Articles | Volume 16, issue 22
https://doi.org/10.5194/acp-16-14397-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-14397-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
18 Nov 2016
Research article |
| 18 Nov 2016
Chemical characterization of organic particulate matter from on-road traffic in São Paulo, Brazil
Beatriz Sayuri Oyama
CORRESPONDING AUTHOR
Institute of Astronomy, Geophysics and Atmospheric Sciences,
University of São Paulo, São Paulo, Brazil
Institute for
Marine and Atmospheric Research (IMAU), Utrecht, Utrecht University, the
Netherlands
Maria de Fátima Andrade
Institute of Astronomy, Geophysics and Atmospheric Sciences,
University of São Paulo, São Paulo, Brazil
Pierre Herckes
School of Molecular Sciences, Arizona State
University, Tempe, USA
Ulrike Dusek
Institute for
Marine and Atmospheric Research (IMAU), Utrecht, Utrecht University, the
Netherlands
Center for Isotope Research, University of
Groningen, Groningen, the Netherlands
Thomas Röckmann
Institute for
Marine and Atmospheric Research (IMAU), Utrecht, Utrecht University, the
Netherlands
Rupert Holzinger
Institute for
Marine and Atmospheric Research (IMAU), Utrecht, Utrecht University, the
Netherlands
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Biogeosciences, 21, 3183–3199, https://doi.org/10.5194/bg-21-3183-2024, https://doi.org/10.5194/bg-21-3183-2024, 2024
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Carbon monoxide (CO) is regarded as an important indirect greenhouse gas. Soils can emit and take up CO, but, until now, uncertainty remains as to which process dominates in tropical rainforests. We present the first soil CO flux measurements from a tropical rainforest. Based on our observations, we report that tropical rainforest soils are a net source of CO. In addition, we show that valley streams and inundated areas are likely additional hot spots of CO in the ecosystem.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
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.
Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
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We evaluated the time-of-flight aerosol chemical speciation monitor (TOF-ACSM) following the implementation of the PM2.5 aerodynamic lens and a capture vaporizer (CV). The results showed that it significantly improved the accuracy and precision of ACSM in the field observations. The paper elucidates the measurement outcomes of various instruments and provides an analysis of their biases. This comprehensive evaluation is expected to benefit the ACSM community and other aerosol field measurements.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
EGUsphere, https://doi.org/10.5194/egusphere-2023-2262, https://doi.org/10.5194/egusphere-2023-2262, 2023
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by Lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve Lidar measurements.
Robbert P. J. Moonen, Getachew A. Adnew, Oscar K. Hartogensis, Jordi Vilà-Guerau de Arellano, David J. Bonell Fontas, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5787–5810, https://doi.org/10.5194/amt-16-5787-2023, https://doi.org/10.5194/amt-16-5787-2023, 2023
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Isotope fluxes allow for net ecosystem gas exchange fluxes to be partitioned into sub-components like plant assimilation, respiration and transpiration, which can help us better understand the environmental drivers of each partial flux. We share the results of a field campaign isotope fluxes were derived using a combination of laser spectroscopy and eddy covariance. We found lag times and high frequency signal loss in the isotope fluxes we derived and present methods to correct for both.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Tim René de Groot, Anne Margriet Mol, Katherine Mesdag, Pierre Ramond, Rachel Ndhlovu, Julia Catherine Engelmann, Thomas Röckmann, and Helge Niemann
Biogeosciences, 20, 3857–3872, https://doi.org/10.5194/bg-20-3857-2023, https://doi.org/10.5194/bg-20-3857-2023, 2023
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This study investigates methane dynamics in the Wadden Sea. Our measurements revealed distinct variations triggered by seasonality and tidal forcing. The methane budget was higher in warmer seasons but surprisingly high in colder seasons. Methane dynamics were amplified during low tides, flushing the majority of methane into the North Sea or releasing it to the atmosphere. Methanotrophic activity was also elevated during low tide but mitigated only a small fraction of the methane efflux.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Particulate matter (PM) is a harmful air pollutant that depends on the complex mixture of natural and anthropogenic emissions into the atmosphere. Thus, in different regions and seasons, the way that PM is formed and grows can differ. In this study, we use a combined statistical analysis of the chemical composition and particle size distribution to determine what drives particle formation and growth across seasons, using varying wind directions to elucidate the role of different sources.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Truls Andersen, Zhao Zhao, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys., 23, 5191–5216, https://doi.org/10.5194/acp-23-5191-2023, https://doi.org/10.5194/acp-23-5191-2023, 2023
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The Upper Silesian Coal Basin, Poland, is one of the hot spots of methane emissions in Europe. Using an uncrewed aerial vehicle (UAV), we performed atmospheric measurements of methane concentrations downwind of five ventilation shafts in this region and determined the emission rates from the individual shafts. We found a strong correlation between quantified shaft-averaged emission rates and hourly inventory data, which also allows us to estimate the methane emissions from the entire region.
David R. Worton, Sergi Moreno, Kieran O'Daly, and Rupert Holzinger
Atmos. Meas. Tech., 16, 1061–1072, https://doi.org/10.5194/amt-16-1061-2023, https://doi.org/10.5194/amt-16-1061-2023, 2023
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Proton-transfer-reaction mass spectrometry is widely used in the environmental, health, and food and beverage sectors. As a result, there is a need for accurate and comparable measurements. In this work we have developed a 20-component gravimetrically prepared traceable primary reference material (gas standard in a high-pressure cylinder) to enable quantitative and comparable measurements. The accuracy of all components was better than 3 %–10 % with stabilities of better than 1–2 years.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
Roland Vernooij, Patrik Winiger, Martin Wooster, Tercia Strydom, Laurent Poulain, Ulrike Dusek, Mark Grosvenor, Gareth J. Roberts, Nick Schutgens, and Guido R. van der Werf
Atmos. Meas. Tech., 15, 4271–4294, https://doi.org/10.5194/amt-15-4271-2022, https://doi.org/10.5194/amt-15-4271-2022, 2022
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Landscape fires are a substantial emitter of greenhouse gases and aerosols. Previous studies have indicated savanna emission factors to be highly variable. Improving fire emission estimates, and understanding future climate- and human-induced changes in fire regimes, requires in situ measurements. We present a drone-based method that enables the collection of a large amount of high-quality emission factor measurements that do not have the biases of aircraft or surface measurements.
