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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Atmos. Meas. Tech., 18, 371–403, https://doi.org/10.5194/amt-18-371-2025, https://doi.org/10.5194/amt-18-371-2025, 2025
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Accurate and comparable measurements of oxygenated organic compounds (OVOCs) are crucial in assessing tropospheric ozone burdens and trends. However, the monitoring of many OVOCs remains challenging because of their low atmospheric abundance and lack of stable and traceable calibration standards. This paper describes the calibration standards developed for OVOCs at a low amount of substance fractions (<100 nmol mol-1) to transfer traceability of the International System of Units to the field.
Chiara Giorio, Anne Monod, Valerio Di Marco, Pierre Herckes, Denise Napolitano, Amy Sullivan, Gautier Landrot, Daniel Warnes, Marika Nasti, Sara D'Aronco, Agathe Gérardin, Nicolas Brun, Karine Desboeufs, Sylvain Triquet, Servanne Chevaillier, Claudia Di Biagio, Francesco Battaglia, Frédéric Burnet, Stuart J. Piketh, Andreas Namwoonde, Jean-François Doussin, and Paola Formenti
EGUsphere, https://doi.org/10.5194/egusphere-2024-4140, https://doi.org/10.5194/egusphere-2024-4140, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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A comparison between the solubility of trace metals in pairs of total suspended particulate (TSP) and fog water samples collected in Henties Bay, Namibia, during the AEROCLO-sA field campaign is presented. We found enhanced solubility of metals in fog samples which we attributed to metal-ligand complexes formation in the early stages of particle activation into droplets which can then remain in a kinetically stable form in fog or lead to the formation of colloidal nanoparticles.
Judith Tettenborn, Daniel Zavala-Araiza, Daan Stroeken, Hossein Maazallahi, Carina van der Veen, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Felix Vogel, Lawson Gillespie, Sebastien Ars, James France, David Lowry, Rebecca Fisher, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3620, https://doi.org/10.5194/egusphere-2024-3620, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Measurements of methane with vehicle-based sensors are an effective method to identify and quantify leaks from urban gas distribution systems. We deliberately released methane in different environments, and calibrated the response of different methane analyzers when they transect the plumes in a vehicle. We derived an improved statistical function for consistent emission estimations using different instruments. Repeated transects reduce the uncertainty in emission rate estimates.
Farhan R. Nursanto, Douglas A. Day, Roy Meinen, Rupert Holzinger, Harald Saathoff, Jinglan Fu, Jan Mulder, Ulrike Dusek, and Juliane L. Fry
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-191, https://doi.org/10.5194/amt-2024-191, 2025
Preprint under review for AMT
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It is of increasing importance to monitor nitrate pollution that can harm ecosystems. However, commonly used aerosol monitoring equipment cannot distinguish inorganic from organic forms of nitrate, which may have different consequences for the environment. We describe a method to differentiate types of nitrates that can be applied to ambient monitoring to improve understanding of its formation and impact.
Gerrit Kuhlmann, Foteini Stavropoulou, Stefan Schwietzke, Daniel Zavala-Araiza, Andrew Thorpe, Andreas Hueni, Lukas Emmenegger, Andreea Calcan, Thomas Röckmann, and Dominik Brunner
EGUsphere, https://doi.org/10.5194/egusphere-2024-3494, https://doi.org/10.5194/egusphere-2024-3494, 2024
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A measurement campaign in 2019 found that methane emissions from oil and gas in Romania were significantly higher than reported. In 2021, our follow-up campaign using airborne remote sensing showed a marked decreases in emissions by 20–60 % due to improved infrastructure. The study highlights the importance of measurement-based emission monitoring and illustrates the value of a multi-scale assessment integrating ground-based observations with large-scale airborne remote sensing campaigns.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3231, https://doi.org/10.5194/egusphere-2024-3231, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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This study presents high-precision measurements of ∆′17O(CO2). Key findings include the extension of the N2O-∆′17O correlation to the upper troposphere and the identification of significant differences in the N2O-∆′17O slope in StratoClim samples. Additionally, the ∆′17O measurements are used to estimate global stratospheric production and surface removal of ∆′17O, providing an independent estimate of global vegetation CO2 exchange.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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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.
