Articles | Volume 17, issue 12
https://doi.org/10.5194/acp-17-7345-2017
© Author(s) 2017. 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-17-7345-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
20 Jun 2017
Research article |
| 20 Jun 2017
Global-scale combustion sources of organic aerosols: sensitivity to formation and removal mechanisms
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz, Germany
Vlassis A. Karydis
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz, Germany
Spyros N. Pandis
Department of Chemical Engineering, University of Patras, Patras,
Greece
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, PA, USA
Jos Lelieveld
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz, Germany
Energy, Environment and Water Research Center, Cyprus Institute,
Nicosia, Cyprus
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Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Huisheng Bian, Mian Chin, Didier A. Hauglustaine, Michael Schulz, Gunnar Myhre, Susanne E. Bauer, Marianne T. Lund, Vlassis A. Karydis, Tom L. Kucsera, Xiaohua Pan, Andrea Pozzer, Ragnhild B. Skeie, Stephen D. Steenrod, Kengo Sudo, Kostas Tsigaridis, Alexandra P. Tsimpidi, and Svetlana G. Tsyro
Atmos. Chem. Phys., 17, 12911–12940, https://doi.org/10.5194/acp-17-12911-2017, https://doi.org/10.5194/acp-17-12911-2017, 2017
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Atmospheric nitrate contributes notably to total aerosol mass in the present day and is likely to be more important over the next century, with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This paper investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
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A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
Xurong Wang, Alexandra P. Tsimpidi, Zhenqi Luo, Benedikt Steil, Andrea Pozzer, Jos Lelieveld, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2025-527, https://doi.org/10.5194/egusphere-2025-527, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Ammonia (NH3) is an abundant alkaline gas and key precursor in particulate matter formation. While SO2 and NOx emissions have decreased, global NH3 emissions are stable or rising. This study investigates NH3 emission impacts on size-resolved aerosol composition and acidity using the EMAC model, analyzing three emission schemes. Sulphate-nitrate-ammonium aerosols in fine mode sizes are most sensitive to NH3 changes. Regional responses vary. NH3 buffers aerosol acidity, mitigating pH shifts.
David Patoulias, Kalliopi Florou, and Spyros N. Pandis
Geosci. Model Dev., 18, 1103–1118, https://doi.org/10.5194/gmd-18-1103-2025, https://doi.org/10.5194/gmd-18-1103-2025, 2025
Short summary
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The effect of the assumed atmospheric nucleation mechanism on particle number concentrations and size distribution was investigated. Two quite different mechanisms involving sulfuric acid and ammonia or a biogenic organic vapor gave quite similar results which were consistent with measurements at 26 measurement stations across Europe. The number of larger particles that serve as cloud condensation nuclei showed little sensitivity to the assumed nucleation mechanism.
Mingxuan Wu, Hailong Wang, Zheng Lu, Xiaohong Liu, Huisheng Bian, David Cohen, Yan Feng, Mian Chin, Didier A. Hauglustaine, Vlassis A. Karydis, Marianne T. Lund, Gunnar Myhre, Andrea Pozzer, Michael Schulz, Ragnhild B. Skeie, Alexandra P. Tsimpidi, Svetlana G. Tsyro, and Shaocheng Xie
EGUsphere, https://doi.org/10.5194/egusphere-2025-235, https://doi.org/10.5194/egusphere-2025-235, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
A key challenge in simulating the lifecycle of nitrate aerosol in global climate models is to accurately represent mass size distribution of nitrate aerosol, which lacks sufficient observational constraints. We found that most climate models underestimate the mass fraction of fine-mode nitrate at surface in all regions. Our study highlights the importance of gas-aerosol partitioning parameterization and simulation of dust and sea salt in correctly simulating mass size distribution of nitrate.