Stephen M. Platt, Øystein Hov, Torunn Berg, Knut Breivik, Sabine Eckhardt, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Markus Fiebig, Rebecca Fisher, Georg Hansen, Hans-Christen Hansson, Jost Heintzenberg, Ove Hermansen, Dominic Heslin-Rees, Kim Holmén, Stephen Hudson, Roland Kallenborn, Radovan Krejci, Terje Krognes, Steinar Larssen, David Lowry, Cathrine Lund Myhre, Chris Lunder, Euan Nisbet, Pernilla B. Nizzetto, Ki-Tae Park, Christina A. Pedersen, Katrine Aspmo Pfaffhuber, Thomas Röckmann, Norbert Schmidbauer, Sverre Solberg, Andreas Stohl, Johan Ström, Tove Svendby, Peter Tunved, Kjersti Tørnkvist, Carina van der Veen, Stergios Vratolis, Young Jun Yoon, Karl Espen Yttri, Paul Zieger, Wenche Aas, and Kjetil Tørseth
Atmos. Chem. Phys., 22, 3321–3369, https://doi.org/10.5194/acp-22-3321-2022, https://doi.org/10.5194/acp-22-3321-2022, 2022
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Here we detail the history of the Zeppelin Observatory, a unique global background site and one of only a few in the high Arctic. We present long-term time series of up to 30 years of atmospheric components and atmospheric transport phenomena. Many of these time series are important to our understanding of Arctic and global atmospheric composition change. Finally, we discuss the future of the Zeppelin Observatory and emerging areas of future research on the Arctic atmosphere.
Roland Vernooij, Ulrike Dusek, Maria Elena Popa, Peng Yao, Anupam Shaikat, Chenxi Qiu, Patrik Winiger, Carina van der Veen, Thomas Callum Eames, Natasha Ribeiro, and Guido R. van der Werf
Atmos. Chem. Phys., 22, 2871–2890, https://doi.org/10.5194/acp-22-2871-2022, https://doi.org/10.5194/acp-22-2871-2022, 2022
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Landscape fires are a major source of greenhouse gases and aerosols, particularly in sub-tropical savannas. Stable carbon isotopes in emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to greenhouse gases and aerosols if the process is well understood. This helps us to link individual vegetation types to emissions, identify biomass burning emissions in the atmosphere, and improve the reconstruction of historic fire regimes.
Rupert Holzinger, Oliver Eppers, Kouji Adachi, Heiko Bozem, Markus Hartmann, Andreas Herber, Makoto Koike, Dylan B. Millet, Nobuhiro Moteki, Sho Ohata, Frank Stratmann, and Atsushi Yoshida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-95, https://doi.org/10.5194/acp-2022-95, 2022
Revised manuscript not accepted
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In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-68, https://doi.org/10.5194/acp-2022-68, 2022
Publication in ACP not foreseen
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The sulfur isotopes (32S and 34S) were studied to understand the sources, sinks and processes of carbonyl sulphide (COS) in the atmosphere. COS is an important source of sulfur aerosol in the stratosphere (SSA). Few measurements of COS and SSA exist, but with our 1D model, we were able to match them and show the importance of COS to sulfate formation. Moreover, we are able to highlight some important processes for the COS budget and where measurements may fill a gap in current knowledge.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
Haiyan Ni, Ru-Jin Huang, Max M. Cosijn, Lu Yang, Jie Guo, Junji Cao, and Ulrike Dusek
Atmos. Chem. Phys., 20, 16041–16053, https://doi.org/10.5194/acp-20-16041-2020, https://doi.org/10.5194/acp-20-16041-2020, 2020
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We investigated sources of carbonaceous aerosols in Beijing and Xi'an during severe winter haze. Elemental carbon (EC) was dominated by vehicle emissions in Xi’an and coal burning in Beijing. Organic carbon (OC) increment during haze days was driven by the increase in primary and secondary OC (SOC). SOC was more from fossil sources in Beijing than Xi’an, especially during haze days. In Xi’an, no strong day–night differences in EC or OC sources suggest a large accumulation of particles.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
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.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Haiyan Ni, Ru-Jin Huang, Junji Cao, Jie Guo, Haoyue Deng, and Ulrike Dusek
Atmos. Chem. Phys., 19, 15609–15628, https://doi.org/10.5194/acp-19-15609-2019, https://doi.org/10.5194/acp-19-15609-2019, 2019
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We present a 1-year source apportionment record of carbonaceous aerosols in Xi'an, China. Biomass burning strongly increases in winter, while seasonal changes of coal and liquid fossil fuel combustion are moderate. We find strong evidence for fossil secondary OC formation during the warm period that is further enhanced in stagnant, polluted conditions due to longer atmospheric residence times. At the same time we find that water-insoluble (primary) fossil is lost due to photochemical processing.