Hossein Maazallahi, Foteini Stavropoulou, Samuel Jonson Sutanto, Michael Steiner, Dominik Brunner, Mariano Mertens, Patrick Jöckel, Antoon Visschedijk, Hugo Denier van der Gon, Stijn Dellaert, Nataly Velandia Salinas, Stefan Schwietzke, Daniel Zavala-Araiza, Sorin Ghemulet, Alexandru Pana, Magdalena Ardelean, Marius Corbu, Andreea Calcan, Stephen A. Conley, Mackenzie L. Smith, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2135, https://doi.org/10.5194/egusphere-2024-2135, 2024
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This article provide insights from airborne in-situ measurements during the ROMEO campaign with support from two model simulations. The results from the evaluations performed for this article are independently consistent with the results from previously published article which was based on ground-based measurements during the ROMEO campaign. The results show that reported methane emissions from oil and gas industry in Romania are largely under-reported to UNFCCC in 2019.
Hella van Asperen, Thorsten Warneke, Alessandro Carioca de Araújo, Bruce Forsberg, Sávio José Filgueiras Ferreira, Thomas Röckmann, Carina van der Veen, Sipko Bulthuis, Leonardo Ramos de Oliveira, Thiago de Lima Xavier, Jailson da Mata, Marta de Oliveira Sá, Paulo Ricardo Teixeira, Julie Andrews de França e Silva, Susan Trumbore, and Justus Notholt
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.
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)
Multiple eco-regions contribute to the seasonal cycle of Antarctic aerosol size distributions
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Long-range transport of air pollutants increases the concentration of hazardous components of PM2.5 in northern South America
Dominant influence of biomass combustion and cross-border transport on nitrogen-containing organic compound levels in the southeastern Tibetan Plateau
The Critical Role of Aqueous-Phase Processes in Aromatic-Derived Nitrogen-Containing Organic Aerosol Formation in Cities with Different Energy Consumption Patterns
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Online characterization of primary and secondary emissions of particulate matter and acidic molecules from a modern fleet of city buses
Atmospheric evolution of environmentally persistent free radicals in the rural North China Plain: effects on water solubility and PM2.5 oxidative potential
Two distinct ship emission profiles for organic-sulfate source apportionment of PM in sulfur emission control areas
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Measurement report: Occurrence of aminiums in PM2.5 during winter in China – aminium outbreak during polluted episodes and potential constraints
Bridging gas and aerosol properties between the northeastern US and Bermuda: analysis of eight transit flights
The behaviour of charged particles (ions) during new particle formation events in urban Leipzig, Germany
Sensitivity of aerosol and cloud properties to coupling strength of marine boundary layer clouds over the northwest Atlantic
Exploring the sources of light-absorbing carbonaceous aerosols by integrating observational and modeling results: insights from Northeast China
Characterization of atmospheric water-soluble brown carbon in the Athabasca Oil Sands Region, Canada
Measurement report: Characteristics of airborne black-carbon-containing particles during the 2021 summer COVID-19 lockdown in a typical Yangtze River Delta city, China
Aerosol optical properties within the atmospheric boundary layer predicted from ground-based observations compared to Raman lidar retrievals during RITA-2021
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Measurement report: Formation of tropospheric brown carbon in a lifting air mass
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Differences in aerosol and cloud properties along the central California coast when winds change from northerly to southerly
International airport emissions and their impact on local air quality: chemical speciation of ambient aerosols at Madrid–Barajas Airport during the AVIATOR campaign
The local ship speed reduction effect on black carbon emissions measured at a remote marine station
High-altitude aerosol chemical characterization and source identification: insights from the CALISHTO campaign
Measurement report: Impact of emission control measures on environmental persistent free radicals and reactive oxygen species – a short-term case study in Beijing
Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique
Measurement report: Impact of cloud processes on secondary organic aerosols at a forested mountain site in southeastern China
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Measurement report: Vanadium-containing ship exhaust particles detected in and above the marine boundary layer in the remote atmosphere
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
Measurement report: Sources and meteorology influencing highly-time resolved PM2.5 trace elements at 3 urban sites in extremely polluted Indo Gangetic Plain in India
Diverse sources and aging change the mixing state and ice nucleation properties of aerosol particles over the western Pacific and Southern Ocean
James Brean, David C. S. Beddows, Eija Asmi, Aki Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Rolf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall'Osto
Atmos. Chem. Phys., 25, 1145–1162, https://doi.org/10.5194/acp-25-1145-2025, https://doi.org/10.5194/acp-25-1145-2025, 2025
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Our results emphasise how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Adam E. Thomas, Hayley S. Glicker, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 25, 959–977, https://doi.org/10.5194/acp-25-959-2025, https://doi.org/10.5194/acp-25-959-2025, 2025
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We present measurements of the organic composition of ultrafine particles collected from the eastern Amazon, an understudied region that is subjected to increasing human influence. We find that while isoprene chemistry is likely significant for ultrafine-particle growth throughout the year, compounds related to other sources, such as biological-spore emissions and biomass burning, exhibit striking seasonal differences, implying extensive variation in regional ultrafine-particle sources.