Alexandros Milousis, Susanne M. C. Scholz, Hendrik Fuchs, Alexandra P. Tsimpidi, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2025-313, https://doi.org/10.5194/egusphere-2025-313, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Nitrate aerosol has become a dominant atmospheric component, surpassing sulfate in aerosol composition. However, its simulation remains challenging due to complex formation processes and regional variability. We use the EMAC model to assess key factors in nitrate aerosol predictions. Increasing grid resolution, reducing N2O5 hydrolysis uptake, and refined emissions improve PM2.5 predictions, but PM1 remains underestimated. Seasonal & diurnal discrepancies persist, requiring further refinements.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
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.
Laura Wüst, Patrick Dewald, Gunther N. T. E. Türk, Jos Lelieveld, and John N. Crowley
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Detection of NO2 via cavity ring-down spectroscopy (CRDS) after thermal dissociation (TD) of alkyl and peroxy nitrates can be used to detect total atmospheric organic nitrates originating from the interaction between biogenic emissions of volatile organic compounds and nitrogen oxides of anthropogenic origin. Here we present an improved TD-CRDS which avoids systematic bias resulting from secondary chemistry in the heated inlets and which can be deployed in regions with strong biogenic emissions.
Alexandra P. Tsimpidi, Susanne M. C. Scholz, Alexandros Milousis, Nikolaos Mihalopoulos, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3590, https://doi.org/10.5194/egusphere-2024-3590, 2024
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This study examines global changes in air pollution from 2000 to 2020, focusing on fine aerosols that impact climate and health. Using models and global data, it finds organic aerosols dominate in many regions, especially with wildfires or natural emissions. Pollution from sulfate and nitrate has decreased in Europe and North America due to regulations, while trends in Asia are more complex. The findings improve understanding and support policies for cleaner air and healthier environments.
Simone T. Andersen, Rolf Sander, Patrick Dewald, Laura Wüst, Tobias Seubert, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Chaoyang Xue, Abdelwahid Mellouki, Alexandre Kukui, Vincent Michoud, Manuela Cirtog, Mathieu Cazaunau, Astrid Bauville, Hichem Bouzidi, Paola Formenti, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Christopher Cantrell, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-3437, https://doi.org/10.5194/egusphere-2024-3437, 2024
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Measurements and modelling of reactive nitrogen gases observed in a suburban temperate forest in Rambouillet, France circa 50 km southwest of Paris in 2022 indicate that the biosphere rapidly scavenges organic nitrates of mixed biogenic and anthropogenic origin, resulting in short lifetimes for e.g. alkyl nitrates and peroxy nitrates.
Konstantinos Mataras, Evangelia Siouti, David Patoulias, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3357, https://doi.org/10.5194/egusphere-2024-3357, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Predicted levels of ultrafine particle mass (PM0.1) vary substantially over Europe with higher values in the summer than in the winter. In summer, PM0.1 was mostly comprised of sulfate (38 %) and secondary organics (32 %). During winter the sulfate fraction increased to 47 % and primary organics contributed 23 %. Correlations between PM0.1 and the regulated PM2.5 were low. This suggests that there are significant differences between the dominant sources and processes of PM0.1 and PM2.5.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
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Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allows for novel model constraints and remote sensing products.
Pantelis Georgiades, Theo Economou, Yiannis Proestos, Jose Araya, Jos Lelieveld, and Marco Neira
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-344, https://doi.org/10.5194/essd-2024-344, 2024
Revised manuscript accepted for ESSD
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Climate change is posing increasing challenges in the dairy cattle farming sector, as heat stress adversely affects the animals' health and milk production. To accurately asses these impacts, we developed a machine learning model to downscale daily climate data to hourly Temperature Humidity Index (THI) values. We utilised historical weather data to train our model and applied it to future climate projections, under two climate scenarios.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
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.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon.
Pantelis Georgiades, Matthias Kohl, Mihalis A. Nicolaou, Theodoros Christoudias, Andrea Pozzer, Constantine Dovrolis, and Jos Lelieveld
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-314, https://doi.org/10.5194/essd-2024-314, 2024
Manuscript not accepted for further review
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This study maps global ultrafine particle (UFP) concentrations, pollutants known to affect health, using machine learning. By combining environmental and urban data, we predicted UFP levels at a fine 1 km resolution, highlighting areas of high exposure. Our results provide data for public health policies aimed at reducing air pollution impacts. This research bridges data gaps, offering a valuable tool for understanding and mitigating the health effects of UFP exposure.
