Articles | Volume 13, issue 5
https://doi.org/10.5194/amt-13-2711-2020
© Author(s) 2020. 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-13-2711-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 May 2020
Research article |
| 27 May 2020
| 27 May 2020
Calibration of an airborne HOx instrument using the All Pressure Altitude-based Calibrator for HOx Experimentation (APACHE)
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Cheryl Ernest
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
now at: Department of Neurology, University Medical Center of the Johannes Gutenberg University Mainz, 55131 Mainz, Germany
Korbinian Hens
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
now at: Hübner GmbH & Co KG – Division Hübner
Photonics, 34123 Kassel, Germany
Umar Javed
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Forschungszentrum Jülich GmbH, IEK-8, 52425 Jülich, Germany
Thomas Klimach
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Monica Martinez
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Markus Rudolf
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Jos Lelieveld
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
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Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
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Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 16, 3013–3028, https://doi.org/10.5194/gmd-16-3013-2023, https://doi.org/10.5194/gmd-16-3013-2023, 2023
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Desert dust has significant impacts on climate, public health, infrastructure and ecosystems. An impact assessment requires numerical predictions, which are challenging because the dust emissions are not well known. We present a novel approach using satellite observations and machine learning to more accurately estimate the emissions and to improve the model simulations.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Andreas Hünig, Oliver Appel, Antonis Dragoneas, Sergej Molleker, Hans-Christian Clemen, Frank Helleis, Thomas Klimach, Franziska Köllner, Thomas Böttger, Frank Drewnick, Johannes Schneider, and Stephan Borrmann
Atmos. Meas. Tech., 15, 2889–2921, https://doi.org/10.5194/amt-15-2889-2022, https://doi.org/10.5194/amt-15-2889-2022, 2022
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We have serially combined the two well-established methods for in situ real-time measurement of fine particle chemical composition, the single-particle laser ablation method and the flash evaporation with electron impact ionization method, into a novel instrument. Here we present the design; instrument characteristics, as derived from laboratory and field measurements; and results from the first field deployment during the 2017 StratoClim aircraft campaign.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
Najin Kim, Yafang Cheng, Nan Ma, Mira L. Pöhlker, Thomas Klimach, Thomas F. Mentel, Ovid O. Krüger, Ulrich Pöschl, and Hang Su
Atmos. Meas. Tech., 14, 6991–7005, https://doi.org/10.5194/amt-14-6991-2021, https://doi.org/10.5194/amt-14-6991-2021, 2021
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A broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of supersaturation simultaneously, can measure a broad range of CCN activity distribution with a high time resolution. We describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve. Intercomparison experiments between typical DMA-CCN and BS2-CCN measurements to evaluate the BS2-CCN system showed high correlation and good agreement.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
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Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Hannes Schulz, Daniel Kunkel, Heiko Bozem, Peter Hoor, Thomas Klimach, Frank Helleis, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 21, 6509–6539, https://doi.org/10.5194/acp-21-6509-2021, https://doi.org/10.5194/acp-21-6509-2021, 2021
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We present in situ observations of vertically resolved particle chemical composition in the summertime Arctic lower troposphere. Our analysis demonstrates the strong vertical contrast between particle properties within the boundary layer and aloft. Emissions from vegetation fires and anthropogenic sources in northern Canada, Europe, and East Asia influenced particle composition in the free troposphere. Organics detected in Arctic aerosol particles can partly be identified as dicarboxylic acids.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
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.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Hans-Christian Clemen, Johannes Schneider, Thomas Klimach, Frank Helleis, Franziska Köllner, Andreas Hünig, Florian Rubach, Stephan Mertes, Heike Wex, Frank Stratmann, André Welti, Rebecca Kohl, Fabian Frank, and Stephan Borrmann
Atmos. Meas. Tech., 13, 5923–5953, https://doi.org/10.5194/amt-13-5923-2020, https://doi.org/10.5194/amt-13-5923-2020, 2020
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We improved the efficiency of a single-particle mass spectrometer with a newly developed aerodynamic lens system, delayed ion extraction, and better electric shielding. The new components result in significantly improved particle analysis and sample statistics. This is particularly important for measurements of low-number-density particles, such as ice-nucleating particles, and for aircraft-based measurements at high altitudes or where high temporal and spatial resolution is required.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Sergej Molleker, Frank Helleis, Thomas Klimach, Oliver Appel, Hans-Christian Clemen, Antonis Dragoneas, Christian Gurk, Andreas Hünig, Franziska Köllner, Florian Rubach, Christiane Schulz, Johannes Schneider, and Stephan Borrmann
Atmos. Meas. Tech., 13, 3651–3660, https://doi.org/10.5194/amt-13-3651-2020, https://doi.org/10.5194/amt-13-3651-2020, 2020
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A novel constant-pressure-inlet design for use in airborne aerosol particle mass spectrometry – an aerodynamic lens focuses aerosol particles into a vacuum chamber – is presented. The pressure of a few hectopascals at the lens is precisely controlled over a large flight altitude range up to 21 km. The constant pressure is achieved by changing the inner diameter of a properly scaled flexible O-ring acting as a critical orifice. Particle transmission at various inlet pressures is characterized.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
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Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Bruna A. Holanda, Mira L. Pöhlker, David Walter, Jorge Saturno, Matthias Sörgel, Jeannine Ditas, Florian Ditas, Christiane Schulz, Marco Aurélio Franco, Qiaoqiao Wang, Tobias Donth, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Ramon Braga, Joel Brito, Yafang Cheng, Maximilian Dollner, Johannes W. Kaiser, Thomas Klimach, Christoph Knote, Ovid O. Krüger, Daniel Fütterer, Jošt V. Lavrič, Nan Ma, Luiz A. T. Machado, Jing Ming, Fernando G. Morais, Hauke Paulsen, Daniel Sauer, Hans Schlager, Johannes Schneider, Hang Su, Bernadett Weinzierl, Adrian Walser, Manfred Wendisch, Helmut Ziereis, Martin Zöger, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 20, 4757–4785, https://doi.org/10.5194/acp-20-4757-2020, https://doi.org/10.5194/acp-20-4757-2020, 2020
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Biomass burning smoke from African savanna and grassland is transported across the South Atlantic Ocean in defined layers within the free troposphere. The combination of in situ aircraft and ground-based measurements aided by satellite observations showed that these layers are transported into the Amazon Basin during the early dry season. The influx of aged smoke, enriched in black carbon and cloud condensation nuclei, has important implications for the Amazonian aerosol and cloud cycling.
Siddika Celik, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Hugh Coe, Jean-Daniel Paris, Philipp G. Eger, Jan Schuladen, Ivan Tadic, Nils Friedrich, Dirk Dienhart, Bettina Hottmann, Horst Fischer, John N. Crowley, Hartwig Harder, and Stephan Borrmann
Atmos. Chem. Phys., 20, 4713–4734, https://doi.org/10.5194/acp-20-4713-2020, https://doi.org/10.5194/acp-20-4713-2020, 2020
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Analysis of 252 ship emission plumes in the Mediterranean Sea and around the Arabian Peninsula examined particulate- and gas-phase characteristics. By identifying the corresponding ships, source features and plume age were determined. Emission factors (amount of pollutant per kilogram of fuel burned) were calculated and investigated for dependencies on source characteristics, atmospheric conditions, and transport time, providing insight into the most relevant influences on ship emissions.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
Pascal Polonik, Christoph Knote, Tobias Zinner, Florian Ewald, Tobias Kölling, Bernhard Mayer, Meinrat O. Andreae, Tina Jurkat-Witschas, Thomas Klimach, Christoph Mahnke, Sergej Molleker, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Ralf Weigel, and Manfred Wendisch
Atmos. Chem. Phys., 20, 1591–1605, https://doi.org/10.5194/acp-20-1591-2020, https://doi.org/10.5194/acp-20-1591-2020, 2020
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A realistic representation of cloud–aerosol interactions is central to accurate climate projections. Here we combine observations collected during the ACRIDICON-CHUVA campaign with chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysics. We find an upper limit for the model sensitivity on cloud condensation nuclei concentrations well below the levels reached during the burning season in the Amazon Basin.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
Horst Fischer, Raoul Axinte, Heiko Bozem, John N. Crowley, Cheryl Ernest, Stefan Gilge, Sascha Hafermann, Hartwig Harder, Korbinian Hens, Ruud H. H. Janssen, Rainer Königstedt, Dagmar Kubistin, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Christian Plass-Dülmer, Andrea Pozzer, Eric Regelin, Andreas Reiffs, Torsten Schmidt, Jan Schuladen, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11953–11968, https://doi.org/10.5194/acp-19-11953-2019, https://doi.org/10.5194/acp-19-11953-2019, 2019
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We use in situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951, https://doi.org/10.5194/acp-19-11939-2019, https://doi.org/10.5194/acp-19-11939-2019, 2019
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We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
Jianzhong Ma, Christoph Brühl, Qianshan He, Benedikt Steil, Vlassis A. Karydis, Klaus Klingmüller, Holger Tost, Bin Chen, Yufang Jin, Ningwei Liu, Xiangde Xu, Peng Yan, Xiuji Zhou, Kamal Abdelrahman, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11587–11612, https://doi.org/10.5194/acp-19-11587-2019, https://doi.org/10.5194/acp-19-11587-2019, 2019
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We find a pronounced maximum in aerosol extinction in the upper troposphere and lower stratosphere over the Tibetan Plateau during the Asian summer monsoon, caused mainly by mineral dust emitted from the northern Tibetan Plateau and slope area, lofted to and accumulating within the anticyclonic circulation. Mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction around the tropopause within the Asian summer monsoon anticyclone.