Kumiko Goto-Azuma, Yoshimi Ogawa-Tsukagawa, Kaori Fukuda, Koji Fujita, Motohiro Hirabayashi, Remi Dallmayr, Jun Ogata, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Sumito Matoba, Moe Kadota, Akane Tsushima, Naoko Nagatsuka, and Teruo Aoki
Atmos. Chem. Phys., 25, 657–683, https://doi.org/10.5194/acp-25-657-2025, https://doi.org/10.5194/acp-25-657-2025, 2025
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Monthly ice core records spanning 350 years from Greenland show trends in refractory black carbon (rBC) concentrations and sizes. rBC levels have increased since the 1870s due to the inflow of anthropogenic rBC, with larger diameters than those from biomass burning (BB) rBC. High summer BB rBC peaks may reduce the ice sheet albedo, but BB rBC showed no increase until the early 2000s. These results are vital for validating aerosol and climate models.
Mingjie Kang, Mengying Bao, Wenhuai Song, Aduburexiati Abulimiti, Changliu Wu, Fang Cao, Sönke Szidat, and Yanlin Zhang
Atmos. Chem. Phys., 25, 73–91, https://doi.org/10.5194/acp-25-73-2025, https://doi.org/10.5194/acp-25-73-2025, 2025
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Reports on molecular-level knowledge of high-temporal-resolution particulate matter ≤2.5 µm in diameter (PM2.5) on hazy days are limited. We investigated various PM2.5 species and their sources. The results show biomass burning (BB) was the main source of organic carbon. Moreover, BB enhanced fungal spore emissions and secondary aerosol formation. The contribution of non-fossil sources increased with increasing haze pollution, suggesting BB may be an important driver of haze events in winter.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Andreas Aktypis, Dontavious J. Sippial, Christina N. Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 13769–13791, https://doi.org/10.5194/acp-24-13769-2024, https://doi.org/10.5194/acp-24-13769-2024, 2024
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A dual-chamber system was deployed in two different environments (Po Valley, Italy, and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary organic aerosol (SOA). In the Po Valley, the system reacts rapidly, forming large amounts of SOA, while in Pertouli the SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Ting Yang, Yu Xu, Yu-Chen Wang, Yi-Jia Ma, Hong-Wei Xiao, Hao Xiao, and Hua-Yun Xiao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3823, https://doi.org/10.5194/egusphere-2024-3823, 2024
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Previous measurement-model comparisons of atmospheric isoprene levels showed a significant unidentified source of isoprene in some northern Chinese cities during winter. Here, the first combination of large-scale observations and field combustion experiments provides novel insights into biomass burning emissions as a significant source of isoprene-derived organosulfates during winter in northern cities, China.
Jie Zhang, Tianyu Zhu, Alexandra Catena, Yaowei Li, Margaret J. Schwab, Pengfei Liu, Akua Asa-Awuku, and James Schwab
Atmos. Chem. Phys., 24, 13445–13456, https://doi.org/10.5194/acp-24-13445-2024, https://doi.org/10.5194/acp-24-13445-2024, 2024
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This study shows the derived organic aerosol hygroscopicity under high-humidity conditions based on a simple optical scatter monitor system, including two nephelometric monitors (pDR-1500), when the aerosol chemical composition is already known.