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Haiyan Ni, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Haoyue Deng, Anita Aerts-Bijma, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 19, 10405–10422, https://doi.org/10.5194/acp-19-10405-2019, https://doi.org/10.5194/acp-19-10405-2019, 2019
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We apply radiocarbon source apportionment of more volatile organic carbon (mvOC) to winter aerosol samples from six Chinese cities. We find a consistently larger contribution of fossil sources to mvOC than to secondary or total organic carbon. Fossil mvOC concentrations are strongly correlated with primary fossil OC but not with secondary fossil OC. The variability in nonfossil mvOC seems to be related to both primary and secondary biomass burning sources.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Haiyan Ni, Ru-Jin Huang, Junji Cao, Weiguo Liu, Ting Zhang, Meng Wang, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 18, 16363–16383, https://doi.org/10.5194/acp-18-16363-2018, https://doi.org/10.5194/acp-18-16363-2018, 2018
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Seasonal changes in organic carbon (OC) and elemental carbon (EC) sources in Xi'an, China, are investigated based on measurements of radiocarbon and the stable isotope 13C. Relative contributions to EC from biomass burning, coal combustion, and vehicle emissions change substantially between different seasons. Biomass burning contributes 60 % to the EC increment in winter. Comparing concentrations and sources of primary OC to total OC suggests non-negligible OC loss due to active photochemistry.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Sergio Ibarra-Espinosa, Rita Ynoue, Shane O'Sullivan, Edzer Pebesma, María de Fátima Andrade, and Mauricio Osses
Geosci. Model Dev., 11, 2209–2229, https://doi.org/10.5194/gmd-11-2209-2018, https://doi.org/10.5194/gmd-11-2209-2018, 2018
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An emissions inventory is a compilation of the mass of pollutants released by different sources. The quantification of vehicular emissions is difficult because these sources are in movement across streets. Also, emissions processes are multiple and complex. In this paper, we present an open-source software for calculating spatial vehicular emissions, including exhaust, evaporation and wear, named VEIN. The software is an R package available at
https://github.com/atmoschem/vein.
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
Y. Mancilla, A. Mendoza, M. P. Fraser, and P. Herckes
Atmos. Chem. Phys., 16, 953–970, https://doi.org/10.5194/acp-16-953-2016, https://doi.org/10.5194/acp-16-953-2016, 2016
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Chemical characterization of fine aerosol was conducted due to air pollution by fine particles in the last decade. The diagnostic ratios and CMB receptor model based on organic markers showed that gasoline- and diesel-powered vehicles are the main emission sources (CMB = 64 %) of this class of organic compounds in PM2.5. Other pyrogenic sources as contributors to fine aerosols. Fine particles are related to human health impacts. In addition, these results can be useful for policy making.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
J. Timkovsky, A. W. H. Chan, T. Dorst, A. H. Goldstein, B. Oyama, and R. Holzinger
Atmos. Meas. Tech., 8, 5177–5187, https://doi.org/10.5194/amt-8-5177-2015, https://doi.org/10.5194/amt-8-5177-2015, 2015
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
R. Holzinger
Atmos. Meas. Tech., 8, 3903–3922, https://doi.org/10.5194/amt-8-3903-2015, https://doi.org/10.5194/amt-8-3903-2015, 2015
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 2014
K. Pohl, M. Cantwell, P. Herckes, and R. Lohmann
Atmos. Chem. Phys., 14, 7431–7443, https://doi.org/10.5194/acp-14-7431-2014, https://doi.org/10.5194/acp-14-7431-2014, 2014
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
J. Brito, L. V. Rizzo, P. Herckes, P. C. Vasconcellos, S. E. S. Caumo, A. Fornaro, R. Y. Ynoue, P. Artaxo, and M. F. Andrade
Atmos. Chem. Phys., 13, 12199–12213, https://doi.org/10.5194/acp-13-12199-2013, https://doi.org/10.5194/acp-13-12199-2013, 2013
J. Timkovsky, P. Gankema, R. Pierik, and R. Holzinger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-6-9005-2013, https://doi.org/10.5194/amtd-6-9005-2013, 2013
Preprint withdrawn
R. Holzinger, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, and J. Timkovsky
Atmos. Chem. Phys., 13, 10125–10141, https://doi.org/10.5194/acp-13-10125-2013, https://doi.org/10.5194/acp-13-10125-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
P. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
B. Ervens, Y. Wang, J. Eagar, W. R. Leaitch, A. M. Macdonald, K. T. Valsaraj, and P. Herckes
Atmos. Chem. Phys., 13, 5117–5135, https://doi.org/10.5194/acp-13-5117-2013, https://doi.org/10.5194/acp-13-5117-2013, 2013
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
J.-H. Park, A. H. Goldstein, J. Timkovsky, S. Fares, R. Weber, J. Karlik, and R. Holzinger
Atmos. Chem. Phys., 13, 1439–1456, https://doi.org/10.5194/acp-13-1439-2013, https://doi.org/10.5194/acp-13-1439-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Diverging trends in aerosol sulfate and nitrate measured in the remote North Atlantic in Barbados are attributed to clean air policies, African smoke, and anthropogenic emissions
Diverse sources and aging change the mixing state and ice nucleation properties of aerosol particles over the western Pacific and Southern Ocean
The water-insoluble organic carbon in PM2.5 of typical Chinese urban areas: light-absorbing properties, potential sources, radiative forcing effects, and a possible light-absorbing continuum
Measurement report: Size-resolved secondary organic aerosol formation modulated by aerosol water uptake in wintertime haze
In situ measurement of organic aerosol molecular markers in urban Hong Kong during a summer period: temporal variations and source apportionment
Technical note: Determining chemical composition of atmospheric single particles by a standard-free mass calibration algorithm
Different formation pathways of nitrogen-containing organic compounds in aerosols and fog water in northern China
Impact of weather patterns and meteorological factors on PM2.5 and O3 responses to the COVID-19 lockdown in China
Daytime and nighttime aerosol soluble iron formation in clean and slightly polluted moist air in a coastal city in eastern China