Eva Y. Pfannerstill, Nijing Wang, Achim Edtbauer, Efstratios Bourtsoukidis, John N. Crowley, Dirk Dienhart, Philipp G. Eger, Lisa Ernle, Horst Fischer, Bettina Hottmann, Jean-Daniel Paris, Christof Stönner, Ivan Tadic, David Walter, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 19, 11501–11523, https://doi.org/10.5194/acp-19-11501-2019, https://doi.org/10.5194/acp-19-11501-2019, 2019
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The Arabian Peninsula is a global hot spot of ozone pollution. Our measurements, made on a ship in summer 2017, indicate underlying reasons. Despite being at sea, we observed ozone-forming reactive trace gases (measured as so-called total OH reactivity) comparable to highly populated urban regions in amount and composition. This is due to strong emissions from oil extraction and ship traffic. These emissions were quickly converted to ozone due to intense solar irradiation and high temperatures.
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
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.
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
Ralph Dlugi, Martina Berger, Chinmay Mallik, Anywhere Tsokankunku, Michael Zelger, Otávio C. Acevedo, Efstratios Bourtsoukidis, Andreas Hofzumahaus, Jürgen Kesselmeier, Gerhard Kramm, Daniel Marno, Monica Martinez, Anke C. Nölscher, Huug Ouwersloot, Eva Y. Pfannerstill, Franz Rohrer, Sebastian Tauer, Jonathan Williams, Ana-Maria Yáñez-Serrano, Meinrat O. Andreae, Hartwig Harder, and Matthias Sörgel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1325, https://doi.org/10.5194/acp-2018-1325, 2019
Publication in ACP not foreseen
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Incomplete mixing (segregation) results in reduced chemical reaction rates compared to those expected from mean values and rate constants. Segregation has been suggested to cause discrepancies between modelled and measured OH radical concentrations. In this work, we summarize the intensities of segregation for the reaction of OH and isoprene for different field and modelling studies and compare those to our results from measurements in a pristine environment.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
Rolf Sander, Andreas Baumgaertner, David Cabrera-Perez, Franziska Frank, Sergey Gromov, Jens-Uwe Grooß, Hartwig Harder, Vincent Huijnen, Patrick Jöckel, Vlassis A. Karydis, Kyle E. Niemeyer, Andrea Pozzer, Hella Riede, Martin G. Schultz, Domenico Taraborrelli, and Sebastian Tauer
Geosci. Model Dev., 12, 1365–1385, https://doi.org/10.5194/gmd-12-1365-2019, https://doi.org/10.5194/gmd-12-1365-2019, 2019
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We present the atmospheric chemistry box model CAABA/MECCA which
now includes a number of new features: skeletal mechanism
reduction, the MOM chemical mechanism for volatile organic
compounds, an option to include reactions from the Master
Chemical Mechanism (MCM) and other chemical mechanisms, updated
isotope tagging, improved and new photolysis modules, and the new
feature of coexisting multiple chemistry mechanisms.
CAABA/MECCA is a community model published under the GPL.
Philipp G. Eger, Frank Helleis, Gerhard Schuster, Gavin J. Phillips, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 12, 1935–1954, https://doi.org/10.5194/amt-12-1935-2019, https://doi.org/10.5194/amt-12-1935-2019, 2019
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We present a chemical ionization quadrupole mass spectrometer (CI-QMS) with a novel discharge ion source. In addition to the expected detection of PAN, peracetic acid and ClNO2, the instrument is also sensitive to SO2, HCl and acetic acid through ion chemistry unique for our ion source. We present ionization schemes along with illustrative datasets from field campaigns underlining the potential of the CI-QMS as an alternative to polonium, especially for application in the marine boundary layer.
Umar Javed, Dagmar Kubistin, Monica Martinez, Jan Pollmann, Markus Rudolf, Uwe Parchatka, Andreas Reiffs, Jim Thieser, Gerhard Schuster, Martin Horbanski, Denis Pöhler, John N. Crowley, Horst Fischer, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 12, 1461–1481, https://doi.org/10.5194/amt-12-1461-2019, https://doi.org/10.5194/amt-12-1461-2019, 2019
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Nitrogen dioxide (NO2) affects the concentration of key species like ozone, hydroxyl radical, and nitrate radical in the atmosphere. In situ, direct, and interference-free NO2 measurements are important for validating our understanding of NOx chemistry related to ozone formation and the radical loss process. This article describes the important features and performance of a newly developed NO2 instrument during a field intercomparison.
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.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
Jonathan M. Liebmann, Jennifer B. A. Muller, Dagmar Kubistin, Anja Claude, Robert Holla, Christian Plass-Dülmer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 12045–12059, https://doi.org/10.5194/acp-18-12045-2018, https://doi.org/10.5194/acp-18-12045-2018, 2018
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We present direct measurements of the summertime total reactivity (inverse lifetime) of NO3 towards organic trace gases at a rural mountain site. High daytime and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during daytime. NO3 radical measurements from one night are presented. For the first time, direct measurements of OH and NO3 reactivity are compared.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Zacharias Marinou Nikolaou, Jyh-Yuan Chen, Yiannis Proestos, Jos Lelieveld, and Rolf Sander
Geosci. Model Dev., 11, 3391–3407, https://doi.org/10.5194/gmd-11-3391-2018, https://doi.org/10.5194/gmd-11-3391-2018, 2018
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Chemistry is an important component of the atmosphere that describes many important physical processes. However, atmospheric chemical mechanisms include hundreds of species and reactions, posing a significant computational load. In this work, we use a powerful reduction method in order to develop a computationally faster chemical mechanism from a detailed mechanism. This enables accelerated simulations, which can be used to examine a wider range of processes in increased detail.
Chinmay Mallik, Laura Tomsche, Efstratios Bourtsoukidis, John N. Crowley, Bettina Derstroff, Horst Fischer, Sascha Hafermann, Imke Hüser, Umar Javed, Stephan Keßel, Jos Lelieveld, Monica Martinez, Hannah Meusel, Anna Novelli, Gavin J. Phillips, Andrea Pozzer, Andreas Reiffs, Rolf Sander, Domenico Taraborrelli, Carina Sauvage, Jan Schuladen, Hang Su, Jonathan Williams, and Hartwig Harder
Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, https://doi.org/10.5194/acp-18-10825-2018, 2018
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OH and HO2 control the transformation of air pollutants and O3 formation. Their implication for air quality over the climatically sensitive Mediterranean region was studied during a field campaign in Cyprus. Production of OH, HO2, and recycled OH was lower in aged marine air masses. Box model simulations of OH and HO2 agreed with measurements except at high terpene concentrations when model RO2 due to terpenes caused large HO2 loss. Autoxidation schemes for RO2 improved the agreement.