Wei Yuan, Ru-Jin Huang, Chao Luo, Lu Yang, Wenjuan Cao, Jie Guo, and Huinan Yang
Atmos. Chem. Phys., 24, 13219–13230, https://doi.org/10.5194/acp-24-13219-2024, https://doi.org/10.5194/acp-24-13219-2024, 2024
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We characterized water-soluble oxidative potential (OP) levels in wintertime PM2.5 in the south and north of Beijing. Our results show that the volume-normalized dithiothreitol (DTTv) in the north was comparable to that in the south, while the mass-normalized dithiothreitol (DTTm) in the north was almost twice that in the south. Traffic-related emissions and biomass burning were the main sources of DTTv in the south, and traffic-related emissions contributed the most to DTTv in the north.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baoling Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
Atmos. Chem. Phys., 24, 13065–13079, https://doi.org/10.5194/acp-24-13065-2024, https://doi.org/10.5194/acp-24-13065-2024, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas–particle partitioning when the site was affected by urban plumes. A box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
Yingjie Shen, Rudra P. Pokhrel, Amy P. Sullivan, Ezra J. T. Levin, Lauren A. Garofalo, Delphine K. Farmer, Wade Permar, Lu Hu, Darin W. Toohey, Teresa Campos, Emily V. Fischer, and Shane M. Murphy
Atmos. Chem. Phys., 24, 12881–12901, https://doi.org/10.5194/acp-24-12881-2024, https://doi.org/10.5194/acp-24-12881-2024, 2024
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The magnitude and evolution of brown carbon (BrC) absorption remain unclear, with uncertainty in climate models. Data from the WE-CAN airborne experiment show that model parameterizations overestimate the mass absorption cross section (MAC) of BrC. Observed decreases in BrC absorption with chemical markers are due to decreasing organic aerosol (OA) mass rather than a decreasing BrC MAC, which is currently implemented in models. Water-soluble BrC contributes 23 % of total absorption at 660 nm.
Qun He, Zhaowen Wang, Houfeng Liu, Pengju Xu, Rongbao Duan, Caihong Xu, Jianmin Chen, and Min Wei
Atmos. Chem. Phys., 24, 12775–12792, https://doi.org/10.5194/acp-24-12775-2024, https://doi.org/10.5194/acp-24-12775-2024, 2024
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Coastal environments provide an ideal setting for investigating the intermixing of terrestrial and marine aerosols. Terrestrial air mass constituted a larger number of microbes from anthropogenic and soil emissions, whereas saprophytic and gut microbes were predominant in marine samples. Mixed air masses indicated a fusion of marine and terrestrial aerosols, characterized by alterations in the ratio of pathogenic and saprophytic microbes when compared to either terrestrial or marine samples.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O'Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
Atmos. Chem. Phys., 24, 12749–12773, https://doi.org/10.5194/acp-24-12749-2024, https://doi.org/10.5194/acp-24-12749-2024, 2024
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Prescribed burning is an important method for managing ecosystems and preventing wildfires. However, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in 2 different years, we characterize emissions and evolutions of up to 8 h of PM2.5 mass, black carbon (BC), and brown carbon (BrC) in smoke from burning of forested lands in the southeastern USA.
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
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We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
Fan Mei, Qi Zhang, Damao Zhang, Jerome Fast, Gourihar Kulkarni, Mikhail Pekour, Christopher Niedek, Susanne Glienke, Isarel Silber, Beat Schmid, Jason Tomlinson, Hardeep Mehta, Xena Mansoura, Zezhen Cheng, Gregory Vandergrift, Nurun Nahar Lata, Swarup China, and Zihua Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2024-3089, https://doi.org/10.5194/egusphere-2024-3089, 2024
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This study highlights the unique capability of the ArcticShark UAS in measuring vertically resolved atmospheric properties over the Southern Great Plains. Data from 32 research flights in 2023 reveal seasonal patterns and correlations with conventional measurements. The consistency and complementarity of in situ and remote sensing methods are highlighted. The study demonstrates the ArcticShark’s versatility in bridging data gaps and improving the understanding of vertical atmospheric structures.
Imad El Haddad, Danielle Vienneau, Kaspar R. Daellenbach, Robin Modini, Jay G. Slowik, Abhishek Upadhyay, Petros N. Vasilakos, David Bell, Kees de Hoogh, and Andre S. H. Prevot
Atmos. Chem. Phys., 24, 11981–12011, https://doi.org/10.5194/acp-24-11981-2024, https://doi.org/10.5194/acp-24-11981-2024, 2024
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing on the most harmful anthropogenic emissions. We highlight key observations, modelling developments, and emission measurements needed to achieve this shift.