Olga Zografou, Christos Kaltsonoudis, Maria Gini, Angeliki Matrali, Elias Panagiotopoulos, Alexandros Lekkas, Dimitris Papanastasiou, Spyros N. Pandis, and Konstantinos Eleftheriadis
EGUsphere, https://doi.org/10.5194/egusphere-2024-2126, https://doi.org/10.5194/egusphere-2024-2126, 2024
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A novel charge transfer ionization orthogonal Time-of-Flight Mass Spectrometer (oToF-MS) was field evaluated for the first time during a field campaign at the suburban DEM station in Athens, Greece from May to August 2023 focusing on key ambient Volatile Organic Compounds (VOCs). The results demonstrate the strengths of the new instrument in performing online, real time measurements of ambient VOCs.
Anna Martin, Veronika Gayler, Benedikt Steil, Klaus Klingmüller, Patrick Jöckel, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 17, 5705–5732, https://doi.org/10.5194/gmd-17-5705-2024, https://doi.org/10.5194/gmd-17-5705-2024, 2024
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The study evaluates the land surface and vegetation model JSBACHv4 as a replacement for the simplified submodel SURFACE in EMAC. JSBACH mitigates earlier problems of soil dryness, which are critical for vegetation modelling. When analysed using different datasets, the coupled model shows strong correlations of key variables, such as land surface temperature, surface albedo and radiation flux. The versatility of the model increases significantly, while the overall performance does not degrade.
Georgia Lazoglou, Theo Economou, Christina Anagnostopoulou, George Zittis, Anna Tzyrkalli, Pantelis Georgiades, and Jos Lelieveld
Geosci. Model Dev., 17, 4689–4703, https://doi.org/10.5194/gmd-17-4689-2024, https://doi.org/10.5194/gmd-17-4689-2024, 2024
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This study focuses on the important issue of the drizzle bias effect in regional climate models, described by an over-prediction of the number of rainy days while underestimating associated precipitation amounts. For this purpose, two distinct methodologies are applied and rigorously evaluated. These results are encouraging for using the multivariate machine learning method random forest to increase the accuracy of climate models concerning the projection of the number of wet days.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Airborne in situ measurements are of great importance to collect valuable data to improve our knowledge of the atmosphere but also present challenges which demand specific designs. This study presents an IR spectrometer for airborne trace-gas measurements with high data efficiency and a simple, compact design. Its in-flight performance is characterized with the help of a test flight and a comparison with another spectrometer. Moreover, results from its first campaign highlight its benefits.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Andreas Aktypis, Christos Kaltsonoudis, David Patoulias, Panayiotis Kalkavouras, Angeliki Matrali, Christina N. Vasilakopoulou, Evangelia Kostenidou, Kalliopi Florou, Nikos Kalivitis, Aikaterini Bougiatioti, Konstantinos Eleftheriadis, Stergios Vratolis, Maria I. Gini, Athanasios Kouras, Constantini Samara, Mihalis Lazaridis, Sofia-Eirini Chatoutsidou, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 65–84, https://doi.org/10.5194/acp-24-65-2024, https://doi.org/10.5194/acp-24-65-2024, 2024
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Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation. The frequency during summer varied from close to zero in southwestern Greece to more than 60 % in the northern, central, and eastern regions. The spatial variability can be explained by the proximity of the sites to coal-fired power plants and agricultural areas.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
Biogeosciences, 20, 4391–4412, https://doi.org/10.5194/bg-20-4391-2023, https://doi.org/10.5194/bg-20-4391-2023, 2023
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We investigated the effect of the El Niño–Southern Oscillation (ENSO) on biogenic volatile organic compound (BVOC) emissions from plants. ENSO events can cause a significant increase in these emissions, which have a long-term impact on the Earth's atmosphere. Persistent ENSO conditions can cause long-term changes in vegetation, resulting in even higher BVOC emissions. We link ENSO-induced emission anomalies with driving atmospheric and vegetational variables.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
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In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Christina N. Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 2837–2850, https://doi.org/10.5194/amt-16-2837-2023, https://doi.org/10.5194/amt-16-2837-2023, 2023
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The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol in areas and periods during which an aerosol mass spectrometer is not available. In this work, an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing the uncertainty of the corresponding source apportionment significantly.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 16, 3013–3028, https://doi.org/10.5194/gmd-16-3013-2023, https://doi.org/10.5194/gmd-16-3013-2023, 2023