Mira L. Pöhlker, Florian Ditas, Jorge Saturno, Thomas Klimach, Isabella Hrabě de Angelis, Alessandro C. Araùjo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Bruna A. Holanda, Konrad Kandler, Jürgen Kesselmeier, Tobias Könemann, Ovid O. Krüger, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Luciana V. Rizzo, Diana Rose, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10289–10331, https://doi.org/10.5194/acp-18-10289-2018, https://doi.org/10.5194/acp-18-10289-2018, 2018
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This paper presents the aerosol and cloud condensation nuclei (CCN) variability for characteristic atmospheric states – such as biomass burning, long-range transport, and pristine rain forest conditions – in the vulnerable and climate-relevant Amazon Basin. It summarizes the key properties of aerosol and CCN and, thus, provides a basis for an in-depth analysis of aerosol–cloud interactions in the Amazon region.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Panos Hadjinicolaou, and Jos Lelieveld
Atmos. Chem. Phys., 18, 1555–1571, https://doi.org/10.5194/acp-18-1555-2018, https://doi.org/10.5194/acp-18-1555-2018, 2018
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We investigate the impact of the choice of gas-phase and aerosol mechanisms, on the simulated summertime concentrations of several pollutants over the eastern Mediterranean, using the WRF-Chem model. The selection of mechanisms significantly affects ozone and fine particulate matter concentrations, and to a lesser extent other gaseous pollutants (NOx, CO). Meteorological components are also affected by the choice of mechanisms due to the interaction of aerosols with radiation.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
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We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Micael A. Cecchini, Luiz A. T. Machado, Manfred Wendisch, Anja Costa, Martina Krämer, Meinrat O. Andreae, Armin Afchine, Rachel I. Albrecht, Paulo Artaxo, Stephan Borrmann, Daniel Fütterer, Thomas Klimach, Christoph Mahnke, Scot T. Martin, Andreas Minikin, Sergej Molleker, Lianet H. Pardo, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, and Bernadett Weinzierl
Atmos. Chem. Phys., 17, 14727–14746, https://doi.org/10.5194/acp-17-14727-2017, https://doi.org/10.5194/acp-17-14727-2017, 2017
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This study introduces and explores the concept of gamma phase space. This space is able to represent all possible variations in the cloud droplet size distributions (DSDs). The methodology was applied to recent in situ aircraft measurements over the Amazon. It is shown that the phase space is able to represent several processes occurring in the clouds in a simple manner. The consequences for cloud studies, modeling, and the representation of the transition from warm to mixed phase are discussed.
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Thomas Klimach, Frank Helleis, Heiko Bozem, Daniel Kunkel, Peter Hoor, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 17, 13747–13766, https://doi.org/10.5194/acp-17-13747-2017, https://doi.org/10.5194/acp-17-13747-2017, 2017
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We conducted aircraft-based single particle chemical composition measurements in the Canadian high Arctic during summer. Our results provide evidence for a marine-biogenic influence on secondary formation of particulate trimethylamine in the Arctic boundary layer. Understanding emission sources and further processes controlling aerosol number concentration and chemical composition in the pristine Arctic summer is crucial for modeling future climate in the area.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Imke Hüser, Hartwig Harder, Angelika Heil, and Johannes W. Kaiser
Atmos. Chem. Phys., 17, 10955–10967, https://doi.org/10.5194/acp-17-10955-2017, https://doi.org/10.5194/acp-17-10955-2017, 2017
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The impact of pollution sources on downwind sites can be quantified by Lagrangian dispersion models. We identified the representation of the mixing layer dynamics as a crucial factor for the vertical mixing of surface pollutants. Our application examples show that inaccuracies may introduce errors in the impact assessment on downwind sites. For vegetation fires, mixing by pyrogenic convection is under-represented. We find an overestimation of downwind smoke concentration of more than 60 %.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Ramon Campos Braga, Daniel Rosenfeld, Ralf Weigel, Tina Jurkat, Meinrat O. Andreae, Manfred Wendisch, Mira L. Pöhlker, Thomas Klimach, Ulrich Pöschl, Christopher Pöhlker, Christiane Voigt, Christoph Mahnke, Stephan Borrmann, Rachel I. Albrecht, Sergej Molleker, Daniel A. Vila, Luiz A. T. Machado, and Paulo Artaxo
Atmos. Chem. Phys., 17, 7365–7386, https://doi.org/10.5194/acp-17-7365-2017, https://doi.org/10.5194/acp-17-7365-2017, 2017
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
Susan Schmidt, Johannes Schneider, Thomas Klimach, Stephan Mertes, Ludwig Paul Schenk, Piotr Kupiszewski, Joachim Curtius, and Stephan Borrmann
Atmos. Chem. Phys., 17, 575–594, https://doi.org/10.5194/acp-17-575-2017, https://doi.org/10.5194/acp-17-575-2017, 2017
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Ice formation in clouds is an important process in the formation of precipitation, especially at midlatitudes, but the exact properties of the aerosol particles that initiate freezing is not fully understood. We analysed residual particles from ice crystals sampled from mixed phase clouds. The results show that the residues contain a larger relative amount of soil dust and minerals, but also particles from industrial emissions and lead-containing particles, than the out-of-cloud aerosol.
Anthony J. Hynes, Stephanie Everhart, Dieter Bauer, James Remeika, and Cheryl Tatum Ernest
Atmos. Chem. Phys., 17, 465–483, https://doi.org/10.5194/acp-17-465-2017, https://doi.org/10.5194/acp-17-465-2017, 2017
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Exposure to mercury (Hg), is a significant issue from a human health perspective. Understanding the chemistry that leads to exposure is important. We have developed a laser-based sensor for the detection of gas-phase elemental mercury, Hg(0). The instrument is capable of fast in situ measurement of Hg(0) at ambient levels. The RAMIX experiment intercompared atmospheric Hg measurement systems. We typically saw good agreement for measurements of Hg(0) but not for total oxidized mercury.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Andrea Pozzer, Yogesh K. Tiwari, K. Ravi Kumar, and Jos Lelieveld
Atmos. Chem. Phys., 17, 257–275, https://doi.org/10.5194/acp-17-257-2017, https://doi.org/10.5194/acp-17-257-2017, 2017
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This study presents first ship-borne measurements of trace gases over the Bay of Bengal during summer monsoon. The observed variations in trace gases are shown to be due to dynamics/transport and en route photochemistry. Analysis of meteorological and chemical fields shows that significantly lower ozone during rainfall is associated with the downdrafts. A regional model reproduces the observed variations and revealed the rapid transport of ozone across the Bay of Bengal during an event.
Mira L. Pöhlker, Christopher Pöhlker, Florian Ditas, Thomas Klimach, Isabella Hrabe de Angelis, Alessandro Araújo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Jürgen Kesselmeier, Tobias Könemann, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Diana Rose, Jorge Saturno, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, and Ulrich Pöschl
Atmos. Chem. Phys., 16, 15709–15740, https://doi.org/10.5194/acp-16-15709-2016, https://doi.org/10.5194/acp-16-15709-2016, 2016
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The paper presents a systematic characterization of cloud condensation nuclei (CCN) concentration in the central Amazonian atmosphere. Our results show that the CCN population in this globally important ecosystem follows a pollution-related seasonal cycle, in which it mainly depends on changes in total aerosol size distribution and to a minor extent in the aerosol chemical composition. Our results allow an efficient modeling and prediction of the CCN population based on a novel approach.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Klaus Klingmüller, Andrea Pozzer, Swen Metzger, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 16, 5063–5073, https://doi.org/10.5194/acp-16-5063-2016, https://doi.org/10.5194/acp-16-5063-2016, 2016
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During the last decade, the Middle East experienced the strongest increase in atmospheric aerosol concentrations worldwide. Based on satellite observations, the present study corroborates this trend and reveals correlations with soil moisture and precipitation in and surrounding the Fertile Crescent. This suggests that the increasing drought conditions in this region have enhanced dust emissions, a tendency which is expected to be intensified by climate change.