Pramod Kumar, Khushboo Sharma, Ankita Malu, Rajeev Rajak, Aparna Gupta, Bidyutjyoti Baruah, Shailesh Yadav, Thupstan Angchuk, Jayant Sharma, Rakesh Kumar Ranjan, Anil Kumar Misra, and Nishchal Wanjari
Atmos. Chem. Phys., 24, 11585–11601, https://doi.org/10.5194/acp-24-11585-2024, https://doi.org/10.5194/acp-24-11585-2024, 2024
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This work monitors and assesses air pollution, especially black and brown carbon, its controlling factor, and its effect on the environment of Sikkim Himalayan region. The huge urban sprawl in recent decades has led to regional human-induced air pollution in the region. Black carbon was highest in April 2021 and March 2022, exceeding the WHO limit. The monsoon season causes huge rainfall over the region, which reduces the pollutants by scavenging (rainout and washout).
Maria P. Velásquez-García, K. Santiago Hernández, James A. Vergara-Correa, Richard J. Pope, Miriam Gómez-Marín, and Angela M. Rendón
Atmos. Chem. Phys., 24, 11497–11520, https://doi.org/10.5194/acp-24-11497-2024, https://doi.org/10.5194/acp-24-11497-2024, 2024
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In the Aburrá Valley, northern South America, local emissions determine air quality conditions. However, we found that external sources, such as regional fires, Saharan dust, and volcanic emissions, increase particulate concentrations and worsen chemical composition by introducing elements like heavy metals. Dry winds and source variability contribute to seasonal influences on these events. This study assesses the air quality risks posed by such events, which can affect broad regions worldwide.
Meng Wang, Qiyuan Wang, Steven Sai Hang Ho, Jie Tian, Yong Zhang, Shun-cheng Lee, and Junji Cao
Atmos. Chem. Phys., 24, 11175–11189, https://doi.org/10.5194/acp-24-11175-2024, https://doi.org/10.5194/acp-24-11175-2024, 2024
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We studied nitrogen-containing organic compounds (NOCs) in particulate matter <2.5 µm particles on the southeastern Tibetan Plateau. We found that biomass burning and transboundary transport are the main sources of NOCs in the high-altitude area. Understanding these aerosol sources informs how they add to regional and potentially global climate changes. Our findings could help shape effective environmental policies to enhance air quality and address climate impacts in this sensitive region.
Yi-Jia Ma, Yu Xu, Ting Yang, Lin Gui, Hong-Wei Xiao, Hao Xiao, and Hua-Yun Xiao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2602, https://doi.org/10.5194/egusphere-2024-2602, 2024
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The abundance, potential precursors, and main formation mechanisms of NOCs in PM2.5 during winter were compared among cities with different energy consumption. We found that the aerosol NOC pollution during winter is closely associated with the intensity of precursor emissions and the efficiency of aqueous-phase processes in converting these emissions into NOCs. The overall results highlight the importance of emission reduction strategies in controlling aerosol NOCs pollution during winter.
Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding
Atmos. Chem. Phys., 24, 11063–11080, https://doi.org/10.5194/acp-24-11063-2024, https://doi.org/10.5194/acp-24-11063-2024, 2024
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In this study, we found large spatial discrepancies in the physical and chemical properties of black carbon over the Tibetan Plateau (TP). Elevated anthropogenic emissions from low-altitude regions can significantly change the mass concentration, mixing state and chemical composition of black-carbon-containing aerosol in the TP region, further altering its light absorption ability. Our study emphasizes the vulnerability of remote plateau regions to intense anthropogenic influences.
Liyuan Zhou, Qianyun Liu, Christian M. Salvador, Michael Le Breton, Mattias Hallquist, Jian Zhen Yu, Chak K. Chan, and Åsa M. Hallquist
Atmos. Chem. Phys., 24, 11045–11061, https://doi.org/10.5194/acp-24-11045-2024, https://doi.org/10.5194/acp-24-11045-2024, 2024
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Our research on city bus emissions reveals that alternative fuels (compressed natural gas and biofuels) reduce fresh particle emissions compared to diesel. However, all fuels lead to secondary air pollution. Aiming at guiding better environmental policies, we studied 76 buses using advanced emission measurement techniques. This work sheds light on the complex effects of bus fuels on urban air quality, emphasizing the need for comprehensive evaluations of future transportation technologies.