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Desert dust has significant impacts on climate, public health, infrastructure and ecosystems. An impact assessment requires numerical predictions, which are challenging because the dust emissions are not well known. We present a novel approach using satellite observations and machine learning to more accurately estimate the emissions and to improve the model simulations.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Spiro D. Jorga, Kalliopi Florou, David Patoulias, and Spyros N. Pandis
Atmos. Chem. Phys., 23, 85–97, https://doi.org/10.5194/acp-23-85-2023, https://doi.org/10.5194/acp-23-85-2023, 2023
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We take advantage of this unexpected low, new particle formation frequency in Greece and use a dual atmospheric simulation chamber system with starting point ambient air in an effort to gain insight about the chemical species that is limiting nucleation in this area. A potential nucleation precursor, ammonia, was added in one of the chambers while the other one was used as a reference. The addition of ammonia assisted new particle formation in almost 50 % of the experiments conducted.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
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The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 15, 6419–6431, https://doi.org/10.5194/amt-15-6419-2022, https://doi.org/10.5194/amt-15-6419-2022, 2022
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Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols when online AMS measurements are not available. In this study, we examine whether and how the low time resolution (usually 24 h) of the offline technique affects source apportionment results. We concluded that use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis.
Stella E. I. Manavi and Spyros N. Pandis
Geosci. Model Dev., 15, 7731–7749, https://doi.org/10.5194/gmd-15-7731-2022, https://doi.org/10.5194/gmd-15-7731-2022, 2022
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The paper describes the first step towards the development of a simulation framework for the chemistry and secondary organic aerosol production of intermediate-volatility organic compounds (IVOCs). These compounds can be a significant source of organic particulate matter. Our approach treats IVOCs as lumped compounds that retain their chemical characteristics. Estimated IVOC emissions from road transport were a factor of 8 higher than emissions used in previous applications.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
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A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys., 22, 1689–1706, https://doi.org/10.5194/acp-22-1689-2022, https://doi.org/10.5194/acp-22-1689-2022, 2022
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Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low-volatility organic compounds have a smaller-than-expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate-volatility organic compounds leads to decreases in the ultrafine-particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
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Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Antonios Tasoglou, Evangelos Louvaris, Kalliopi Florou, Aikaterini Liangou, Eleni Karnezi, Christos Kaltsonoudis, Ningxin Wang, and Spyros N. Pandis
Atmos. Chem. Phys., 20, 11625–11637, https://doi.org/10.5194/acp-20-11625-2020, https://doi.org/10.5194/acp-20-11625-2020, 2020
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A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption. The measured light absorption was two or more times higher than that of fresh black carbon. The absorption enhancement due to the coating of black carbon cores by other aerosol components could explain only part of this absorption enhancement. The rest was due to brown carbon, mostly in the form of extremely low volatility organic compounds.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
Horst Fischer, Raoul Axinte, Heiko Bozem, John N. Crowley, Cheryl Ernest, Stefan Gilge, Sascha Hafermann, Hartwig Harder, Korbinian Hens, Ruud H. H. Janssen, Rainer Königstedt, Dagmar Kubistin, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Christian Plass-Dülmer, Andrea Pozzer, Eric Regelin, Andreas Reiffs, Torsten Schmidt, Jan Schuladen, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11953–11968, https://doi.org/10.5194/acp-19-11953-2019, https://doi.org/10.5194/acp-19-11953-2019, 2019
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We use in situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951, https://doi.org/10.5194/acp-19-11939-2019, https://doi.org/10.5194/acp-19-11939-2019, 2019
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We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
Jianzhong Ma, Christoph Brühl, Qianshan He, Benedikt Steil, Vlassis A. Karydis, Klaus Klingmüller, Holger Tost, Bin Chen, Yufang Jin, Ningwei Liu, Xiangde Xu, Peng Yan, Xiuji Zhou, Kamal Abdelrahman, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11587–11612, https://doi.org/10.5194/acp-19-11587-2019, https://doi.org/10.5194/acp-19-11587-2019, 2019
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We find a pronounced maximum in aerosol extinction in the upper troposphere and lower stratosphere over the Tibetan Plateau during the Asian summer monsoon, caused mainly by mineral dust emitted from the northern Tibetan Plateau and slope area, lofted to and accumulating within the anticyclonic circulation. Mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction around the tropopause within the Asian summer monsoon anticyclone.
