Articles | Volume 14, issue 11
https://doi.org/10.5194/amt-14-6955-2021
© Author(s) 2021. 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-14-6955-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Constraining the response factors of an extractive electrospray ionization mass spectrometer for near-molecular aerosol speciation
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Chuan Ping Lee
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Jordan E. Krechmer
Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc.,
Billerica, Massachusetts 01821, United States
Francesca Majluf
Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc.,
Billerica, Massachusetts 01821, United States
Yandong Tong
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Manjula R. Canagaratna
Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc.,
Billerica, Massachusetts 01821, United States
Julia Schmale
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Extreme Environments Research Laboratory, École Polytechnique
Fédérale de Lausanne, 1951 Sion, Switzerland
André S. H. Prévôt
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Urs Baltensperger
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Josef Dommen
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Jay G. Slowik
CORRESPONDING AUTHOR
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
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Benjamin C. Sapper, Sean Youn, Daven K. Henze, Manjula Canagaratna, Harald Stark, and Jose L. Jimenez
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Laura Cadeo, Beatrice Biffi, Benjamin Chazeau, Cristina Colombi, Rosario Cosenza, Eleonora Cuccia, Manousos-Ioannis Manousakas, Kaspar R. Daellenbach, André S. H. Prévôt, and Roberta Vecchi
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Brice Barret, Patrice Medina, Natalie Brett, Roman Pohorsky, Kathy S. Law, Slimane Bekki, Gilberto J. Fochesatto, Julia Schmale, Steve R. Arnold, Andrea Baccarini, Maurizio Busetto, Meeta Cesler-Maloney, Barbara D'Anna, Stefano Decesari, Jingqiu Mao, Gianluca Pappaccogli, Joel Savarino, Federico Scoto, and William R. Simpson
Atmos. Meas. Tech., 18, 1163–1184, https://doi.org/10.5194/amt-18-1163-2025, https://doi.org/10.5194/amt-18-1163-2025, 2025
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The Fairbanks area experiences severe pollution episodes in winter because of enhanced emissions of pollutants trapped near the surface by strong temperature inversions. Low-cost sensors were deployed on board a car and a tethered balloon to measure the concentrations of gaseous pollutants (CO, O3, and NOx) in Fairbanks during winter 2022. Data calibration with reference measurements and machine learning methods enabled us to document pollution at the surface and power plant plumes aloft.
Tiantian Wang, Jun Zhang, Houssni Lamkaddam, Kun Li, Ka Yuen Cheung, Lisa Kattner, Erlend Gammelsæter, Michael Bauer, Zachary C. J. Decker, Deepika Bhattu, Rujin Huang, Rob L. Modini, Jay G. Slowik, Imad El Haddad, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 25, 2707–2724, https://doi.org/10.5194/acp-25-2707-2025, https://doi.org/10.5194/acp-25-2707-2025, 2025
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Our study analyzes real-time emissions of organic vapors from solid fuel combustion. Using the mass spectrometer, we tested various fuels, finding higher emission factors for organic vapors from wood burning. Intermediate-volatility organic compounds constituted a significant fraction of emissions in solid fuel combustion. Statistical tests identified unique potential markers. Our insights benefit air quality, climate, and health, aiding accurate emission assessments.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
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Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiia Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
Atmos. Chem. Phys., 25, 2207–2241, https://doi.org/10.5194/acp-25-2207-2025, https://doi.org/10.5194/acp-25-2207-2025, 2025
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Limited aerosol measurements in the central Arctic hinder our understanding of aerosol–climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Local wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