N. Sobanski, M. J. Tang, J. Thieser, G. Schuster, D. Pöhler, H. Fischer, W. Song, C. Sauvage, J. Williams, J. Fachinger, F. Berkes, P. Hoor, U. Platt, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 16, 4867–4883, https://doi.org/10.5194/acp-16-4867-2016, https://doi.org/10.5194/acp-16-4867-2016, 2016
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The nitrate radical (NO3) is an important nocturnal oxidant. By measuring NO3, its precursors (nitrogen dioxide and ozone) and several trace gases with which it reacts, we examined the chemical and meteorological factors influencing the lifetime of NO3 at a semi-rural mountain site. Unexpectedly long lifetimes, approaching 1 h, were observed on several nights and were associated with a low-lying residual layer. We discuss the role of other reactions that convert NO2 to NO3.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
J. Thieser, G. Schuster, J. Schuladen, G. J. Phillips, A. Reiffs, U. Parchatka, D. Pöhler, J. Lelieveld, and J. N. Crowley
Atmos. Meas. Tech., 9, 553–576, https://doi.org/10.5194/amt-9-553-2016, https://doi.org/10.5194/amt-9-553-2016, 2016
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We report on the use of thermal dissociation cavity ring-down spectroscopy to detect NO2, peroxy nitrates and alkyl nitrates. We present both laboratory studies that characterise the chemical formation and loss of NO2 in the heated inlets and also result from a first field deployment.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
M. Abdelkader, S. Metzger, R. E. Mamouri, M. Astitha, L. Barrie, Z. Levin, and J. Lelieveld
Atmos. Chem. Phys., 15, 9173–9189, https://doi.org/10.5194/acp-15-9173-2015, https://doi.org/10.5194/acp-15-9173-2015, 2015
H. G. Ouwersloot, A. Pozzer, B. Steil, H. Tost, and J. Lelieveld
Geosci. Model Dev., 8, 2435–2445, https://doi.org/10.5194/gmd-8-2435-2015, https://doi.org/10.5194/gmd-8-2435-2015, 2015
H. Fischer, A. Pozzer, T. Schmitt, P. Jöckel, T. Klippel, D. Taraborrelli, and J. Lelieveld
Atmos. Chem. Phys., 15, 6971–6980, https://doi.org/10.5194/acp-15-6971-2015, https://doi.org/10.5194/acp-15-6971-2015, 2015
S. Zheng, A. Pozzer, C. X. Cao, and J. Lelieveld
Atmos. Chem. Phys., 15, 5715–5725, https://doi.org/10.5194/acp-15-5715-2015, https://doi.org/10.5194/acp-15-5715-2015, 2015
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The present study uses aerosol optical depth as proxy to estimate 12 years of PM2.5 data for the Beijing central area and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals/year for the period 2001--2012 in the Beijing central area, and the per capita mortality for all ages due to PM2.5 is around 15 per 10,000 person-years for the period 2010--2012.
R. Oswald, M. Ermel, K. Hens, A. Novelli, H. G. Ouwersloot, P. Paasonen, T. Petäjä, M. Sipilä, P. Keronen, J. Bäck, R. Königstedt, Z. Hosaynali Beygi, H. Fischer, B. Bohn, D. Kubistin, H. Harder, M. Martinez, J. Williams, T. Hoffmann, I. Trebs, and M. Sörgel
Atmos. Chem. Phys., 15, 799–813, https://doi.org/10.5194/acp-15-799-2015, https://doi.org/10.5194/acp-15-799-2015, 2015
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Nitrous acid (HONO) is a key species in atmospheric photochemistry since the photolysis leads to the important hydroxyl radical (OH). Although the importance of HONO as a precursor of OH is known, the formation pathways of HONO, especially during daytime, are a major challenge in atmospheric science. We present a detailed analysis of sources and sinks for HONO in the atmosphere for a field measurement campaign in the boreal forest in Finland and wonder if there is really a source term missing.
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
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A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
K. Klingmüller, B. Steil, C. Brühl, H. Tost, and J. Lelieveld
Geosci. Model Dev., 7, 2503–2516, https://doi.org/10.5194/gmd-7-2503-2014, https://doi.org/10.5194/gmd-7-2503-2014, 2014
B. Bonn, E. Bourtsoukidis, T. S. Sun, H. Bingemer, L. Rondo, U. Javed, J. Li, R. Axinte, X. Li, T. Brauers, H. Sonderfeld, R. Koppmann, A. Sogachev, S. Jacobi, and D. V. Spracklen
Atmos. Chem. Phys., 14, 10823–10843, https://doi.org/10.5194/acp-14-10823-2014, https://doi.org/10.5194/acp-14-10823-2014, 2014
A. Novelli, K. Hens, C. Tatum Ernest, D. Kubistin, E. Regelin, T. Elste, C. Plass-Dülmer, M. Martinez, J. Lelieveld, and H. Harder
Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, https://doi.org/10.5194/amt-7-3413-2014, 2014
H. Bozem, H. Fischer, C. Gurk, C. L. Schiller, U. Parchatka, R. Koenigstedt, A. Stickler, M. Martinez, H. Harder, D. Kubistin, J. Williams, G. Eerdekens, and J. Lelieveld
Atmos. Chem. Phys., 14, 8917–8931, https://doi.org/10.5194/acp-14-8917-2014, https://doi.org/10.5194/acp-14-8917-2014, 2014
D. Y. Chang, H. Tost, B. Steil, and J. Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-21975-2014, https://doi.org/10.5194/acpd-14-21975-2014, 2014
Preprint withdrawn
K. Hens, A. Novelli, M. Martinez, J. Auld, R. Axinte, B. Bohn, H. Fischer, P. Keronen, D. Kubistin, A. C. Nölscher, R. Oswald, P. Paasonen, T. Petäjä, E. Regelin, R. Sander, V. Sinha, M. Sipilä, D. Taraborrelli, C. Tatum Ernest, J. Williams, J. Lelieveld, and H. Harder
Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, https://doi.org/10.5194/acp-14-8723-2014, 2014
A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren
Atmos. Chem. Phys., 14, 7213–7231, https://doi.org/10.5194/acp-14-7213-2014, https://doi.org/10.5194/acp-14-7213-2014, 2014
T. Christoudias, Y. Proestos, and J. Lelieveld
Atmos. Chem. Phys., 14, 4607–4616, https://doi.org/10.5194/acp-14-4607-2014, https://doi.org/10.5194/acp-14-4607-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
J. A. Adame, M. Martínez, M. Sorribas, P. J. Hidalgo, H. Harder, J.-M. Diesch, F. Drewnick, W. Song, J. Williams, V. Sinha, M. A. Hernández-Ceballos, J. Vilà-Guerau de Arellano, R. Sander, Z. Hosaynali-Beygi, H. Fischer, J. Lelieveld, and B. De la Morena
Atmos. Chem. Phys., 14, 2325–2342, https://doi.org/10.5194/acp-14-2325-2014, https://doi.org/10.5194/acp-14-2325-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Y. F. Elshorbany, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld
Atmos. Chem. Phys., 14, 1167–1184, https://doi.org/10.5194/acp-14-1167-2014, https://doi.org/10.5194/acp-14-1167-2014, 2014
D. Giannadaki, A. Pozzer, and J. Lelieveld
Atmos. Chem. Phys., 14, 957–968, https://doi.org/10.5194/acp-14-957-2014, https://doi.org/10.5194/acp-14-957-2014, 2014
P. Zanis, P. Hadjinicolaou, A. Pozzer, E. Tyrlis, S. Dafka, N. Mihalopoulos, and J. Lelieveld
Atmos. Chem. Phys., 14, 115–132, https://doi.org/10.5194/acp-14-115-2014, https://doi.org/10.5194/acp-14-115-2014, 2014
J. Yoon, A. Pozzer, P. Hoor, D. Y. Chang, S. Beirle, T. Wagner, S. Schloegl, J. Lelieveld, and H. M. Worden
Atmos. Chem. Phys., 13, 11307–11316, https://doi.org/10.5194/acp-13-11307-2013, https://doi.org/10.5194/acp-13-11307-2013, 2013
E. Regelin, H. Harder, M. Martinez, D. Kubistin, C. Tatum Ernest, H. Bozem, T. Klippel, Z. Hosaynali-Beygi, H. Fischer, R. Sander, P. Jöckel, R. Königstedt, and J. Lelieveld
Atmos. Chem. Phys., 13, 10703–10720, https://doi.org/10.5194/acp-13-10703-2013, https://doi.org/10.5194/acp-13-10703-2013, 2013
J. Lelieveld, C. Barlas, D. Giannadaki, and A. Pozzer
Atmos. Chem. Phys., 13, 7023–7037, https://doi.org/10.5194/acp-13-7023-2013, https://doi.org/10.5194/acp-13-7023-2013, 2013
A.C. Nölscher, E. Bourtsoukidis, B. Bonn, J. Kesselmeier, J. Lelieveld, and J. Williams
Biogeosciences, 10, 4241–4257, https://doi.org/10.5194/bg-10-4241-2013, https://doi.org/10.5194/bg-10-4241-2013, 2013
M. D. Andrés-Hernández, D. Kartal, J. N. Crowley, V. Sinha, E. Regelin, M. Martínez-Harder, V. Nenakhov, J. Williams, H. Harder, H. Bozem, W. Song, J. Thieser, M. J. Tang, Z. Hosaynali Beigi, and J. P. Burrows
Atmos. Chem. Phys., 13, 5731–5749, https://doi.org/10.5194/acp-13-5731-2013, https://doi.org/10.5194/acp-13-5731-2013, 2013
C. Brühl, J. Lelieveld, M. Höpfner, and H. Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-11395-2013, https://doi.org/10.5194/acpd-13-11395-2013, 2013
Revised manuscript not accepted