Eva Y. Pfannerstill, Nijing Wang, Achim Edtbauer, Efstratios Bourtsoukidis, John N. Crowley, Dirk Dienhart, Philipp G. Eger, Lisa Ernle, Horst Fischer, Bettina Hottmann, Jean-Daniel Paris, Christof Stönner, Ivan Tadic, David Walter, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 19, 11501–11523, https://doi.org/10.5194/acp-19-11501-2019, https://doi.org/10.5194/acp-19-11501-2019, 2019
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The Arabian Peninsula is a global hot spot of ozone pollution. Our measurements, made on a ship in summer 2017, indicate underlying reasons. Despite being at sea, we observed ozone-forming reactive trace gases (measured as so-called total OH reactivity) comparable to highly populated urban regions in amount and composition. This is due to strong emissions from oil extraction and ship traffic. These emissions were quickly converted to ozone due to intense solar irradiation and high temperatures.
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
Christos Kaltsonoudis, Spiro D. Jorga, Evangelos Louvaris, Kalliopi Florou, and Spyros N. Pandis
Atmos. Meas. Tech., 12, 2733–2743, https://doi.org/10.5194/amt-12-2733-2019, https://doi.org/10.5194/amt-12-2733-2019, 2019
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A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers surrounded by UV lamps. The system has been designed to use ambient air as the starting point of the experiments. It can be easily disassembled and transported, enabling the study of various atmospheric environments and it can be used with natural sunlight. The results of test experiments using ambient air are discussed as examples of applications of this system.
Vincent Huijnen, Andrea Pozzer, Joaquim Arteta, Guy Brasseur, Idir Bouarar, Simon Chabrillat, Yves Christophe, Thierno Doumbia, Johannes Flemming, Jonathan Guth, Béatrice Josse, Vlassis A. Karydis, Virginie Marécal, and Sophie Pelletier
Geosci. Model Dev., 12, 1725–1752, https://doi.org/10.5194/gmd-12-1725-2019, https://doi.org/10.5194/gmd-12-1725-2019, 2019
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We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in ECMWF’s Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). This configuration of having various chemistry versions within IFS provides a quantification of uncertainties in CAMS trace gas products that are induced by chemistry modelling.
Katerina S. Karadima, Vlasis G. Mavrantzas, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5571–5587, https://doi.org/10.5194/acp-19-5571-2019, https://doi.org/10.5194/acp-19-5571-2019, 2019
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We explore the morphologies of multicomponent nanoparticles through atomistic molecular dynamics simulations under atmospherically relevant conditions. Phase separation is predicted for almost all simulated nanoparticles either between organics and inorganics or between hydrophobic and hydrophilic constituents. Three main particle types were identified: organic islands at the surface, inorganic core-organic shell morphologies and complex structures with hydrophobic and hydrophilic domains.