Yugo Kanaya, Roberto Sommariva, Alfonso Saiz-Lopez, Andrea Mazzeo, Theodore K. Koenig, Kaori Kawana, James E. Johnson, Aurélie Colomb, Pierre Tulet, Suzie Molloy, Ian E. Galbally, Rainer Volkamer, Anoop Mahajan, John W. Halfacre, Paul B. Shepson, Julia Schmale, Hélène Angot, Byron Blomquist, Matthew D. Shupe, Detlev Helmig, Junsu Gil, Meehye Lee, Sean C. Coburn, Ivan Ortega, Gao Chen, James Lee, Kenneth C. Aikin, David D. Parrish, John S. Holloway, Thomas B. Ryerson, Ilana B. Pollack, Eric J. Williams, Brian M. Lerner, Andrew J. Weinheimer, Teresa Campos, Frank M. Flocke, J. Ryan Spackman, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Ralf M. Staebler, Amir A. Aliabadi, Wanmin Gong, Roeland Van Malderen, Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Juan Carlos Gómez Martin, Masatomo Fujiwara, Katie Read, Matthew Rowlinson, Keiichi Sato, Junichi Kurokawa, Yoko Iwamoto, Fumikazu Taketani, Hisahiro Takashima, Monica Navarro Comas, Marios Panagi, and Martin G. Schultz
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-566, https://doi.org/10.5194/essd-2024-566, 2025
Revised manuscript accepted for ESSD
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The first comprehensive dataset of tropospheric ozone over oceans/polar regions is presented, including 77 ship/buoy and 48 aircraft campaign observations (1977–2022, 0–5000 m altitude), supplemented by ozonesonde and surface data. Air masses isolated from land for 72+ hours are systematically selected as essentially oceanic. Among the 11 global regions, they show daytime decreases of 10–16% in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
Sophie Bogler, Jun Zhang, Rico K. Y. Cheung, Kun Li, Andre S. H. Prevot, Imad El Haddad, and David M. Bell
EGUsphere, https://doi.org/10.5194/egusphere-2025-385, https://doi.org/10.5194/egusphere-2025-385, 2025
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Authentic aerosols emitted from residential wood stoves and open burning processes are only slightly oxidized by ozone in the atmosphere. Under dry conditions the reaction does not proceed to completion, while under high humidity conditions the reactivity proceeds further. These results indicate the reactivity with ozone is likely impacted by aerosol phase state (e.g. aerosol viscosity).
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
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We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
Imad El Haddad, Danielle Vienneau, Kaspar R. Daellenbach, Robin Modini, Jay G. Slowik, Abhishek Upadhyay, Petros N. Vasilakos, David Bell, Kees de Hoogh, and Andre S. H. Prevot
Atmos. Chem. Phys., 24, 11981–12011, https://doi.org/10.5194/acp-24-11981-2024, https://doi.org/10.5194/acp-24-11981-2024, 2024
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing on the most harmful anthropogenic emissions. We highlight key observations, modelling developments, and emission measurements needed to achieve this shift.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech., 17, 2387–2400, https://doi.org/10.5194/amt-17-2387-2024, https://doi.org/10.5194/amt-17-2387-2024, 2024
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In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During the Cloud–Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini aerosol mass spectrometers analyse the particles on which clouds form. The seeded clouds showed higher concentrations of chlorine and potassium, the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
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Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Roman Pohorsky, Andrea Baccarini, Julie Tolu, Lenny H. E. Winkel, and Julia Schmale
Atmos. Meas. Tech., 17, 731–754, https://doi.org/10.5194/amt-17-731-2024, https://doi.org/10.5194/amt-17-731-2024, 2024
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This manuscript presents a new tethered-balloon-based platform for in situ vertical measurements of aerosols and trace gases in the lower atmosphere of polar and alpine regions. The system can host various instrumental setups to target different research questions and features new instruments, in particular a miniaturized scanning electrical mobility spectrometer, deployed for the first time in a tethered balloon.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
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PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
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.