G. J. Phillips, N. Pouvesle, J. Thieser, G. Schuster, R. Axinte, H. Fischer, J. Williams, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 13, 1129–1139, https://doi.org/10.5194/acp-13-1129-2013, https://doi.org/10.5194/acp-13-1129-2013, 2013
J. Lelieveld, M. G. Lawrence, and D. Kunkel
Atmos. Chem. Phys., 13, 31–34, https://doi.org/10.5194/acp-13-31-2013, https://doi.org/10.5194/acp-13-31-2013, 2013
A. Jugold, F. Althoff, M. Hurkuck, M. Greule, K. Lenhart, J. Lelieveld, and F. Keppler
Biogeosciences, 9, 5291–5301, https://doi.org/10.5194/bg-9-5291-2012, https://doi.org/10.5194/bg-9-5291-2012, 2012
Related subject area
Subject: Gases | Technique: Laboratory Measurement | Topic: Instruments and Platforms
Water vapor stable isotope memory effects of common tubing materials
Evaluation of a reduced-pressure chemical ion reactor utilizing adduct ionization for the detection of gaseous organic and inorganic species
Ammonium CI-Orbitrap: a tool for characterizing the reactivity of oxygenated organic molecules
A high-accuracy dynamic dilution method for generating reference gas mixtures of carbonyl sulfide at sub-nanomole-per-mole levels for long-term atmospheric observation
Optimizing the iodide-adduct chemical ionization mass spectrometry (CIMS) quantitative method for toluene oxidation intermediates: experimental insights into functional-group differences
A new portable sampler of atmospheric methane for radiocarbon measurements
Characterization of a new Teflon chamber and on-line analysis of isomeric multifunctional photooxidation products
A versatile water vapor generation module for vapor isotope calibration and liquid isotope measurements
Extraction, purification, and clumped isotope analysis of methane (Δ13CDH3 and Δ12CD2H2) from sources and the atmosphere
Response of protonated, adduct, and fragmented ions in Vocus proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS)
Absorption of volatile organic compounds (VOCs) by polymer tubing: implications for indoor air and use as a simple gas-phase volatility separation technique
High precision δ18O measurements of atmospheric dioxygen using optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS)
A flexible device to produce a gas stream with a precisely controlled water vapour mixing ratio and isotope composition based on microdrop dispensing technology
Revision of an open-split-based dual-inlet system for elemental and isotope ratio mass spectrometers with a focus on clumped-isotope measurements
Characterisation of gaseous iodine species detection using the multi-scheme chemical ionisation inlet 2 with bromide and nitrate chemical ionisation methods
A novel inlet for enriching concentrations of reactive organic gases in low sampling flows
Characterizing the automatic radon flux transfer standard system Autoflux: laboratory calibration and field experiments
Influence of ozone and humidity on PTR-MS and GC-MS VOC measurements with and without a Na2S2O3 ozone scrubber
Laser-induced sublimation extraction for centimeter-resolution multi-species greenhouse gas analysis on ice cores
Ozone reactivity measurement of biogenic volatile organic compound emissions
Comparison of two photolytic calibration methods for nitrous acid
Measurement of enantiomer percentages for five monoterpenes from six conifer species by cartridge-tube-based passive sampling adsorption–thermal desorption (ps-ATD)
Identification, monitoring, and reaction kinetics of reactive trace species using time-resolved mid-infrared quantum cascade laser absorption spectroscopy: development, characterisation, and initial results for the CH2OO Criegee intermediate
Air pollution monitoring: development of ammonia (NH3) dynamic reference gas mixtures at nanomoles per mole levels to improve the lack of traceability of measurements
Formaldehyde and glyoxal measurement deploying a selected ion flow tube mass spectrometer (SIFT-MS)
Fragmentation inside proton-transfer-reaction-based mass spectrometers limits the detection of ROOR and ROOH peroxides
MULTICHARME: a modified Chernin-type multi-pass cell designed for IR and THz long-path absorption measurements in the CHARME atmospheric simulation chamber
Silicone tube humidity generator
A source for the continuous generation of pure and quantifiable HONO mixtures
Photochemical method for removing methane interference for improved gas analysis
A simulation chamber for absorption spectroscopy in planetary atmospheres
An automated system for trace gas flux measurements from plant foliage and other plant compartments
Simultaneous measurement of δ13C, δ18O and δ17O of atmospheric CO2 – performance assessment of a dual-laser absorption spectrometer
Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers
A method for resolving changes in atmospheric He ∕ N2 as an indicator of fossil fuel extraction and stratospheric circulation
Application of chemical derivatization techniques combined with chemical ionization mass spectrometry to detect stabilized Criegee intermediates and peroxy radicals in the gas phase
Atomic emission detector with gas chromatographic separation and cryogenic pre-concentration (CryoTrap–GC–AED) for atmospheric trace gas measurements
New technique for high-precision, simultaneous measurements of CH4, N2O and CO2 concentrations; isotopic and elemental ratios of N2, O2 and Ar; and total air content in ice cores by wet extraction
High-precision laser spectrometer for multiple greenhouse gas analysis in 1 mL air from ice core samples
A thermal-dissociation–cavity ring-down spectrometer (TD-CRDS) for the detection of organic nitrates in gas and particle phases
Interference from alkenes in chemiluminescent NOx measurements
Measurement of ammonia, amines and iodine compounds using protonated water cluster chemical ionization mass spectrometry
An instrument for in situ measurement of total ozone reactivity
Portable calibrator for NO based on the photolysis of N2O and a combined NO2∕NO∕O3 source for field calibrations of air pollution monitors
A new instrument for time-resolved measurement of HO2 radicals
Investigation of adsorption and desorption behavior of small-volume cylinders and its relevance for atmospheric trace gas analysis
Towards an understanding of surface effects: testing of various materials in a small volume measurement chamber and its relevance for atmospheric trace gas analysis
Stability of halocarbons in air samples stored in stainless- steel canisters
High-precision atmospheric oxygen measurement comparisons between a newly built CRDS analyzer and existing measurement techniques
Characterisation of the transfer of cluster ions through an atmospheric pressure interface time-of-flight mass spectrometer with hexapole ion guides
Alexandra L. Meyer and Lisa R. Welp
Atmos. Meas. Tech., 17, 6193–6212, https://doi.org/10.5194/amt-17-6193-2024, https://doi.org/10.5194/amt-17-6193-2024, 2024
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Water molecules stick to air intake tubing wall surfaces, smoothing measurements of fast isotopic variability in the atmosphere. We tested this stickiness and saw small differences in isotopic signal speed between materials, tubing inner dimensions, and isotopic switch direction, although no consistent temperature effects. Researchers can confidently compare measurements across observation systems using different commonly used tubing materials and plan for optimal inlet designs of new systems.
Matthieu Riva, Veronika Pospisilova, Carla Frege, Sebastien Perrier, Priyanka Bansal, Spiro Jorga, Patrick Sturm, Joel A. Thornton, Urs Rohner, and Felipe Lopez-Hilfiker
Atmos. Meas. Tech., 17, 5887–5901, https://doi.org/10.5194/amt-17-5887-2024, https://doi.org/10.5194/amt-17-5887-2024, 2024
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We present a newly designed reduced-pressure chemical ionization reactor for detection of gas-phase organic and inorganic species. The system operates through the combined use of vacuum ultraviolet ionization and photosensitizers to generate numerous adduct ionization schemes. As a result, it offers the ability to simultaneously measure a wide variety of organic and inorganic species in terms of compound volatility and functionality, while being largely independent of changes in sample humidity.