Xu Yang, Fobang Liu, Shuqi Yang, Yuling Yang, Yanan Wang, Jingjing Li, Mingyu Zhao, Zhao Wang, Kai Wang, Chi He, and Haijie Tong
Atmos. Chem. Phys., 24, 11029–11043, https://doi.org/10.5194/acp-24-11029-2024, https://doi.org/10.5194/acp-24-11029-2024, 2024
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A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs) in atmospheric particulate matter (PM), with a notable water-soluble fraction likely from atmospheric oxidation during transport. Significant positive correlations between EPFRs and the water-soluble oxidative potential of PM2.5 were found, primarily attributable to the water-soluble fractions of EPFRs. These findings emphasize understanding EPFRs' atmospheric evolution for climate and health impacts.
Kirsten N. Fossum, Chunshui Lin, Niall O'Sullivan, Lu Lei, Stig Hellebust, Darius Ceburnis, Aqeel Afzal, Anja Tremper, David Green, Srishti Jain, Steigvilė Byčenkienė, Colin O'Dowd, John Wenger, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
Xiao He, Xuan Zheng, Shuwen Guo, Lewei Zeng, Ting Chen, Bohan Yang, Shupei Xiao, Qiongqiong Wang, Zhiyuan Li, Yan You, Shaojun Zhang, and Ye Wu
Atmos. Chem. Phys., 24, 10655–10666, https://doi.org/10.5194/acp-24-10655-2024, https://doi.org/10.5194/acp-24-10655-2024, 2024
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This study introduces an innovative method for identifying and quantifying complex organic vapors and aerosols. By combining advanced analytical techniques and new algorithms, we categorized thousands of compounds from heavy-duty diesel vehicles and ambient air and highlighted specific tracers for emission sources. The innovative approach enhances peak identification, reduces quantification uncertainties, and offers new insights for air quality management and atmospheric chemistry.
Emmanuel Chevassus, Kirsten N. Fossum, Darius Ceburnis, Lu Lei, Chunshui Lin, Wei Xu, Colin D. O’ Dowd, and Jurgita Ovadnevaite
EGUsphere, https://doi.org/10.5194/egusphere-2024-2890, https://doi.org/10.5194/egusphere-2024-2890, 2024
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This study presents the first source apportionment of OA at Mace Head via high-resolution mass spectrometry. Introducing transfer entropy as a novel method reveals that aged OA originate from open ocean ozonolysis and local peat burning oxidation. Methanesulphonic acid OA and primary marine OA both mirror phytoplankton activity as observed with their chemical makeup, with MSA-OA closely tied to coccolithophore blooms and PMOA linked to diatoms, chlorophytes, and cyanobacteria.
Yu Xu, Tang Liu, Yi-Jia Ma, Qi-Bin Sun, Hong-Wei Xiao, Hao Xiao, Hua-Yun Xiao, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 10531–10542, https://doi.org/10.5194/acp-24-10531-2024, https://doi.org/10.5194/acp-24-10531-2024, 2024
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This study investigates the characteristics of aminiums and ammonium in PM2.5 on clean and polluted winter days in 11 Chinese cities, highlighting the possibility of the competitive uptake of ammonia versus amines on acidic aerosols or the displacement of aminiums by ammonia under high-ammonia conditions. The overall results deepen the understanding of the spatiotemporal differences in aminium characteristics and formation in China.