Mitchell W. Alton, Harald J. Stark, Manjula R. Canagaratna, and Eleanor C. Browne
Atmos. Meas. Tech., 16, 3273–3282, https://doi.org/10.5194/amt-16-3273-2023, https://doi.org/10.5194/amt-16-3273-2023, 2023
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Mass spectrometric measurements of atmospheric composition routinely detect hundreds of different ions of varying chemical composition, creating challenges for visualization and data interpretation. We present a new analysis technique to facilitate visualization, while providing greater chemical insight. Additionally, it can aid in identifying the chemical composition of ions. A graphical user interface for performing the analysis is introduced and freely available, enabling broad applications.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Joschka Pfeifer, Naser G. A. Mahfouz, Benjamin C. Schulze, Serge Mathot, Dominik Stolzenburg, Rima Baalbaki, Zoé Brasseur, Lucia Caudillo, Lubna Dada, Manuel Granzin, Xu-Cheng He, Houssni Lamkaddam, Brandon Lopez, Vladimir Makhmutov, Ruby Marten, Bernhard Mentler, Tatjana Müller, Antti Onnela, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Meredith Schervish, Ping Tian, Nsikanabasi S. Umo, Dongyu S. Wang, Mingyi Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Antonio Amorim, Imad El Haddad, Markku Kulmala, Katrianne Lehtipalo, Tuukka Petäjä, António Tomé, Sander Mirme, Hanna E. Manninen, Neil M. Donahue, Richard C. Flagan, Andreas Kürten, Joachim Curtius, and Jasper Kirkby
Atmos. Chem. Phys., 23, 6703–6718, https://doi.org/10.5194/acp-23-6703-2023, https://doi.org/10.5194/acp-23-6703-2023, 2023
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Attachment rate coefficients between ions and charged aerosol particles determine their lifetimes and may also influence cloud dynamics and aerosol processing. Here we present novel experiments that measure ion–aerosol attachment rate coefficients for multiply charged aerosol particles under atmospheric conditions in the CERN CLOUD chamber. Our results provide experimental discrimination between various theoretical models.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Vaishali Jain, Nidhi Tripathi, Sachchida N. Tripathi, Mansi Gupta, Lokesh K. Sahu, Vishnu Murari, Sreenivas Gaddamidi, Ashutosh K. Shukla, and Andre S. H. Prevot
Atmos. Chem. Phys., 23, 3383–3408, https://doi.org/10.5194/acp-23-3383-2023, https://doi.org/10.5194/acp-23-3383-2023, 2023
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This research chemically characterises 173 different NMVOCs (non-methane volatile organic compounds) measured in real time for three seasons in the city of the central Indo-Gangetic basin of India, Lucknow. Receptor modelling is used to analyse probable sources of NMVOCs and their crucial role in forming ozone and secondary organic aerosols. It is observed that vehicular emissions and solid fuel combustion are the highest contributors to the emission of primary and secondary NMVOCs.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
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The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech., 15, 7265–7291, https://doi.org/10.5194/amt-15-7265-2022, https://doi.org/10.5194/amt-15-7265-2022, 2022
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
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.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Jerome D. Fast, David M. Bell, Gourihar Kulkarni, Jiumeng Liu, Fan Mei, Georges Saliba, John E. Shilling, Kaitlyn Suski, Jason Tomlinson, Jian Wang, Rahul Zaveri, and Alla Zelenyuk
Atmos. Chem. Phys., 22, 11217–11238, https://doi.org/10.5194/acp-22-11217-2022, https://doi.org/10.5194/acp-22-11217-2022, 2022
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Recent aircraft measurements from the HI-SCALE campaign conducted over the Southern Great Plains (SGP) site in Oklahoma are used to quantify spatial variability of aerosol properties in terms of grid spacings typically used by weather and climate models. Surprisingly large horizontal gradients in aerosol properties were frequently observed in this rural area. This spatial variability can be used as an uncertainty range when comparing surface point measurements with model predictions.
Yutong Liang, Christos Stamatis, Edward C. Fortner, Rebecca A. Wernis, Paul Van Rooy, Francesca Majluf, Tara I. Yacovitch, Conner Daube, Scott C. Herndon, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 9877–9893, https://doi.org/10.5194/acp-22-9877-2022, https://doi.org/10.5194/acp-22-9877-2022, 2022
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This article reports the measurements of organic compounds emitted from western US wildfires. We identified and quantified 240 particle-phase compounds and 72 gas-phase compounds emitted in wildfire and related the emissions to the modified combustion efficiency. Higher emissions of diterpenoids and monoterpenes were observed, likely due to distillation from unburned heated vegetation. Our results can benefit future source apportionment and modeling studies as well as exposure assessments.