Georgia N. Theodoritsi and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5403–5415, https://doi.org/10.5194/acp-19-5403-2019, https://doi.org/10.5194/acp-19-5403-2019, 2019
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The chemical transport model PMCAMx was extended to investigate the effects of partitioning and photochemical aging of biomass burning emissions on organic aerosol (OA) concentrations and was applied in Europe. During the summer, the contribution of biomass burning to total OA levels over continental Europe was 16 % and during winter 47 %. Intermediate volatility organic compounds are predicted to be important precursors of secondary OA from biomass burning.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
Rolf Sander, Andreas Baumgaertner, David Cabrera-Perez, Franziska Frank, Sergey Gromov, Jens-Uwe Grooß, Hartwig Harder, Vincent Huijnen, Patrick Jöckel, Vlassis A. Karydis, Kyle E. Niemeyer, Andrea Pozzer, Hella Riede, Martin G. Schultz, Domenico Taraborrelli, and Sebastian Tauer
Geosci. Model Dev., 12, 1365–1385, https://doi.org/10.5194/gmd-12-1365-2019, https://doi.org/10.5194/gmd-12-1365-2019, 2019
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We present the atmospheric chemistry box model CAABA/MECCA which
now includes a number of new features: skeletal mechanism
reduction, the MOM chemical mechanism for volatile organic
compounds, an option to include reactions from the Master
Chemical Mechanism (MCM) and other chemical mechanisms, updated
isotope tagging, improved and new photolysis modules, and the new
feature of coexisting multiple chemistry mechanisms.
CAABA/MECCA is a community model published under the GPL.
Philipp G. Eger, Frank Helleis, Gerhard Schuster, Gavin J. Phillips, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 12, 1935–1954, https://doi.org/10.5194/amt-12-1935-2019, https://doi.org/10.5194/amt-12-1935-2019, 2019
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We present a chemical ionization quadrupole mass spectrometer (CI-QMS) with a novel discharge ion source. In addition to the expected detection of PAN, peracetic acid and ClNO2, the instrument is also sensitive to SO2, HCl and acetic acid through ion chemistry unique for our ion source. We present ionization schemes along with illustrative datasets from field campaigns underlining the potential of the CI-QMS as an alternative to polonium, especially for application in the marine boundary layer.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Anthoula D. Drosatou, Ksakousti Skyllakou, Georgia N. Theodoritsi, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 973–986, https://doi.org/10.5194/acp-19-973-2019, https://doi.org/10.5194/acp-19-973-2019, 2019
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The ability of positive matrix factorization (PMF) factor analysis to identify and quantify the organic aerosol (OA) sources accurately is tested in this modeling study. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources is less than 40 %, when these sources contribute more than 20 % to the OA. Τhe first oxygenated OA factor includes mainly highly aged OA, while the second oxygenated OA factor contains fresher secondary OA.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
Jonathan M. Liebmann, Jennifer B. A. Muller, Dagmar Kubistin, Anja Claude, Robert Holla, Christian Plass-Dülmer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 12045–12059, https://doi.org/10.5194/acp-18-12045-2018, https://doi.org/10.5194/acp-18-12045-2018, 2018
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We present direct measurements of the summertime total reactivity (inverse lifetime) of NO3 towards organic trace gases at a rural mountain site. High daytime and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during daytime. NO3 radical measurements from one night are presented. For the first time, direct measurements of OH and NO3 reactivity are compared.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Zacharias Marinou Nikolaou, Jyh-Yuan Chen, Yiannis Proestos, Jos Lelieveld, and Rolf Sander
Geosci. Model Dev., 11, 3391–3407, https://doi.org/10.5194/gmd-11-3391-2018, https://doi.org/10.5194/gmd-11-3391-2018, 2018
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Chemistry is an important component of the atmosphere that describes many important physical processes. However, atmospheric chemical mechanisms include hundreds of species and reactions, posing a significant computational load. In this work, we use a powerful reduction method in order to develop a computationally faster chemical mechanism from a detailed mechanism. This enables accelerated simulations, which can be used to examine a wider range of processes in increased detail.