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.
Hideki Nara, Takuya Saito, Taku Umezawa, and Yasunori Tohjima
Atmos. Meas. Tech., 17, 5187–5200, https://doi.org/10.5194/amt-17-5187-2024, https://doi.org/10.5194/amt-17-5187-2024, 2024
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We have developed a high-accuracy dynamic dilution system for generating reference gas mixtures containing carbonyl sulfide (COS). Although COS at ambient levels generally has poor storage stability, our approach involves the dilution of a gas mixture containing micromole-per-mole levels of COS, the stability of which was validated for more than 1 decade. The developed system has excellent dilution performance and will facilitate accurate instrumental calibration for atmospheric COS observation.
Mengdi Song, Shuyu He, Xin Li, Ying Liu, Shengrong Lou, Sihua Lu, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 17, 5113–5127, https://doi.org/10.5194/amt-17-5113-2024, https://doi.org/10.5194/amt-17-5113-2024, 2024
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We introduce detailed and improved quantitation and semi-quantitation methods of iodide-adduct time-of-flight chemical ionization mass spectrometry (I-CIMS) to measure toluene oxidation intermediates. We assess the experimental sensitivity of various functional group species and their binding energy with iodide ions in I-CIMS. A novel classification approach was introduced to significantly enhance the accuracy of semi-quantitative methods (improving R2 values from 0.52 to beyond 0.88).
Giulia Zazzeri, Lukas Wacker, Negar Haghipour, Philip Gautchi, Thomas Laemmel, Sönke Szidat, and Heather Graven
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-123, https://doi.org/10.5194/amt-2024-123, 2024
Revised manuscript accepted for AMT
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Radiocarbon (14C) is an optimal tracer of methane (CH4) emissions, as 14C measurements enable distinguishing fossil from biogenic methane. However, these measurements are particularly challenging, mainly due to technical difficulties in the sampling procedure. With this work we made the sample extraction much simpler and time efficient, providing a new technology that can be used by any research group, with the goal of expanding 14C measurements for an improved understanding of methane sources.
Finja Löher, Esther Borrás, Amalia Muñoz, and Anke Christine Nölscher
Atmos. Meas. Tech., 17, 4553–4579, https://doi.org/10.5194/amt-17-4553-2024, https://doi.org/10.5194/amt-17-4553-2024, 2024
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We constructed and characterized a new indoor Teflon atmospheric simulation chamber. We evaluated wall losses, photolysis rates, and secondary reactions of multifunctional photooxidation products in the chamber. To measure these products on-line, we combined chromatographic and mass spectrometric analyses to obtain both isomeric information and a high temporal resolution. For method validation, we studied the formation yields of the main ring-retaining products of toluene.
Hans Christian Steen-Larsen and Daniele Zannoni
Atmos. Meas. Tech., 17, 4391–4409, https://doi.org/10.5194/amt-17-4391-2024, https://doi.org/10.5194/amt-17-4391-2024, 2024
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The water vapor generation module is completely scalable, allowing autonomous calibrations to use N standards and providing integration times only restricted by sample availability. We document improved reproducibility in 17O-excess liquid measurements. This module makes spectroscopy measurements comparable to mass spectrometry. We document that the vapor generation module can be used to analyze instrument performance and for vapor isotope calibration during field campaign measurements.
Malavika Sivan, Thomas Röckmann, Carina van der Veen, and Maria Elena Popa
Atmos. Meas. Tech., 17, 2687–2705, https://doi.org/10.5194/amt-17-2687-2024, https://doi.org/10.5194/amt-17-2687-2024, 2024
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We have set up a measurement system for methane-clumped isotopologues. We have built an extraction and purification system to extract pure methane for these measurements, for samples of various origins, including atmospheric air, for which we need to process about 1000 L of air for one measurement. We report here the technical setup for extraction and measurements, as well as the calibration, and we give an overview of the samples measured so far.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Clément Piel, Daniele Romanini, Morgane Farradèche, Justin Chaillot, Clémence Paul, Nicolas Bienville, Thomas Lauwers, Joana Sauze, Kévin Jaulin, Frédéric Prié, and Amaëlle Landais
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-14, https://doi.org/10.5194/amt-2024-14, 2024
Revised manuscript accepted for AMT
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This paper introduces a new optical gas analyzer based on the Optical-Feedback Cavity-Enhanced Absorption Spectroscopy technique (OF-CEAS) enabling high temporal resolution and high precision measurement of δ18O and concentration of atmospheric O2. The results underscore the good agreement with dual inlet IRMS measurements and the ability of the instrument to monitor biological processes.
Harald Sodemann, Alena Dekhtyareva, Alvaro Fernandez, Andrew Seidl, and Jenny Maccali
Atmos. Meas. Tech., 16, 5181–5203, https://doi.org/10.5194/amt-16-5181-2023, https://doi.org/10.5194/amt-16-5181-2023, 2023
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We describe a device that allows one to produce a continuous stream of water vapour with a specified level of humidity. As a main innovation, we can mix waters with different water isotope composition. Through a series of tests we show that the performance characteristics of the device are in line with specifications. We present two laboratory applications where the device proves useful, first in characterizing instruments, and second for the analysis of water contained in stalagmites.
Stephan Räss, Peter Nyfeler, Paul Wheeler, Will Price, and Markus Christian Leuenberger
Atmos. Meas. Tech., 16, 4489–4505, https://doi.org/10.5194/amt-16-4489-2023, https://doi.org/10.5194/amt-16-4489-2023, 2023
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Due to technological advances clumped-isotope studies have gained importance in recent years. Typically, these studies are performed with high-resolution isotope ratio mass spectrometers (IRMSs) along with a changeover-valve-based dual-inlet system (DIS). We are taking a different approach, namely performing clumped-isotope measurements with a compact low-resolution IRMS with an open-split-based DIS. Currently, we are working with pure-oxygen gas for which we are providing a proof of concept.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Namrata Shanmukh Panji and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4319–4330, https://doi.org/10.5194/amt-16-4319-2023, https://doi.org/10.5194/amt-16-4319-2023, 2023
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Measuring volatile organic compounds (VOCs) in the atmosphere is crucial for understanding air quality and environmental impact. Since these compounds are present in low concentrations, preconcentration of samples is often necessary for accurate detection. To address this issue, we have developed a novel inlet that uses selective permeation to concentrate organic gases in small sample flows. This device offers a promising approach for accurately detecting low levels of VOCs in the atmosphere.
Claudia Grossi, Daniel Rabago, Scott Chambers, Carlos Sáinz, Roger Curcoll, Peter P. S. Otáhal, Eliška Fialová, Luis Quindos, and Arturo Vargas
Atmos. Meas. Tech., 16, 2655–2672, https://doi.org/10.5194/amt-16-2655-2023, https://doi.org/10.5194/amt-16-2655-2023, 2023
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The automatic and low-maintenance radon flux system Autoflux, completed with environmental soil and atmosphere sensors, has been theoretically and experimentally characterized and calibrated under laboratory conditions to be used as transfer standard for in situ measurements. It will offer for the first time long-term measurements to validate radon flux maps used by the climate and the radiation protection communities for assessing the radon gas emissions in the atmosphere.
Lisa Ernle, Monika Akima Ringsdorf, and Jonathan Williams
Atmos. Meas. Tech., 16, 1179–1194, https://doi.org/10.5194/amt-16-1179-2023, https://doi.org/10.5194/amt-16-1179-2023, 2023
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Atmospheric ozone can induce artefacts in volatile organic compound measurements. Laboratory tests were made using GC-MS and PTR-MS aircraft systems under tropospheric and stratospheric conditions of humidity and ozone, with and without sodium thiosulfate filter scrubbers. Ozone in dry air produces some carbonyls and degrades alkenes. The scrubber lifetime depends on ozone concentration, flow rate and humidity. For the troposphere with scrubber, no significant artefacts were found over 14 d.