Christian Tatzelt, Silvia Henning, André Welti, Andrea Baccarini, Markus Hartmann, Martin Gysel-Beer, Manuela van Pinxteren, Robin L. Modini, Julia Schmale, and Frank Stratmann
Atmos. Chem. Phys., 22, 9721–9745, https://doi.org/10.5194/acp-22-9721-2022, https://doi.org/10.5194/acp-22-9721-2022, 2022
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We present the abundance and origin of cloud-relevant aerosol particles in the preindustral-like conditions of the Southern Ocean (SO) during austral summer. Cloud condensation nuclei (CCN) and ice-nucleating particles (INP) were measured during a circum-Antarctic scientific cruise with in situ instrumentation and offline filter measurements, respectively. Transport processes were found to play an equally important role as local sources for both the CCN and INP population of the SO.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Andrew J. Lindsay, Daniel C. Anderson, Rebecca A. Wernis, Yutong Liang, Allen H. Goldstein, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Ed C. Fortner, Philip L. Croteau, Francesca Majluf, Jordan E. Krechmer, Tara I. Yacovitch, Walter B. Knighton, and Ezra C. Wood
Atmos. Chem. Phys., 22, 4909–4928, https://doi.org/10.5194/acp-22-4909-2022, https://doi.org/10.5194/acp-22-4909-2022, 2022
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Wildfire smoke dramatically impacts air quality and often has elevated concentrations of ozone. We present measurements of ozone and its precursors at a rural site periodically impacted by wildfire smoke. Measurements of total peroxy radicals, key ozone precursors that have been studied little within wildfires, compare well with chemical box model predictions. Our results indicate no serious issues with using current chemistry mechanisms to model chemistry in aged wildfire plumes.
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.
Julia Schmale, Sangeeta Sharma, Stefano Decesari, Jakob Pernov, Andreas Massling, Hans-Christen Hansson, Knut von Salzen, Henrik Skov, Elisabeth Andrews, Patricia K. Quinn, Lucia M. Upchurch, Konstantinos Eleftheriadis, Rita Traversi, Stefania Gilardoni, Mauro Mazzola, James Laing, and Philip Hopke
Atmos. Chem. Phys., 22, 3067–3096, https://doi.org/10.5194/acp-22-3067-2022, https://doi.org/10.5194/acp-22-3067-2022, 2022
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Long-term data sets of Arctic aerosol properties from 10 stations across the Arctic provide evidence that anthropogenic influence on the Arctic atmospheric chemical composition has declined in winter, a season which is typically dominated by mid-latitude emissions. The number of significant trends in summer is smaller than in winter, and overall the pattern is ambiguous with some significant positive and negative trends. This reflects the mixed influence of natural and anthropogenic emissions.
Juliana Gil-Loaiza, Joseph R. Roscioli, Joanne H. Shorter, Till H. M. Volkmann, Wei-Ren Ng, Jordan E. Krechmer, and Laura K. Meredith
Biogeosciences, 19, 165–185, https://doi.org/10.5194/bg-19-165-2022, https://doi.org/10.5194/bg-19-165-2022, 2022
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We evaluated a new diffusive soil probe integrated with high-resolution gas analyzers to measure soil gases in real time at a centimeter scale. Using columns with simple silica and soil, we captured changes in carbon dioxide (CO2), volatile organic compounds (VOCs), and nitrous oxide (N2O) with its isotopes to distinguish potential nutrient sources and microbial metabolism. This approach will advance the use of soil gases as important signals to understand and monitor soil fertility and health.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
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The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
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Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
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.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Benjamin Sumlin, Edward Fortner, Andrew Lambe, Nishit J. Shetty, Conner Daube, Pai Liu, Francesca Majluf, Scott Herndon, and Rajan K. Chakrabarty
Atmos. Chem. Phys., 21, 11843–11856, https://doi.org/10.5194/acp-21-11843-2021, https://doi.org/10.5194/acp-21-11843-2021, 2021
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We present a comparison of the changes to light absorption behavior and chemical composition of wildfire smoke particles from day- and nighttime oxidation processes and discuss the results within the context of previous laboratory findings.
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.