Chinmay Mallik, Laura Tomsche, Efstratios Bourtsoukidis, John N. Crowley, Bettina Derstroff, Horst Fischer, Sascha Hafermann, Imke Hüser, Umar Javed, Stephan Keßel, Jos Lelieveld, Monica Martinez, Hannah Meusel, Anna Novelli, Gavin J. Phillips, Andrea Pozzer, Andreas Reiffs, Rolf Sander, Domenico Taraborrelli, Carina Sauvage, Jan Schuladen, Hang Su, Jonathan Williams, and Hartwig Harder
Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, https://doi.org/10.5194/acp-18-10825-2018, 2018
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OH and HO2 control the transformation of air pollutants and O3 formation. Their implication for air quality over the climatically sensitive Mediterranean region was studied during a field campaign in Cyprus. Production of OH, HO2, and recycled OH was lower in aged marine air masses. Box model simulations of OH and HO2 agreed with measurements except at high terpene concentrations when model RO2 due to terpenes caused large HO2 loss. Autoxidation schemes for RO2 improved the agreement.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
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This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Panos Hadjinicolaou, and Jos Lelieveld
Atmos. Chem. Phys., 18, 1555–1571, https://doi.org/10.5194/acp-18-1555-2018, https://doi.org/10.5194/acp-18-1555-2018, 2018
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We investigate the impact of the choice of gas-phase and aerosol mechanisms, on the simulated summertime concentrations of several pollutants over the eastern Mediterranean, using the WRF-Chem model. The selection of mechanisms significantly affects ozone and fine particulate matter concentrations, and to a lesser extent other gaseous pollutants (NOx, CO). Meteorological components are also affected by the choice of mechanisms due to the interaction of aerosols with radiation.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Kerrigan P. Cain and Spyros N. Pandis
Atmos. Meas. Tech., 10, 4865–4876, https://doi.org/10.5194/amt-10-4865-2017, https://doi.org/10.5194/amt-10-4865-2017, 2017
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Hygroscopicity, oxidation level, and volatility of organic pollutants are three crucial properties that determine their fate in the atmosphere. This study assesses the feasibility of a novel measurement and analysis technique to determine these properties of organic aerosol
components at the same time and to establish their relationship.
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Huisheng Bian, Mian Chin, Didier A. Hauglustaine, Michael Schulz, Gunnar Myhre, Susanne E. Bauer, Marianne T. Lund, Vlassis A. Karydis, Tom L. Kucsera, Xiaohua Pan, Andrea Pozzer, Ragnhild B. Skeie, Stephen D. Steenrod, Kengo Sudo, Kostas Tsigaridis, Alexandra P. Tsimpidi, and Svetlana G. Tsyro
Atmos. Chem. Phys., 17, 12911–12940, https://doi.org/10.5194/acp-17-12911-2017, https://doi.org/10.5194/acp-17-12911-2017, 2017
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Atmospheric nitrate contributes notably to total aerosol mass in the present day and is likely to be more important over the next century, with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This paper investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Evangelos E. Louvaris, Eleni Karnezi, Evangelia Kostenidou, Christos Kaltsonoudis, and Spyros N. Pandis
Atmos. Meas. Tech., 10, 3909–3918, https://doi.org/10.5194/amt-10-3909-2017, https://doi.org/10.5194/amt-10-3909-2017, 2017
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A method for the determination of the organic aerosol volatility distribution combining thermodenuder and isothermal dilution measurements is developed. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol produced during meat charbroiling. Addition of the dilution measurements to the thermodenuder data results in a lower uncertainty of the estimated vaporization enthalpy as well as the semivolatile content of the aerosol.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Christos Kaltsonoudis, Evangelia Kostenidou, Evangelos Louvaris, Magda Psichoudaki, Epameinondas Tsiligiannis, Kalliopi Florou, Aikaterini Liangou, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 7143–7155, https://doi.org/10.5194/acp-17-7143-2017, https://doi.org/10.5194/acp-17-7143-2017, 2017
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Cooking emissions can be a significant source of particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. More than 99% of the aerosol emitted was composed of organic compounds. The fresh particles were similar to the cooking organic aerosol over Greek cities during the winter, while the reacted particles were similar to those found in the atmosphere during the summer.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