Cassidy Soloff, Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Francesca Gallo, Johnathan W. Hair, Miguel Ricardo A. Hilario, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 10385–10408, https://doi.org/10.5194/acp-24-10385-2024, https://doi.org/10.5194/acp-24-10385-2024, 2024
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Using aircraft measurements over the northwestern Atlantic between the US East Coast and Bermuda and trajectory modeling of continental outflow, we identify trace gas and particle properties that exhibit gradients with offshore distance and quantify these changes with high-resolution measurements of concentrations and particle chemistry, size, and scattering properties. This work furthers our understanding of the complex interactions between continental and marine environments.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
Atmos. Chem. Phys., 24, 10349–10361, https://doi.org/10.5194/acp-24-10349-2024, https://doi.org/10.5194/acp-24-10349-2024, 2024
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Ions enhance the formation and growth rates of new particles, affecting the Earth's radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Kira Zeider, Kayla McCauley, Sanja Dmitrovic, Leong Wai Siu, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Simon Kirschler, John B. Nowak, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, Paquita Zuidema, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2024-2743, https://doi.org/10.5194/egusphere-2024-2743, 2024
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In-situ aircraft data collected over the northwest Atlantic Ocean are utilized to compare aerosol conditions and turbulence between near-surface and below cloud base altitudes for different regimes of coupling strength between those two levels, along with how cloud microphysical properties vary across those regimes. Stronger coupling yields more homogenous aerosol structure vertically along with higher cloud drop concentrations and sea salt influence in clouds.
Yuan Cheng, Xu-bing Cao, Sheng-qiang Zhu, Zhi-qing Zhang, Jiu-meng Liu, Hong-liang Zhang, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 24, 9869–9883, https://doi.org/10.5194/acp-24-9869-2024, https://doi.org/10.5194/acp-24-9869-2024, 2024
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The agreement between observational and modeling results is essential for the development of efficient air pollution control strategies. Here we constrained the modeling results of carbonaceous aerosols by field observation in Northeast China, a historically overlooked but recently targeted region of national clean-air actions. Our study suggested that the simulation of agricultural fire emissions and secondary organic aerosols remains challenging.
Dane Blanchard, Mark Gordon, Duc Huy Dang, Paul Andrew Makar, and Julian Aherne
EGUsphere, https://doi.org/10.5194/egusphere-2024-2584, https://doi.org/10.5194/egusphere-2024-2584, 2024
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This study offers the first known evaluation of water-soluble brown carbon aerosols in the Athabasca Oil Sands Region (AOSR), Canada. Fluorescence spectroscopy analysis of aerosol samples from five regional sites (summer 2021) found that oil sands operations were a measurable source of brown carbon. Industrial aerosol emissions may impact atmospheric reaction chemistry and albedo. These findings demonstrate that fluorescence spectroscopy can be applied to monitor brown carbon in the ASOR.
Yuan Dai, Junfeng Wang, Houjun Wang, Shijie Cui, Yunjiang Zhang, Haiwei Li, Yun Wu, Ming Wang, Eleonora Aruffo, and Xinlei Ge
Atmos. Chem. Phys., 24, 9733–9748, https://doi.org/10.5194/acp-24-9733-2024, https://doi.org/10.5194/acp-24-9733-2024, 2024
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Short-term strict emission control can improve air quality, but its effectiveness needs assessment. During the 2021 summer COVID-19 lockdown in Yangzhou, we found that PM2.5 levels did not decrease despite reduced primary emissions. Aged black-carbon particles increased substantially due to higher O3 levels and transported pollutants. High humidity and low wind also played key roles. The results highlight the importance of a regionally balanced control strategy for future air quality management.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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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.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
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We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts 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 relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Can Wu, Xiaodi Liu, Ke Zhang, Si Zhang, Cong Cao, Jianjun Li, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 9263–9275, https://doi.org/10.5194/acp-24-9263-2024, https://doi.org/10.5194/acp-24-9263-2024, 2024
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Brown carbon (BrC) is prevalent in the troposphere and can efficiently absorb solar and terrestrial radiation. Our observations show 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.
Taiwo 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 D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9197–9218, https://doi.org/10.5194/acp-24-9197-2024, https://doi.org/10.5194/acp-24-9197-2024, 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 the vertical dependence of trace gas and aerosol properties.
Guilherme Martins Pereira, Leonardo Yoshiaki Kamigauti, Rubens Fabio Pereira, Djacinto Monteiro dos Santos, Thayná da Silva Santos, José Vinicius Martins, Célia Alves, Cátia Gonçalves, Ismael Casotti Rienda, Nora Kováts, Thiago Nogueira, Luciana Rizzo, Paulo Artaxo, Regina Maura de Miranda, Marcia Akemi Yamasoe, Edmilson Dias de Freitas, Pérola de Castro Vasconcellos, and Maria de Fatima Andrade
EGUsphere, https://doi.org/10.5194/egusphere-2024-2212, https://doi.org/10.5194/egusphere-2024-2212, 2024
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The chemical composition of fine particulate matter was studied in the megacity of São Paulo (Brazil) during a polluted period. Vehicular-related sources were dominant; however, a high contribution of biomass burning was observed and correlated with sample ecotoxicity. Emerging biomass burning sources, such as forest fires and sugarcane bagasse-based power plants, highlight the need for additional control measures alongside stricter rules concerning vehicular emissions.