Non-negligible secondary contribution to brown carbon in autumn and winter: inspiration from particulate nitrated and oxygenated aromatic compounds in urban Beijing
Simultaneous organic aerosol source apportionment at two Antarctic sites reveals large-scale and ecoregion-specific components
Measurement report: Optical characterization, seasonality, and sources of brown carbon in fine aerosols from Tianjin, North China: year-round observations
Bayesian inference-based estimation of hourly primary and secondary organic carbon in suburban Hong Kong: multi-temporal-scale variations and evolution characteristics during PM2.5 episodes
Vertical variability of aerosol properties and trace gases over a remote marine region: A case study over Bermuda
Hygroscopic Growth and Activation Changed Submicron Aerosol Composition and Properties in North China Plain
Measurement report: Characteristics of nitrogen-containing organics in PM2.5 in Ürümqi, northwestern China – differential impacts of combustion of fresh and aged biomass materials
Measurement report: Formation of tropospheric brown carbon in a lifting air mass
Measurement report: Bio-physicochemistry of tropical clouds at Maïdo (Réunion, Indian Ocean): overview of results from the BIO-MAÏDO campaign
Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign
High Altitude Aerosol Chemical Characterization and Source Identification: Insights from the CALISHTO Campaign
Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique
Measurement report: Evaluation of the TOF-ACSM-CV for PM1.0 and PM2.5 measurements during the RITA-2021 field campaign
Sea salt reactivity over the northwest Atlantic: an in-depth look using the airborne ACTIVATE dataset
Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia
Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes
Chemical composition, sources and formation mechanism of urban PM2.5 in Southwest China: a case study at the beginning of 2023
Chemical characterization of atmospheric aerosols at a high-altitude mountain site: a study of source apportionment
Composition and sources of carbonaceous aerosol in the European Arctic at Zeppelin Observatory, Svalbard (2017 to 2020)
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
Elucidating the mechanisms of atmospheric new particle formation in the highly polluted Po Valley, Italy
Differences in aerosol and cloud properties along the central California coast when winds change from northerly to southerly
Local ship speed reduction effect on black carbon emissions measured at remote marine station
Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean
Evolution of nucleophilic high molecular-weight organic compounds in ambient aerosols: a case study
Fractional solubility of iron in mineral dust aerosols over coastal Namibia: a link to marine biogenic emissions?
Real-world observations of reduced nitrogen and ultrafine particles in commercial cooking organic aerosol emissions
Source apportionment of PM2.5 in Montréal, Canada, and health risk assessment for potentially toxic elements
Physicochemical and temporal characteristics of individual atmospheric aerosol particles in urban Seoul during KORUS-AQ campaign: insights from single-particle analysis
Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic
Short-term source apportionment of fine particulate matter with time-dependent profiles using SoFi Pro: exploring the reliability of rolling positive matrix factorization (PMF) applied to bihourly molecular and elemental tracer data
Particulate-bound alkyl nitrate pollution and formation mechanisms in Beijing, China
Measurement report: Impact of emission control measures on environmental persistent free radicals and reactive oxygen species – A short-term case study in Beijing
Characterization of water-soluble brown carbon chromophores from wildfire plumes in the western USA using size-exclusion chromatography
Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 1: Observational data analysis
Measurement report: Brown carbon aerosol in polluted urban air of the North China Plain – day–night differences in the chromophores and optical properties
Aerosol optical properties within the atmospheric boundary layer predicted from ground-based observations compared to Raman lidar retrievals during RITA-2021
Measurement report: Secondary organic aerosols at a forested mountain site in southeastern China
Cassandra J. Gaston, Joseph M. Prospero, Kristen Foley, Havala O. T. Pye, Lillian Custals, Edmund Blades, Peter Sealy, and James A. Christie
Atmos. Chem. Phys., 24, 8049–8066, https://doi.org/10.5194/acp-24-8049-2024, https://doi.org/10.5194/acp-24-8049-2024, 2024
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To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate in Barbados and compared them to model predictions from EPA’s Air QUAlity TimE Series (EQUATES). Nitrate was stable, except for spikes in 2008 and 2010 due to transported smoke. Sulfate decreased in the 1990s due to reductions in sulfur dioxide (SO2) in the US and Europe; then it increased in the 2000s, likely due to anthropogenic emissions from Africa.
Jiao Xue, Tian Zhang, Keyhong Park, Jinpei Yan, Young Jun Yoon, Jiyeon Park, and Bingbing Wang
Atmos. Chem. Phys., 24, 7731–7754, https://doi.org/10.5194/acp-24-7731-2024, https://doi.org/10.5194/acp-24-7731-2024, 2024
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Ice formation by particles is an important way of making mixed-phase and ice clouds. We found that particles collected in the marine atmosphere exhibit diverse ice nucleation abilities and mixing states. Sea salt mixed-sulfate particles were enriched in ice-nucleating particles. Selective aging on sea salt particles made particle populations more externally mixed. Characterizations of particles and their mixing state are needed for a better understanding of aerosol–cloud interactions.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 24, 7755–7772, https://doi.org/10.5194/acp-24-7755-2024, https://doi.org/10.5194/acp-24-7755-2024, 2024
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In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibiting the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O'Dowd
Atmos. Chem. Phys., 24, 7687–7698, https://doi.org/10.5194/acp-24-7687-2024, https://doi.org/10.5194/acp-24-7687-2024, 2024
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, and Hai Guo
Atmos. Chem. Phys., 24, 7085–7100, https://doi.org/10.5194/acp-24-7085-2024, https://doi.org/10.5194/acp-24-7085-2024, 2024
