https://doi.org/10.5194/amt-13-6053-2020, https://doi.org/10.5194/amt-13-6053-2020, 2020
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Aerosol acidity plays an important role in regulating the chemistry, health, and ecological effect of aerosol particles. However, a direct measurement of aerosol pH is very challenging because of its fast transition and equilibrium with adjacent environments. Therefore, most early studies have to use modeled pH, resulting in intensive debates about model uncertainties. Here we developed an optimized approach to measure aerosol pH by using pH-indicator papers combined with RGB-based colorimetry.
Tommaso Zanca, Jakub Kubečka, Evgeni Zapadinsky, Monica Passananti, Theo Kurtén, and Hanna Vehkamäki
Atmos. Meas. Tech., 13, 3581–3593, https://doi.org/10.5194/amt-13-3581-2020, https://doi.org/10.5194/amt-13-3581-2020, 2020
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In this paper we quantify (using a statistical model) the probability of decomposition of a representative class of HOM clusters in an APi-TOF mass spectrometer. This is important because it quantifies the systematic error of measurements in a APi-TOF MS due to cluster decomposition. The results (specific for our selected clusters) show that decomposition is negligible, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
Pourya Shahpoury, Tom Harner, Gerhard Lammel, Steven Lelieveld, Haijie Tong, and Jake Wilson
Atmos. Meas. Tech., 12, 6529–6539, https://doi.org/10.5194/amt-12-6529-2019, https://doi.org/10.5194/amt-12-6529-2019, 2019
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789, https://doi.org/10.5194/amt-12-4779-2019, https://doi.org/10.5194/amt-12-4779-2019, 2019
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The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Tak W. Chan, Lin Huang, Kulbir Banwait, Wendy Zhang, Darrell Ernst, Xiaoliang Wang, John G. Watson, Judith C. Chow, Mark Green, Claudia I. Czimczik, Guaciara M. Santos, Sangeeta Sharma, and Keith Jones
Atmos. Meas. Tech., 12, 4543–4560, https://doi.org/10.5194/amt-12-4543-2019, https://doi.org/10.5194/amt-12-4543-2019, 2019
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This study compared 10 years of carbonaceous aerosol measurements collected at Egbert by three North American long-term monitoring networks. The study evaluated how differences in sample collection and analysis affected the concentrations of total carbon (TC), organic carbon (OC), and elemental carbon (EC). Various carbonaceous fractions measured by the three networks were consistent and comparable over the period. Elevated OC and EC were observed when ambient temperature exceeded 10 °C.
David Picard, Michel Attoui, and Karine Sellegri
Atmos. Meas. Tech., 12, 2531–2543, https://doi.org/10.5194/amt-12-2531-2019, https://doi.org/10.5194/amt-12-2531-2019, 2019
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We report here how we managed to improve the performance of an aerosol particle counter model TSI3010. Our device is based on a secondhand unit and reuses its core elements (saturator, condenser, optics). We redesigned the electronics and thermal management. Laboratory experiments show that the cutoff diameter was decreased from 10 to 2.5 nm, bringing the B3010 close to more complex and expensive products. These results may help designers and users improve the performance of their devices.
Hansol D. Lee, Chathuri P. Kaluarachchi, Elias S. Hasenecz, Jonic Z. Zhu, Eduard Popa, Elizabeth A. Stone, and Alexei V. Tivanski
Atmos. Meas. Tech., 12, 2033–2042, https://doi.org/10.5194/amt-12-2033-2019, https://doi.org/10.5194/amt-12-2033-2019, 2019
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Dry and wet aerosol deposition modes are commonly used to collect particles on a solid substrate for experiments. We demonstrate, using single-particle microscopy and bulk methods, how the substrate-deposited particles with two components can yield the same core–shell morphology but different shell thicknesses depending on the deposition method. Thus we strongly advise future works to use wet deposition when possible to obtain accurate assessment of the single-particle organic volume fraction.
Tobias Könemann, Nicole Savage, Thomas Klimach, David Walter, Janine Fröhlich-Nowoisky, Hang Su, Ulrich Pöschl, J. Alex Huffman, and Christopher Pöhlker
Atmos. Meas. Tech., 12, 1337–1363, https://doi.org/10.5194/amt-12-1337-2019, https://doi.org/10.5194/amt-12-1337-2019, 2019
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This study presents a comprehensive assessment of the SIBS, an instrument for spectrally resolved fluorescence detection of single particles. Exemplary ambient data and fluorescence spectra obtained for 16 reference compounds (biofluorophores and PSLs) show that the SIBS has the ability to expand the scope of fluorescent bioaerosol quantification and classification. Detailed technical insights will be broadly beneficial for users of various WIBS generations and other LIF instruments.