Kira Zeider, Grace Betito, Anthony Bucholtz, Peng Xian, Annette Walker, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9059–9083, https://doi.org/10.5194/acp-24-9059-2024, https://doi.org/10.5194/acp-24-9059-2024, 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 and continental sources, and clouds had more but smaller droplets.
Saleh Alzahrani, Doğuşhan Kılıç, Michael Flynn, Paul I. Williams, and James Allan
Atmos. Chem. Phys., 24, 9045–9058, https://doi.org/10.5194/acp-24-9045-2024, https://doi.org/10.5194/acp-24-9045-2024, 2024
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This paper investigates emissions from aviation activities at an international airport to evaluate their impact on local air quality. The study provides detailed insights into the chemical composition of aerosols and key pollutants in the airport environment. Source apportionment analysis using positive matrix factorisation (PMF) identified three significant sources: less oxidised oxygenated organic aerosol, alkane organic aerosol, and more oxidised oxygenated organic aerosol.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
Atmos. Chem. Phys., 24, 8927–8941, https://doi.org/10.5194/acp-24-8927-2024, https://doi.org/10.5194/acp-24-8927-2024, 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 per kilogram of fuel. Ships with an exhaust gas cleaning system (EGCS) were found to have median BC emissions per fuel consumed 5 times lower than ships without an EGCS. However, this might be because of non-EGCS ships running at low engine loads rather than the EGCS itself. A local speed restriction would increase BC emissions of ships.
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
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
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
Atmos. Chem. Phys., 24, 8737–8750, https://doi.org/10.5194/acp-24-8737-2024, https://doi.org/10.5194/acp-24-8737-2024, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROSs) play an active role in the atmosphere. Despite control measures having effectively reduced their emissions, reductions were less than in PM2.5. Emission control measures performed well in achieving Parade Blue, but reducing the impact of the atmosphere on human health remains challenging. Thus, there is a need to reassess emission control measures to better address the challenges posed by EPFRs and ROSs.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 24, 8507–8518, https://doi.org/10.5194/acp-24-8507-2024, https://doi.org/10.5194/acp-24-8507-2024, 2024
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The water solubility of secondary organic aerosols (SOAs) 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 SOAs 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.
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, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
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We investigated aerosol composition and 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.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
Atmos. Chem. Phys., 24, 8397–8411, https://doi.org/10.5194/acp-24-8397-2024, https://doi.org/10.5194/acp-24-8397-2024, 2024
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Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance mass spectrometry (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 real samples.
Maya Abou-Ghanem, Daniel M. Murphy, Gregory P. Schill, Michael J. Lawler, and Karl D. Froyd
Atmos. Chem. Phys., 24, 8263–8275, https://doi.org/10.5194/acp-24-8263-2024, https://doi.org/10.5194/acp-24-8263-2024, 2024
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Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
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.
Ashutosh Kumar Shukla, Sachchida Nand Tripathi, Shamitaksha Talukdar, Vishnu Murari, Sreenivas Gaddamidi, Manousos-Ioannis Manousakas, Vipul Lalchandani, Kuldeep Dixit, Vinayak M Ruge, Peeyush Khare, Mayank Kumar, Vikram Singh, Neeraj Rastogi, Suresh Tiwari, Atul K. Srivastava, Dilip Ganguly, Kaspar Rudolf Daellenbach, and Andre Stephan Henry Prevot
EGUsphere, https://doi.org/10.5194/egusphere-2024-1385, https://doi.org/10.5194/egusphere-2024-1385, 2024
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Our study delves into the elemental composition of aerosols across the Indo-Gangetic Plain (IGP), revealing distinct patterns during pollution episodes. We found significant increases in Cl-rich and SFC1 sources, indicating dynamic emissions and agricultural burning impacts. Surges in Cl-rich particles during cold periods highlight their role in particle growth under specific conditions.
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.
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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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