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Organic aerosol is ubiquitous in the atmosphere and largely explains the gap between current levels of fine particulate matter in many cities and the World Health Organization guideline values. This study highlights the dominant contributions of cooking emissions to organic aerosol when marine air prevailed in Hong Kong, which were occasionally overwhelmed by aromatics-derived secondary organic aerosol in continental ouflows.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Wei Sun, Xiaodong Hu, Yuzhen Fu, Guohua Zhang, Yujiao Zhu, Xinfeng Wang, Caiqing Yan, Likun Xue, He Meng, Bin Jiang, Yuhong Liao, Xinming Wang, Ping'an Peng, and Xinhui Bi
Atmos. Chem. Phys., 24, 6987–6999, https://doi.org/10.5194/acp-24-6987-2024, https://doi.org/10.5194/acp-24-6987-2024, 2024
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The formation pathways of nitrogen-containing compounds (NOCs) in the atmosphere remain unclear. We investigated the composition of aerosols and fog water by state-of-the-art mass spectrometry and compared the formation pathways of NOCs. We found that NOCs in aerosols were mainly formed through nitration reaction, while ammonia addition played a more important role in fog water. The results deepen our understanding of the processes of organic particulate pollution.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
Atmos. Chem. Phys., 24, 6539–6553, https://doi.org/10.5194/acp-24-6539-2024, https://doi.org/10.5194/acp-24-6539-2024, 2024
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We attempt to use a novel structural self-organising map and machine learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights that temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
Atmos. Chem. Phys., 24, 6495–6508, https://doi.org/10.5194/acp-24-6495-2024, https://doi.org/10.5194/acp-24-6495-2024, 2024
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
Atmos. Chem. Phys., 24, 6525–6538, https://doi.org/10.5194/acp-24-6525-2024, https://doi.org/10.5194/acp-24-6525-2024, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAH and NAC concentrations were much higher during heating than before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
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Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 5803–5821, https://doi.org/10.5194/acp-24-5803-2024, https://doi.org/10.5194/acp-24-5803-2024, 2024
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal-scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Taiwo Adedayo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Johnathan W. Hair, Miguel Ricardo A. Hilario, Chris A. Hostetler, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Cassidy Soloff, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke Ziemba, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2024-1065, https://doi.org/10.5194/egusphere-2024-1065, 2024
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This study uses airborne data to examine vertical profiles of trace gases, aerosol particles, and meteorological variables over a remote marine area (Bermuda). Results show distinct differences based on both air mass source region (North America, Ocean, Caribbean/North Africa) and altitude for a given air mass type. This work highlights the sensitivity of remote marine areas to long-range transport and the importance of considering vertical dependence of trace gas and aerosol properties.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
EGUsphere, https://doi.org/10.5194/egusphere-2024-998, https://doi.org/10.5194/egusphere-2024-998, 2024
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We deployed an advanced aerosol-fog sampling system at a rural site in the North China Plain to investigate the impact of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient RH conditions, and RH levels would impact significantly on aerosol sampling through aerosol swelling effect.
Yi-Jia Ma, Yu Xu, Ting Yang, Hong-Wei Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 24, 4331–4346, https://doi.org/10.5194/acp-24-4331-2024, https://doi.org/10.5194/acp-24-4331-2024, 2024
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This study provides field-based evidence about the differential impacts of combustion of fresh and aged biomass materials on aerosol nitrogen-containing organic compounds (NOCs) in different seasons in Ürümqi, bridging the linkages between the observations and previous laboratory studies showing the formation mechanisms of NOCs.
Can Wu, Xiaodi Liu, Ke Zhang, Si Zhang, Cong Cao, Jianjun Li, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-891, https://doi.org/10.5194/egusphere-2024-891, 2024
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Brown carbon (BrC) is prevalent in the troposphere, and can efficiently absorb solar and terrestrial radiation. Our observations manifested that the enhanced light-absorption of BrC relative to black carbon at the tropopause can be attributed to the formation of nitrogen-containing organic compounds through the aqueous-phase reactions of carbonyls with ammonium.
Maud Leriche, Pierre Tulet, Laurent Deguillaume, Frédéric Burnet, Aurélie Colomb, Agnès Borbon, Corinne Jambert, Valentin Duflot, Stéphan Houdier, Jean-Luc Jaffrezo, Mickaël Vaïtilingom, Pamela Dominutti, Manon Rocco, Camille Mouchel-Vallon, Samira El Gdachi, Maxence Brissy, Maroua Fathalli, Nicolas Maury, Bert Verreyken, Crist Amelynck, Niels Schoon, Valérie Gros, Jean-Marc Pichon, Mickael Ribeiro, Eric Pique, Emmanuel Leclerc, Thierry Bourrianne, Axel Roy, Eric Moulin, Joël Barrie, Jean-Marc Metzger, Guillaume Péris, Christian Guadagno, Chatrapatty Bhugwant, Jean-Mathieu Tibere, Arnaud Tournigand, Evelyn Freney, Karine Sellegri, Anne-Marie Delort, Pierre Amato, Muriel Joly, Jean-Luc Baray, Pascal Renard, Angelica Bianco, Anne Réchou, and Guillaume Payen
Atmos. Chem. Phys., 24, 4129–4155, https://doi.org/10.5194/acp-24-4129-2024, https://doi.org/10.5194/acp-24-4129-2024, 2024
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Aerosol particles in the atmosphere play a key role in climate change and air pollution. A large number of aerosol particles are formed from the oxidation of volatile organic compounds (VOCs and secondary organic aerosols – SOA). An important field campaign was organized on Réunion in March–April 2019 to understand the formation of SOA in a tropical atmosphere mostly influenced by VOCs emitted by forest and in the presence of clouds. This work synthesizes the results of this campaign.