Congbo Song, Manuel Dall'Osto, Angelo Lupi, Mauro Mazzola, Rita Traversi, Silvia Becagli, Stefania Gilardoni, Stergios Vratolis, Karl Espen Yttri, David C. S. Beddows, Julia Schmale, James Brean, Agung Ghani Kramawijaya, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 11317–11335, https://doi.org/10.5194/acp-21-11317-2021, https://doi.org/10.5194/acp-21-11317-2021, 2021
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We present a cluster analysis of relatively long-term (2015–2019) aerosol aerodynamic volume size distributions up to 20 μm in the Arctic for the first time. The study found that anthropogenic and natural aerosols comprised 27 % and 73 % of the occurrence of the coarse-mode aerosols, respectively. Our study shows that about two-thirds of the coarse-mode aerosols are related to two sea-spray-related aerosol clusters, indicating that sea spray aerosol may more complex in the Arctic environment.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Mutian Ma, Laura-Hélèna Rivellini, YuXi Cui, Megan D. Willis, Rio Wilkie, Jonathan P. D. Abbatt, Manjula R. Canagaratna, Junfeng Wang, Xinlei Ge, and Alex K. Y. Lee
Atmos. Meas. Tech., 14, 2799–2812, https://doi.org/10.5194/amt-14-2799-2021, https://doi.org/10.5194/amt-14-2799-2021, 2021
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Chemical characterization of organic coatings is important to advance our understanding of the physio-chemical properties and atmospheric processing of black carbon (BC) particles. This work develops two approaches to improve the elemental analysis of oxygenated organic coatings using a soot-particle aerosol mass spectrometer. Analyzing ambient data with the new approaches indicated that secondary organics that coated on BC were likely less oxygenated compared to those externally mixed with BC.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Rosaria E. Pileci, Robin L. Modini, Michele Bertò, Jinfeng Yuan, Joel C. Corbin, Angela Marinoni, Bas Henzing, Marcel M. Moerman, Jean P. Putaud, Gerald Spindler, Birgit Wehner, Thomas Müller, Thomas Tuch, Arianna Trentini, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Meas. Tech., 14, 1379–1403, https://doi.org/10.5194/amt-14-1379-2021, https://doi.org/10.5194/amt-14-1379-2021, 2021
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Black carbon (BC), which is an important constituent of atmospheric aerosols, remains difficult to quantify due to various limitations of available methods. This study provides an extensive comparison of co-located field measurements, applying two methods based on different principles. It was shown that both methods indeed quantify the same aerosol property – BC mass concentration. The level of agreement that can be expected was quantified, and some reasons for discrepancy were identified.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Jinfeng Yuan, Robin Lewis Modini, Marco Zanatta, Andreas B. Herber, Thomas Müller, Birgit Wehner, Laurent Poulain, Thomas Tuch, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 21, 635–655, https://doi.org/10.5194/acp-21-635-2021, https://doi.org/10.5194/acp-21-635-2021, 2021
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Black carbon (BC) aerosols contribute substantially to climate warming due to their unique light absorption capabilities. We performed field measurements at a central European background site in winter and found that variability in the absorption efficiency of BC particles is driven mainly by their internal mixing state. Our results suggest that, at this site, knowing the BC mixing state is sufficient to describe BC light absorption enhancements due to the lensing effect in good approximation.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
André Welti, E. Keith Bigg, Paul J. DeMott, Xianda Gong, Markus Hartmann, Mike Harvey, Silvia Henning, Paul Herenz, Thomas C. J. Hill, Blake Hornblow, Caroline Leck, Mareike Löffler, Christina S. McCluskey, Anne Marie Rauker, Julia Schmale, Christian Tatzelt, Manuela van Pinxteren, and Frank Stratmann
Atmos. Chem. Phys., 20, 15191–15206, https://doi.org/10.5194/acp-20-15191-2020, https://doi.org/10.5194/acp-20-15191-2020, 2020
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Ship-based measurements of maritime ice nuclei concentrations encompassing all oceans are compiled. From this overview it is found that maritime ice nuclei concentrations are typically 10–100 times lower than over continents, while concentrations are surprisingly similar in different oceanic regions. The analysis of the influence of ship emissions shows no effect on the data, making ship-based measurements an efficient strategy for the large-scale exploration of ice nuclei concentrations.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
Short summary
Short summary
We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
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Short summary
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.
To understand the sources and fate of particulate matter in the atmosphere, the ability to...