Lars Mächler, Daniel Baggenstos, Florian Krauss, Jochen Schmitt, Bernhard Bereiter, Remo Walther, Christoph Reinhard, Béla Tuzson, Lukas Emmenegger, and Hubertus Fischer
Atmos. Meas. Tech., 16, 355–372, https://doi.org/10.5194/amt-16-355-2023, https://doi.org/10.5194/amt-16-355-2023, 2023
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We present a new method to extract the gases from ice cores and measure their greenhouse gas composition. The ice is sublimated continuously with a near-infrared laser, releasing the gases, which are then analyzed on a laser absorption spectrometer. The main advantage over previous efforts is a low effective resolution of 1–2 cm. This capability is crucial for the analysis of highly thinned ice, as expected from ongoing drilling efforts to extend ice core history further back in time.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Andrew J. Lindsay and Ezra C. Wood
Atmos. Meas. Tech., 15, 5455–5464, https://doi.org/10.5194/amt-15-5455-2022, https://doi.org/10.5194/amt-15-5455-2022, 2022
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Nitrous acid (HONO) is an important source of the main atmospheric oxidant – the hydroxyl radical (OH). Advances in nitrous acid measurement techniques and calibration methods therefore improve our understanding of atmospheric oxidation processes. In this paper, we present two calibration methods based on photo-dissociating water vapor. These calibration methods are useful alternatives to conventional calibrations that involve a reacting hydrogen chloride vapor with sodium nitrite.
Ying Wang, Wentai Luo, Todd N. Rosenstiel, and James F. Pankow
Atmos. Meas. Tech., 15, 4651–4661, https://doi.org/10.5194/amt-15-4651-2022, https://doi.org/10.5194/amt-15-4651-2022, 2022
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A rapid, sensitive, and precise analytical method was developed for measuring the fractional amounts of the (−) and (+) forms of chiral enantiomeric forms of monoterpenes in air containing biogenic plant emissions. The method uses passive air sampling onto adsorption–thermal desorption (ATD) gas sampling cartridge tubes; this is followed by automatable thermal desorption onto a chiral gas chromatography (GC) column, followed by detection with mass spectrometry (MS).
Zara S. Mir, Matthew Jamieson, Nicholas R. Greenall, Paul W. Seakins, Mark A. Blitz, and Daniel Stone
Atmos. Meas. Tech., 15, 2875–2887, https://doi.org/10.5194/amt-15-2875-2022, https://doi.org/10.5194/amt-15-2875-2022, 2022
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In this work we describe the development and characterisation of an experiment using laser flash photolysis coupled with time-resolved mid-infrared (mid-IR) quantum cascade laser (QCL) absorption spectroscopy, with initial results reported for measurements of the infrared spectrum, kinetics, and product yields for the reaction of the CH2OO Criegee intermediate with SO2. This work has significance for the identification and measurement of reactive trace species in complex systems.
Tatiana Macé, Maitane Iturrate-Garcia, Céline Pascale, Bernhard Niederhauser, Sophie Vaslin-Reimann, and Christophe Sutour
Atmos. Meas. Tech., 15, 2703–2718, https://doi.org/10.5194/amt-15-2703-2022, https://doi.org/10.5194/amt-15-2703-2022, 2022
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LNE developed, with the company 2M PROCESS, a gas reference generator to dynamically generate NH3 reference gas mixtures in the air at very low fractions between 1 and 400 nmol/mol. The procedure defined by LNE for calibrating NH3 analyzers used for monitoring air quality guarantees relative expanded uncertainties lower than 2 % for this measurement range. The results of a comparison organized between METAS and LNE allowed the validation of LNE's reference generator and calibration procedure.
Antonia G. Zogka, Manolis N. Romanias, and Frederic Thevenet
Atmos. Meas. Tech., 15, 2001–2019, https://doi.org/10.5194/amt-15-2001-2022, https://doi.org/10.5194/amt-15-2001-2022, 2022
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We emphasize the application of SIFT-MS to detect two important atmospheric pollutants, i.e., formaldehyde (FM) and glyoxal (GL). FM and GL are secondary products formed by volatile organic compound oxidation in indoor and outdoor environments and play a key role in air quality and climate. We show that SIFT-MS is able to monitor these species selectively and in real time, overcoming the limitations of other, classical analytical techniques used to monitor these species in the atmosphere.
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.
Jean Decker, Éric Fertein, Jonas Bruckhuisen, Nicolas Houzel, Pierre Kulinski, Bo Fang, Weixiong Zhao, Francis Hindle, Guillaume Dhont, Robin Bocquet, Gaël Mouret, Cécile Coeur, and Arnaud Cuisset
Atmos. Meas. Tech., 15, 1201–1215, https://doi.org/10.5194/amt-15-1201-2022, https://doi.org/10.5194/amt-15-1201-2022, 2022
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We present a multiple pass system developed for the CHamber for Atmospheric Reactivity and Metrology of the Environment. This multi-pass cell allows monitoring of atmospheric species at trace levels by high-resolution spectroscopy with long interaction path lengths in the IR and for the first time in the terahertz range. Interesting prospects are highlighted in this frequency domain, such as a high degree of selectivity or the possibility to monitor in real-time atmospheric processes.
Robert F. Berg, Nicola Chiodo, and Eric Georgin
Atmos. Meas. Tech., 15, 819–832, https://doi.org/10.5194/amt-15-819-2022, https://doi.org/10.5194/amt-15-819-2022, 2022
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We made a humidity generator that adds water vapor to a flowing gas. Its range of humidity is useful for calibrating balloon-borne probes to the Earth's stratosphere. The generator’s novel feature is a saturator that comprises 5 m of silicone tubing immersed in water. The length was enough to ensure that the saturator’s output was independent of the dimensions and permeability of the tube. This simple, low-cost design provides an accuracy that is acceptable for many applications.
Guillermo Villena and Jörg Kleffmann
Atmos. Meas. Tech., 15, 627–637, https://doi.org/10.5194/amt-15-627-2022, https://doi.org/10.5194/amt-15-627-2022, 2022
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A continuous source for the generation of pure HONO mixtures was developed and characterized, which is based on the Henry's law solubility of HONO in acidic aqueous solutions. The source shows a fast time response and an excellent long-term stability and can be easily adjusted to HONO mixing ratios in the range 0.05–500 ppb. A general equation based on Henry's law is developed, whereby the HONO concentration of the source can be absolutely calculated with an accuracy of better than 10 %.
Merve Polat, Jesper Baldtzer Liisberg, Morten Krogsbøll, Thomas Blunier, and Matthew S. Johnson
Atmos. Meas. Tech., 14, 8041–8067, https://doi.org/10.5194/amt-14-8041-2021, https://doi.org/10.5194/amt-14-8041-2021, 2021
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We have designed a process for removing methane from a gas stream so that nitrous oxide can be measured without interference. These are both key long-lived greenhouse gases frequently studied in relation to ice cores, plants, water treatment and so on. However, many researchers are not aware of the problem of methane interference, and in addition there have not been good methods available for solving the problem. Here we present and evaluate such a method.
Marcel Snels, Stefania Stefani, Angelo Boccaccini, David Biondi, and Giuseppe Piccioni
Atmos. Meas. Tech., 14, 7187–7197, https://doi.org/10.5194/amt-14-7187-2021, https://doi.org/10.5194/amt-14-7187-2021, 2021
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A novel simulation chamber, PASSxS (Planetary Atmosphere Simulation System for Spectroscopy), has been developed for absorption measurements with a Fourier transform spectrometer (FTS) and possibly a cavity ring-down (CRD) spectrometer, with a sample temperature ranging from 100 K up to 550 K, while the pressure of the gas can be varied up to 60 bar. These temperature and pressure ranges cover a significant part of the planetary atmospheres in the solar system and possibly extrasolar planets.
Lukas Kohl, Markku Koskinen, Tatu Polvinen, Salla Tenhovirta, Kaisa Rissanen, Marjo Patama, Alessandro Zanetti, and Mari Pihlatie
Atmos. Meas. Tech., 14, 4445–4460, https://doi.org/10.5194/amt-14-4445-2021, https://doi.org/10.5194/amt-14-4445-2021, 2021
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We present ShoTGa-FluMS, a measurement system designed for continuous and automated measurements of trace gas and volatile organic compound (VOC) fluxes from plant shoots. ShoTGa-FluMS uses transparent shoot enclosures equipped with cooling elements, automatically replaces fixated CO2, and removes transpired water from the enclosure, thus solving multiple technical problems that have so far prevented automated plant shoot trace gas flux measurements.