Ryan N. Farley, James E. Lee, Laura-Hélèna Rivellini, Alex K. Y. Lee, Rachael Dal Porto, Christopher D. Cappa, Kyle Gorkowski, Abu Sayeed Md Shawon, Katherine B. Benedict, Allison C. Aiken, Manvendra K. Dubey, and Qi Zhang
Atmos. Chem. Phys., 24, 3953–3971, https://doi.org/10.5194/acp-24-3953-2024, https://doi.org/10.5194/acp-24-3953-2024, 2024
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The black carbon aerosol composition and mixing state were characterized using a soot particle aerosol mass spectrometer. Single-particle measurements revealed the major role of atmospheric processing in modulating the black carbon mixing state. A significant fraction of soot particles were internally mixed with oxidized organic aerosol and sulfate, with implications for activation as cloud nuclei.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
EGUsphere, https://doi.org/10.5194/egusphere-2024-737, https://doi.org/10.5194/egusphere-2024-737, 2024
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PM1 chemical characterization and PMF source apportionment on the combined organic and inorganic fraction took place at the high-altitude (HAC)2 station. Cloud presence was found to reduce PM1 concentrations, affecting sulphate more than organics. Interstitial aerosol was richer in low hygroscopic organics and acidic inorganics, compared to activated. Higher relative abundance of eBC compared to the other components was revealed for FT conditions compared to PBL.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
EGUsphere, https://doi.org/10.5194/egusphere-2024-736, https://doi.org/10.5194/egusphere-2024-736, 2024
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The water solubility of secondary organic aerosols (SOA) is a crucial factor in determining their hygroscopicity and climatic impact. Stable carbon isotope and mass spectrometry techniques were combined to assess the water solubility of SOA with different aging degrees in a coastal megacity in China. This work revealed a much higher water-soluble fraction of aged SOA compared to fresh SOA, indicating that the aging degree of SOA has considerable impacts on its water solubility.
Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
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We evaluated the time-of-flight aerosol chemical speciation monitor (TOF-ACSM) following the implementation of the PM2.5 aerodynamic lens and a capture vaporizer (CV). The results showed that it significantly improved the accuracy and precision of ACSM in the field observations. The paper elucidates the measurement outcomes of various instruments and provides an analysis of their biases. This comprehensive evaluation is expected to benefit the ACSM community and other aerosol field measurements.
Eva-Lou Edwards, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Claire E. Robinson, Michael A. Shook, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 3349–3378, https://doi.org/10.5194/acp-24-3349-2024, https://doi.org/10.5194/acp-24-3349-2024, 2024
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We investigate Cl− depletion in sea salt particles over the northwest Atlantic from December 2021 to June 2022 using an airborne dataset. Losses of Cl− are greatest in May and least in December–February and March. Inorganic acidic species can account for all depletion observed for December–February, March, and June near Bermuda but none in May. Quantifying Cl− depletion as a percentage captures seasonal trends in depletion but fails to convey the effects it may have on atmospheric oxidation.
Yue Sun, Yujiao Zhu, Yanbin Qi, Lanxiadi Chen, Jiangshan Mu, Ye Shan, Yu Yang, Yanqiu Nie, Ping Liu, Can Cui, Ji Zhang, Mingxuan Liu, Lingli Zhang, Yufei Wang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 24, 3241–3256, https://doi.org/10.5194/acp-24-3241-2024, https://doi.org/10.5194/acp-24-3241-2024, 2024
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Field observations were conducted at the summit of Changbai Mountain in northeast Asia. The cumulative number concentration of ice-nucleating particles (INPs) varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 ℃. Biological INPs (bio-INPs) accounted for the majority of INPs, and the proportion exceeded 90% above −13.0 ℃. Planetary boundary layer height, valley breezes, and long-distance transport of air mass influence the abundance of bio-INPs.
Cuizhi Sun, Yongyun Zhang, Baoling Liang, Min Gao, Xi Sun, Fei Li, Xue Ni, Qibin Sun, Hengjia Ou, Dexian Chen, Shengzhen Zhou, and Jun Zhao
Atmos. Chem. Phys., 24, 3043–3063, https://doi.org/10.5194/acp-24-3043-2024, https://doi.org/10.5194/acp-24-3043-2024, 2024
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In a May–June 2021 expedition in the South China Sea, we analyzed black and brown carbon in marine aerosols, key to light absorption and climate impact. Using advanced in situ and microscope techniques, we observed particle size, structure, and tar balls mixed with various elements. Results showed biomass burning and fossil fuels majorly influence light absorption, especially during significant burning events. This research aids the understanding of carbonaceous aerosols' role in marine climate.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-37, https://doi.org/10.5194/egusphere-2024-37, 2024
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Targeted derivatization and non-targeted analysis with FT-ICR MS were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in the real samples.
C. Isabel Moreno, Radovan Krejci, Jean-Luc Jaffrezo, Gaëlle Uzu, Andrés Alastuey, Marcos F. Andrade, Valeria Mardóñez, Alkuin Maximilian Koenig, Diego Aliaga, Claudia Mohr, Laura Ticona, Fernando Velarde, Luis Blacutt, Ricardo Forno, David N. Whiteman, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 24, 2837–2860, https://doi.org/10.5194/acp-24-2837-2024, https://doi.org/10.5194/acp-24-2837-2024, 2024
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Aerosol chemical composition (ions, sugars, carbonaceous matter) from 2011 to 2020 was studied at Mt. Chacaltaya (5380 m a.s.l., Bolivian Andes). Minimum concentrations occur in the rainy season with maxima in the dry and transition seasons. The origins of the aerosol are located in a radius of hundreds of kilometers: nearby urban and rural areas, natural biogenic emissions, vegetation burning from Amazonia and Chaco, Pacific Ocean emissions, soil dust, and Peruvian volcanism.
Junke Zhang, Yunfei Su, Chunying Chen, Wenkai Guo, Qinwen Tan, Miao Feng, Danlin Song, Tao Jiang, Qiang Chen, Yuan Li, Wei Li, Yizhi Wang, Xiaojuan Huang, Lin Han, Wanqing Wu, and Gehui Wang
Atmos. Chem. Phys., 24, 2803–2820, https://doi.org/10.5194/acp-24-2803-2024, https://doi.org/10.5194/acp-24-2803-2024, 2024
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Typical haze events in Chengdu at the beginning of 2023 were investigated with bulk-chemical and single-particle analyses along with numerical model simulations. By integrating the obtained chemical composition, source, mixing state and numerical simulation results, we infer that Haze-1 was mainly caused by pollutants related to fossil fuel combustion, especially local mobile sources, while Haze-2 was triggered by the secondary pollutants, which mainly came from regional transmission.