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
D. Al Fischer and Geoffrey D. Smith
Atmos. Meas. Tech., 11, 6419–6427, https://doi.org/10.5194/amt-11-6419-2018, https://doi.org/10.5194/amt-11-6419-2018, 2018
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Photoacoustic spectroscopy is a commonly used technique for measuring light absorption by aerosols, but it requires careful calibration to be accurate. Here, we explore the use of one popular calibrant, ozone, and demonstrate that its response is dependent on the identity of the bath gas used.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Yangxi Chu, Erin Evoy, Saeid Kamal, Young Chul Song, Jonathan P. Reid, Chak K. Chan, and Allan K. Bertram
Atmos. Meas. Tech., 11, 4809–4822, https://doi.org/10.5194/amt-11-4809-2018, https://doi.org/10.5194/amt-11-4809-2018, 2018
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The viscosity of erythritol, a tetrol found in aerosol particles, is highly uncertain. To help resolve this uncertainty, we measured the viscosities of
erythritol–water particles using rectangular-area fluorescence recovery after photobleaching and aerosol optical tweezers techniques. These results
should help improve the understanding of the viscosity of secondary organic aerosol particles. In addition, we present an intercomparison of techniques
for measuring the viscosity of particles.
Tobias Könemann, Nicole J. Savage, J. Alex Huffman, and Christopher Pöhlker
Atmos. Meas. Tech., 11, 3987–4003, https://doi.org/10.5194/amt-11-3987-2018, https://doi.org/10.5194/amt-11-3987-2018, 2018
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This study presents an overview of fluorescence properties of polystyrene latex spheres (PSLs), which are widely used in numerous scientific disciplines. By using different spectroscopic techniques, we show that the
fluorescence landscapeof PSLs is more complex than the information provided by manufacturers may imply. By understanding general fluorescence properties of PSLs, individual researchers may probe specific spectral features important to the operation of their own instruments.
Ru-Jin Huang, Junji Cao, Yang Chen, Lu Yang, Jincan Shen, Qihua You, Kai Wang, Chunshui Lin, Wei Xu, Bo Gao, Yongjie Li, Qi Chen, Thorsten Hoffmann, Colin D. O'Dowd, Merete Bilde, and Marianne Glasius
Atmos. Meas. Tech., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, https://doi.org/10.5194/amt-11-3447-2018, 2018
Chelsea E. Stockwell, Agnieszka Kupc, Bartłomiej Witkowski, Ranajit K. Talukdar, Yong Liu, Vanessa Selimovic, Kyle J. Zarzana, Kanako Sekimoto, Carsten Warneke, Rebecca A. Washenfelder, Robert J. Yokelson, Ann M. Middlebrook, and James M. Roberts
Atmos. Meas. Tech., 11, 2749–2768, https://doi.org/10.5194/amt-11-2749-2018, https://doi.org/10.5194/amt-11-2749-2018, 2018
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This work investigates the total conversion of particle-bound nitrogen and organic carbon across platinum and molybdenum catalysts followed by NO–O3 chemiluminescence and nondispersive infrared CO2 detection. We show the instrument is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation through comparisons with a calibrated particle-into-liquid sampler coupled to an electrospray ionization source of a mass spectrometer.
Nicholas W. Davies, Michael I. Cotterell, Cathryn Fox, Kate Szpek, Jim M. Haywood, and Justin M. Langridge
Atmos. Meas. Tech., 11, 2313–2324, https://doi.org/10.5194/amt-11-2313-2018, https://doi.org/10.5194/amt-11-2313-2018, 2018
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The poorly characterised optical properties of atmospheric aerosols are one of the major uncertainties when modelling future climate change. Photoacoustic spectroscopy is an accurate and sensitive method for measurement of aerosol light absorption. Photoacoustic spectrometers require calibration; hence this study validates the use of ozone as a calibrant and simultaneously verifies the accuracy of the photoacoustic spectrometers in question.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Juha Kangasluoma, Susanne Hering, David Picard, Gregory Lewis, Joonas Enroth, Frans Korhonen, Markku Kulmala, Karine Sellegri, Michel Attoui, and Tuukka Petäjä
Atmos. Meas. Tech., 10, 2271–2281, https://doi.org/10.5194/amt-10-2271-2017, https://doi.org/10.5194/amt-10-2271-2017, 2017
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The manuscript presents a characterization of three new particle counters able to detect airborne nanoparticles smaller than 3 nm in diameter. We explored some of the parameters affecting the smallest detectable particle size, such as sample flow relative humidity, the particle chemical composition and the electrical charging state. The characterization results help one to select a suitable particle counter for a given application.
Claudia Linke, Inas Ibrahim, Nina Schleicher, Regina Hitzenberger, Meinrat O. Andreae, Thomas Leisner, and Martin Schnaiter
Atmos. Meas. Tech., 9, 5331–5346, https://doi.org/10.5194/amt-9-5331-2016, https://doi.org/10.5194/amt-9-5331-2016, 2016
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Various carbonaceous materials are present in the atmosphere. Besides gaseous organic compounds, carbonaceous particles like soot are emitted into the air from traffic sources, residential wood combustion, or wildfires. Variable chemical compositions of such materials, which often result from incomplete combustion processes, show differences in the absorption behavior at visible wavelengths. Our instrument is able to measure the absorption at three visible wavelengths.