Pharahilda M. Steur, Hubertus A. Scheeren, Dave D. Nelson, J. Barry McManus, and Harro A. J. Meijer
Atmos. Meas. Tech., 14, 4279–4304, https://doi.org/10.5194/amt-14-4279-2021, https://doi.org/10.5194/amt-14-4279-2021, 2021
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For understanding the sources and sinks of atmospheric CO2, measurement of stable isotopes has proven to be highly valuable. We present a new method using laser absorption spectroscopy to simultaneously conduct measurements of three CO2 isotopes, directly on dry-air samples. This new method reduces sample preparation time significantly, compared to the conventional method in which measurements are conducted on pure CO2, and avoids measurement biases introduced by CO2 extraction.
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.
Benjamin Birner, William Paplawsky, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Meas. Tech., 14, 2515–2527, https://doi.org/10.5194/amt-14-2515-2021, https://doi.org/10.5194/amt-14-2515-2021, 2021
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The atmospheric helium-to-nitrogen ratio is a promising indicator for circulation changes in the upper atmosphere and fossil fuel burning by humans. We present a very precise analysis method to determine changes in the helium-to-nitrogen ratio of air samples. The method relies on stabilizing the gas flow to a mass spectrometer and continuous removal of reactive gases. These advances enable new insights and monitoring possibilities for anthropogenic and natural processes.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Ikumi Oyabu, Kenji Kawamura, Kyotaro Kitamura, Remi Dallmayr, Akihiro Kitamura, Chikako Sawada, Jeffrey P. Severinghaus, Ross Beaudette, Anaïs Orsi, Satoshi Sugawara, Shigeyuki Ishidoya, Dorthe Dahl-Jensen, Kumiko Goto-Azuma, Shuji Aoki, and Takakiyo Nakazawa
Atmos. Meas. Tech., 13, 6703–6731, https://doi.org/10.5194/amt-13-6703-2020, https://doi.org/10.5194/amt-13-6703-2020, 2020
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Air in polar ice cores provides information on past atmosphere and climate. We present a new method for simultaneously measuring eight gases (CH4, N2O and CO2 concentrations; isotopic ratios of N2 and O2; elemental ratios between N2, O2 and Ar; and total air content) from single ice-core samples with high precision.
Bernhard Bereiter, Béla Tuzson, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Lars Mächler, Daniel Baggenstos, Jochen Schmitt, Hubertus Fischer, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 6391–6406, https://doi.org/10.5194/amt-13-6391-2020, https://doi.org/10.5194/amt-13-6391-2020, 2020
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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Deciphering this archive requires highly accurate and spatially resolved analysis of the very small amount of gas that is trapped in the ice. This is achieved with a mid-IR laser absorption spectrometer that provides simultaneous, high-precision measurements of CH4, N2O, CO2, and δ13C(CO2) and which will be coupled to a quantitative sublimation extraction method.
Natalie I. Keehan, Bellamy Brownwood, Andrey Marsavin, Douglas A. Day, and Juliane L. Fry
Atmos. Meas. Tech., 13, 6255–6269, https://doi.org/10.5194/amt-13-6255-2020, https://doi.org/10.5194/amt-13-6255-2020, 2020
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This paper describes a new instrument (a thermal-dissociation–cavity ring-down spectrometer, TD-CRDS) for the measurement of key atmospheric gaseous and particle-phase molecules containing the nitrate functional group. Several operational considerations affecting the measurements are described, as well as several characterization experiments comparing the TD-CRDS measurements to analogous measurements from other instruments. Examples are given using a TD-CRDS for ambient and laboratory studies.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
Roberto Sommariva, Louisa J. Kramer, Leigh R. Crilley, Mohammed S. Alam, and William J. Bloss
Atmos. Meas. Tech., 13, 1655–1670, https://doi.org/10.5194/amt-13-1655-2020, https://doi.org/10.5194/amt-13-1655-2020, 2020
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Ozone is a key atmospheric pollutant formed through chemical processing of natural and anthropogenic emissions and removed by reaction with organic compounds emitted by plants. We describe a new instrument – the
Total Ozone Reactivity Systemor TORS – that measures the total loss of ozone in the troposphere. The objective of the TORS instrument is to provide an estimate of the organic compounds emitted by plants which are not measured and thus to improve our understanding of the ozone budget.
John W. Birks, Andrew A. Turnipseed, Peter C. Andersen, Craig J. Williford, Stanley Strunk, Brian Carpenter, and Christine A. Ennis
Atmos. Meas. Tech., 13, 1001–1018, https://doi.org/10.5194/amt-13-1001-2020, https://doi.org/10.5194/amt-13-1001-2020, 2020
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We describe a portable calibration source of nitric oxide (NO) based on the photolysis of nitrous oxide. Combining this with a previous photolytic ozone (O3) source yields a calibrator that produces known mixing ratios of NO, O3, and nitrogen dioxide (NO2); NO2 is produced by the reaction of NO with O3. This portable
NO2/NO/O3 calibration source requires no external gas cylinders and can be used as a standard to calibrate O3 and NOx air pollution monitors in the field.
Thomas H. Speak, Mark A. Blitz, Daniel Stone, and Paul W. Seakins
Atmos. Meas. Tech., 13, 839–852, https://doi.org/10.5194/amt-13-839-2020, https://doi.org/10.5194/amt-13-839-2020, 2020
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OH and HO2 radicals are important trace constituents of the atmosphere that are closely coupled via several types of reaction. This paper describes a new laboratory method to simultaneously determine OH kinetics and HO2 yields from chemical processes. The instrument also provides some time resolution on HO2 detection allowing one to separate HO2 produced from the target reaction from HO2 arising from secondary chemistry. Examples of applications are presented.
Ece Satar, Peter Nyfeler, Bernhard Bereiter, Céline Pascale, Bernhard Niederhauser, and Markus Leuenberger
Atmos. Meas. Tech., 13, 101–117, https://doi.org/10.5194/amt-13-101-2020, https://doi.org/10.5194/amt-13-101-2020, 2020
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Good-quality measurements of atmospheric trace gases are only possible with regular calibrations and stable measurements from the standard cylinders. This study investigates instabilities due to surface effects on newly built aluminum and steel cylinders. We present measurements over a set of temperature and pressure ranges for the amount fractions of CO2, CO, CH4 and H2O using a commercial and a novel laser spectroscopic analyzer.
Ece Satar, Peter Nyfeler, Céline Pascale, Bernhard Niederhauser, and Markus Leuenberger
Atmos. Meas. Tech., 13, 119–130, https://doi.org/10.5194/amt-13-119-2020, https://doi.org/10.5194/amt-13-119-2020, 2020
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To ensure the best preparation and measurement conditions for trace gases, usage of coated materials is in demand in gas metrology and atmospheric measurement communities. In this article, the previously introduced aluminum measurement chamber is used to investigate materials such as glass, aluminum, copper, brass, steel and three different commercially available coatings. Our measurements focus on temperature and pressure dependencies for the species CO2, CO, CH4 and H2O using a CRDS analyzer.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
Tesfaye A. Berhanu, John Hoffnagle, Chris Rella, David Kimhak, Peter Nyfeler, and Markus Leuenberger
Atmos. Meas. Tech., 12, 6803–6826, https://doi.org/10.5194/amt-12-6803-2019, https://doi.org/10.5194/amt-12-6803-2019, 2019
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Accurate measurement of variations in atmospheric O2 can provide useful information about atmospheric, biospheric, and oceanic processes, which is a challenge for existing measurement techniques. Here, we introduce a newly built high-precision, stable CRDS analyzer (Picarro G2207) that can measure O2 mixing ratios with a short-term precision of < 1 ppm and only requires calibration every 12 h. Measurements from tower and mountain sites are also presented.
Markus Leiminger, Stefan Feil, Paul Mutschlechner, Arttu Ylisirniö, Daniel Gunsch, Lukas Fischer, Alfons Jordan, Siegfried Schobesberger, Armin Hansel, and Gerhard Steiner
Atmos. Meas. Tech., 12, 5231–5246, https://doi.org/10.5194/amt-12-5231-2019, https://doi.org/10.5194/amt-12-5231-2019, 2019
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We introduce an alternative type of atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF) with the main difference of using hexapole instead of quadrupole ion guides. The transfer of cluster ions through the hexapoles was characterised with focus on transmission efficiency, mass range and fragmentation of cluster ions. At the CERN CLOUD experiment we compared the performance of the ioniAPi-TOF with a standard quadrupole APi-TOF under controlled conditions.
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Short summary
In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
In this study, a calibration device for OH and HO2 instruments is characterized at pressures of...