Elena Barbaro, Matteo Feltracco, Fabrizio De Blasi, Clara Turetta, Marta Radaelli, Warren Cairns, Giulio Cozzi, Giovanna Mazzi, Marco Casula, Jacopo Gabrieli, Carlo Barbante, and Andrea Gambaro
Atmos. Chem. Phys., 24, 2821–2835, https://doi.org/10.5194/acp-24-2821-2024, https://doi.org/10.5194/acp-24-2821-2024, 2024
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The study analyzed a year of atmospheric aerosol composition at Col Margherita in the Italian Alps. Over 100 chemical markers were identified, including major ions, organic compounds, and trace elements. It revealed sources of aerosol, highlighted impacts of Saharan dust events, and showed anthropogenic pollution's influence despite the site's remoteness. Enrichment factors emphasized non-natural sources of trace elements. Source apportionment identified four key factors affecting the area.
Karl Espen Yttri, Are Bäcklund, Franz Conen, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Anne Kasper-Giebl, Avram Gold, Hans Gundersen, Cathrine Lund Myhre, Stephen Matthew Platt, David Simpson, Jason D. Surratt, Sönke Szidat, Martin Rauber, Kjetil Tørseth, Martin Album Ytre-Eide, Zhenfa Zhang, and Wenche Aas
Atmos. Chem. Phys., 24, 2731–2758, https://doi.org/10.5194/acp-24-2731-2024, https://doi.org/10.5194/acp-24-2731-2024, 2024
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We discuss carbonaceous aerosol (CA) observed at the high Arctic Zeppelin Observatory (2017 to 2020). We find that organic aerosol is a significant fraction of the Arctic aerosol, though less than sea salt aerosol and mineral dust, as well as non-sea-salt sulfate, originating mainly from anthropogenic sources in winter and from natural sources in summer, emphasizing the importance of wildfires for biogenic secondary organic aerosol and primary biological aerosol particles observed in the Arctic.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Kira Zeider, Grace Betito, Anthony Bucholtz, Peng Xian, Annette Walker, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2024-392, https://doi.org/10.5194/egusphere-2024-392, 2024
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The predominant wind direction along the California coast (northerly) reverses several times during the summer (to southerly). The effects of these wind reversals on aerosol and cloud characteristics are not well understood. Using data from multiple datasets we found that southerly flow periods had enhanced signatures of anthropogenic emissions due to shipping/continental sources, and clouds had more but smaller droplets.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
EGUsphere, https://doi.org/10.5194/egusphere-2023-2823, https://doi.org/10.5194/egusphere-2023-2823, 2024
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Black carbon (BC) concentration was measured from 211 ship exhaust gas plumes at a remote marine station. Emission factors of BC were calculated in grams/kilograms fuel. Ships using exhaust gas cleaning systems (EGCS) were found to emit 80 % less BC than ships without EGCS. Emission factors were used to model BC emissions as a function of speed to define the effect of speed reduction. BC emissions increased with a decrease in speed from the ship’s service speed.
Kaori Kawana, Fumikazu Taketani, Kazuhiko Matsumoto, Yutaka Tobo, Yoko Iwamoto, Takuma Miyakawa, Akinori Ito, and Yugo Kanaya
Atmos. Chem. Phys., 24, 1777–1799, https://doi.org/10.5194/acp-24-1777-2024, https://doi.org/10.5194/acp-24-1777-2024, 2024
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Based on comprehensive shipborne observations, we found strong links between sea-surface biological materials and the formation of atmospheric fluorescent bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the Arctic Ocean and Bering Sea during autumn 2019. Taking the wind-speed effect into account, we propose equations to approximate the links for this cruise, which can be used as a guide for modeling as well as for systematic comparisons with other observations.
Chen He, Hanxiong Che, Zier Bao, Yiliang Liu, Qing Li, Miao Hu, Jiawei Zhou, Shumin Zhang, Xiaojiang Yao, Quan Shi, Chunmao Chen, Yan Han, Lingshuo Meng, Xin Long, Fumo Yang, and Yang Chen
Atmos. Chem. Phys., 24, 1627–1639, https://doi.org/10.5194/acp-24-1627-2024, https://doi.org/10.5194/acp-24-1627-2024, 2024
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We examined the daily evolution of high molecular-weight organic compounds with a molecular weight of up to 1000 Da in order to comprehend their behaviors in the atmosphere under actual conditions. These compounds were proven to undergo multi-generation oxidation, carboxylation, and nitrification via both day- and nighttime chemistry.
Karine Desboeufs, Paola Formenti, Raquel Torres-Sánchez, Kerstin Schepanski, Jean-Pierre Chaboureau, Hendrik Andersen, Jan Cermak, Stefanie Feuerstein, Benoit Laurent, Danitza Klopper, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Mirande-Bret, Sylvain Triquet, and Stuart J. Piketh
Atmos. Chem. Phys., 24, 1525–1541, https://doi.org/10.5194/acp-24-1525-2024, https://doi.org/10.5194/acp-24-1525-2024, 2024
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This study investigates the fractional solubility of iron (Fe) in dust particles along the coast of Namibia, a critical region for the atmospheric Fe supply of the South Atlantic Ocean. Our results suggest a possible two-way interplay whereby marine biogenic emissions from the coastal marine ecosystems into the atmosphere would increase the solubility of Fe-bearing dust by photo-reduction processes. The subsequent deposition of soluble Fe could act to further enhance marine biogenic emissions.