Cheng Wu, X. H. Hilda Huang, Wai Man Ng, Stephen M. Griffith, and Jian Zhen Yu
Atmos. Meas. Tech., 9, 4547–4560, https://doi.org/10.5194/amt-9-4547-2016, https://doi.org/10.5194/amt-9-4547-2016, 2016
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Organic carbon (OC) and elemental carbon (EC) in more than 1300 Hong Kong samples were analyzed using both NIOSH TOT and IMPROVE TOR protocols. EC discrepancy between the two protocols mainly (83 %) arises from a difference in peak inert mode temperature, while the rest (17 %) is attributed to a difference in the optical method (transmittance vs. reflectance) applied for the charring correction. Two approaches are proposed to translate NIOSH TOT OC and EC data into IMPROVE TOR OC and EC data.
Juha Kangasluoma, Alessandro Franchin, Jonahtan Duplissy, Lauri Ahonen, Frans Korhonen, Michel Attoui, Jyri Mikkilä, Katrianne Lehtipalo, Joonas Vanhanen, Markku Kulmala, and Tuukka Petäjä
Atmos. Meas. Tech., 9, 2977–2988, https://doi.org/10.5194/amt-9-2977-2016, https://doi.org/10.5194/amt-9-2977-2016, 2016
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The paper describes technical aspects of using the Airmodus A11 nCNC at various inlet pressures and how temperature selection affects the performance of the instrument. We also present a sampling box to minimize the inlet losses and make use of the instrument more convenient.
G. O. Mouteva, S. M. Fahrni, G. M. Santos, J. T. Randerson, Y.-L. Zhang, S. Szidat, and C. I. Czimczik
Atmos. Meas. Tech., 8, 3729–3743, https://doi.org/10.5194/amt-8-3729-2015, https://doi.org/10.5194/amt-8-3729-2015, 2015
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We describe a stepwise uncertainty analysis of 14C measurements of organic (OC) and elemental (EC) carbon fractions of aerosols. Using the Swiss_4S thermal-optical protocol with a newly established trapping setup, we show that we can efficiently isolate and trap each carbon fraction and perform 14C analysis of ultra-small OC and EC samples with high accuracy and low 14C blanks. Our study presents a first step towards the development of a common protocol for OC and EC 14C measurements.
K. Ruusuvuori, P. Hietala, O. Kupiainen-Määttä, T. Jokinen, H. Junninen, M. Sipilä, T. Kurtén, and H. Vehkamäki
Atmos. Meas. Tech., 8, 2577–2588, https://doi.org/10.5194/amt-8-2577-2015, https://doi.org/10.5194/amt-8-2577-2015, 2015
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Ionization reagents suitable for accurate measurements of the atmospheric gas-phase amine vapour concentrations are needed. Based on computational results, acetone is a viable option for use as an ionization reagent in CI-APi-TOF measurements on atmospheric dimethylamine. However, comparison between the computational and experimental results revealed notable discrepancies. Further study is still required before the acetone CI-APi-TOF can be considered a viable option in practice.
J. W. Grayson, M. Song, M. Sellier, and A. K. Bertram
Atmos. Meas. Tech., 8, 2463–2472, https://doi.org/10.5194/amt-8-2463-2015, https://doi.org/10.5194/amt-8-2463-2015, 2015
A. P. S. Hettiyadura, E. A. Stone, S. Kundu, Z. Baker, E. Geddes, K. Richards, and T. Humphry
Atmos. Meas. Tech., 8, 2347–2358, https://doi.org/10.5194/amt-8-2347-2015, https://doi.org/10.5194/amt-8-2347-2015, 2015
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Organosulfates are SOA products that have proven difficult to quantify. This study addresses the need for authentic quantification standards with a straightforward approach to synthesizing highly pure organosulfate potassium salts. New standards are used to develop a new separation protocol for small, functionalized organosulfates. Upon validation, this method is used to assess sample preparation protocols and to make new measurements of organosulfates in Centreville, Alabama.
M. Rodigast, A. Mutzel, Y. Iinuma, S. Haferkorn, and H. Herrmann
Atmos. Meas. Tech., 8, 2409–2416, https://doi.org/10.5194/amt-8-2409-2015, https://doi.org/10.5194/amt-8-2409-2015, 2015
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An optimised method for derivatisation of carbonyl compounds with o-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine (PFBHA) in aqueous samples is described. The comprehensive optimisation of the method leads to an improvement of the detection limit up to a factor of 10 highlighting the good sensitivity of the optimised method for atmospherically relevant carbonyl compounds. The optimised method was successfully applied to detect carbonyl compounds from the aqueous phase oxidation of 3-methylbutanone.
E. A. Bruns, I. El Haddad, A. Keller, F. Klein, N. K. Kumar, S. M. Pieber, J. C. Corbin, J. G. Slowik, W. H. Brune, U. Baltensperger, and A. S. H. Prévôt
Atmos. Meas. Tech., 8, 2315–2332, https://doi.org/10.5194/amt-8-2315-2015, https://doi.org/10.5194/amt-8-2315-2015, 2015
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Short summary
Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the...