Sunhye Kim, Jo Machesky, Drew R. Gentner, and Albert A. Presto
Atmos. Chem. Phys., 24, 1281–1298, https://doi.org/10.5194/acp-24-1281-2024, https://doi.org/10.5194/acp-24-1281-2024, 2024
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Cooking emissions are often an overlooked source of air pollution. We used a mobile lab to measure the characteristics of particles emitted from cooking sites in two cities. Our findings showed that cooking releases a substantial number of fine particles. While most emissions were similar, a bakery site showed distinctive chemical compositions with higher nitrogen compound levels. Thus, understanding the particle emissions from different cooking activities is crucial.
Nansi Fakhri, Robin Stevens, Arnold Downey, Konstantina Oikonomou, Jean Sciare, Charbel Afif, and Patrick L. Hayes
Atmos. Chem. Phys., 24, 1193–1212, https://doi.org/10.5194/acp-24-1193-2024, https://doi.org/10.5194/acp-24-1193-2024, 2024
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We investigated the chemical composition of atmospheric fine particles, their emission sources, and the potential human health risk associated with trace elements in particles for an urban site in Montréal over a 3-month period (August–November). This study represents the first time that such extensive composition measurements were included in an urban source apportionment study in Canada, and it provides greater resolution of fine-particle sources than has been previously achieved in Canada.
Hanjin Yoo, Li Wu, Hong Geng, and Chul-Un Ro
Atmos. Chem. Phys., 24, 853–867, https://doi.org/10.5194/acp-24-853-2024, https://doi.org/10.5194/acp-24-853-2024, 2024
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We conducted an investigation of atmospheric aerosols collected in Seoul, South Korea, during the KORUS-AQ campaign on a single-particle basis. We were able to identify their sources, the atmospheric fate, and the impacts of local emissions and long-range transport on aerosol composition. Additionally, we traced potential sources of non-exhaust heavy-metal particles. This comprehensive analysis provides valuable insights into the complex dynamics of urban aerosols.
Eric Schneider, Hendryk Czech, Olga Popovicheva, Marina Chichaeva, Vasily Kobelev, Nikolay Kasimov, Tatiana Minkina, Christopher Paul Rüger, and Ralf Zimmermann
Atmos. Chem. Phys., 24, 553–576, https://doi.org/10.5194/acp-24-553-2024, https://doi.org/10.5194/acp-24-553-2024, 2024
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This study provides insights into the complex chemical composition of long-range-transported wildfire plumes from Yakutia, which underwent different levels of atmospheric processing. With complementary mass spectrometric techniques, we improve our understanding of the chemical processes and atmospheric fate of wildfire plumes. Unprecedented high levels of carbonaceous aerosols crossed the polar circle with implications for the Arctic ecosystem and consequently climate.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yusen Duan, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 475–486, https://doi.org/10.5194/acp-24-475-2024, https://doi.org/10.5194/acp-24-475-2024, 2024
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We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 d during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Jiyuan Yang, Guoyang Lei, Jinfeng Zhu, Yutong Wu, Chang Liu, Kai Hu, Junsong Bao, Zitong Zhang, Weili Lin, and Jun Jin
Atmos. Chem. Phys., 24, 123–136, https://doi.org/10.5194/acp-24-123-2024, https://doi.org/10.5194/acp-24-123-2024, 2024
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The atmospheric pollution and formation mechanisms of particulate-bound alkyl nitrate in Beijing were studied. C9–C16 long-chain n-alkyl nitrates negatively correlated with O3 but positively correlated with PM2.5 and NO2, so they may not be produced during gas-phase homogeneous reactions in the photochemical process but form through reactions between alkanes and nitrates on PM surfaces. Particulate-bound n-alkyl nitrates strongly affect both haze pollution and atmospheric visibility.
Yuanyuan Qin, Xinghua Zhang, Wei Huang, Juanjuan Qin, Xiaoyu Hu, Yuxuan Cao, Tianyi Zhao, Yang Zhang, Jihua Tan, Ziyin Zhang, Xinming Wang, and Zhenzhen Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2703, https://doi.org/10.5194/egusphere-2023-2703, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROS) play an active role in the atmosphere. We quantified the impact of control measures on EPFRs and ROS and found that strict control measures have effectively reduced their emissions, largely linked to a significant decrease in secondary aerosols. Our findings have great implications for further understanding the formation and sources and for developing future air quality management policies targeting EPFRs and ROS.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 15561–15587, https://doi.org/10.5194/acp-23-15561-2023, https://doi.org/10.5194/acp-23-15561-2023, 2023
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Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles, and potentially contribute to the formation of fog and clouds. Here, we present the results of a sea–air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Xing Wei, Yanjie Shen, Xiao-Ying Yu, Yang Gao, Huiwang Gao, Ming Chu, Yujiao Zhu, and Xiaohong Yao
Atmos. Chem. Phys., 23, 15325–15350, https://doi.org/10.5194/acp-23-15325-2023, https://doi.org/10.5194/acp-23-15325-2023, 2023
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We investigate the contribution of grown new particles to Nccn at a rural mountain site in the North China Plain. The total particle number concentrations (Ncn) observed on 8 new particle formation (NPF) days were higher compared to non-NPF days. The Nccn at 0.2 % supersaturation (SS) and 0.4 % SS on the NPF days was significantly lower than on non-NPF days. Only one of eight NPF events had detectable net contributions to Nccn at 0.4 % SS and 1.0 % SS with increased κ values.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
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This study reveals the large day–night differences in brown carbon (BrC) chromophore composition, which was not known previously. The results provide insights into the effects of atmospheric processes and emissions on BrC composition.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
EGUsphere, https://doi.org/10.5194/egusphere-2023-2262, https://doi.org/10.5194/egusphere-2023-2262, 2023
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by Lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve Lidar measurements.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyang Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
EGUsphere, https://doi.org/10.5194/egusphere-2023-2684, https://doi.org/10.5194/egusphere-2023-2684, 2023
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We investigated aerosol composition, sources, and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more-oxidized SOA; however, cloud evaporation leads to the production of less-oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
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Short summary
Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was...
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