Kalliopi Florou, Dimitrios K. Papanastasiou, Michael Pikridas, Christos Kaltsonoudis, Evangelos Louvaris, Georgios I. Gkatzelis, David Patoulias, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 3145–3163, https://doi.org/10.5194/acp-17-3145-2017, https://doi.org/10.5194/acp-17-3145-2017, 2017
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The composition of fine particulate matter (PM) in two major Greek cities (Athens and Patras) was measured during two wintertime campaigns in 2012 and 2013. Residential wood burning has dramatically increased due to the Greek financial crisis, contributing around 50 % of the fine PM on average and more than 80 % during nighttime. Cooking is also an important source during both midday and evening, while transportation dominates only during the morning rush hour.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Andrea Pozzer, Yogesh K. Tiwari, K. Ravi Kumar, and Jos Lelieveld
Atmos. Chem. Phys., 17, 257–275, https://doi.org/10.5194/acp-17-257-2017, https://doi.org/10.5194/acp-17-257-2017, 2017
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This study presents first ship-borne measurements of trace gases over the Bay of Bengal during summer monsoon. The observed variations in trace gases are shown to be due to dynamics/transport and en route photochemistry. Analysis of meteorological and chemical fields shows that significantly lower ozone during rainfall is associated with the downdrafts. A regional model reproduces the observed variations and revealed the rapid transport of ozone across the Bay of Bengal during an event.
Christos Kaltsonoudis, Evangelia Kostenidou, Kalliopi Florou, Magda Psichoudaki, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 14825–14842, https://doi.org/10.5194/acp-16-14825-2016, https://doi.org/10.5194/acp-16-14825-2016, 2016
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Volatile organic compounds (VOCs) were monitored in urban backgrounds sites, in Athens and Patras in Greece. In summer most of the measured VOCs were due to biogenic and traffic emissions. Winter measurements in Athens revealed that biomass burning used for residential heating was the dominant VOC source. The biomass burning VOC emission ratios and emission factors were estimated.
Antigoni Panagiotopoulou, Panagiotis Charalampidis, Christos Fountoukis, Christodoulos Pilinis, and Spyros N. Pandis
Geosci. Model Dev., 9, 4257–4272, https://doi.org/10.5194/gmd-9-4257-2016, https://doi.org/10.5194/gmd-9-4257-2016, 2016
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The ability of chemical transport model PMCAMx to reproduce ground and satellite aerosol optical depth (AOD) measurements over Europe is evaluated. PMCAMx reproduces AOD values over Spain, the UK, central Europe, and Russia with a fractional bias of less than 15 % and a fractional error of less than 30 %. The model overestimates the AOD over northern Europe probably due to an overestimation of organic aerosol and sulfates, and underestimates over the Balkans due to an underestimation of sulfates.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Klaus Klingmüller, Andrea Pozzer, Swen Metzger, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 16, 5063–5073, https://doi.org/10.5194/acp-16-5063-2016, https://doi.org/10.5194/acp-16-5063-2016, 2016
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During the last decade, the Middle East experienced the strongest increase in atmospheric aerosol concentrations worldwide. Based on satellite observations, the present study corroborates this trend and reveals correlations with soil moisture and precipitation in and surrounding the Fertile Crescent. This suggests that the increasing drought conditions in this region have enhanced dust emissions, a tendency which is expected to be intensified by climate change.
N. Sobanski, M. J. Tang, J. Thieser, G. Schuster, D. Pöhler, H. Fischer, W. Song, C. Sauvage, J. Williams, J. Fachinger, F. Berkes, P. Hoor, U. Platt, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 16, 4867–4883, https://doi.org/10.5194/acp-16-4867-2016, https://doi.org/10.5194/acp-16-4867-2016, 2016
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The nitrate radical (NO3) is an important nocturnal oxidant. By measuring NO3, its precursors (nitrogen dioxide and ozone) and several trace gases with which it reacts, we examined the chemical and meteorological factors influencing the lifetime of NO3 at a semi-rural mountain site. Unexpectedly long lifetimes, approaching 1 h, were observed on several nights and were associated with a low-lying residual layer. We discuss the role of other reactions that convert NO2 to NO3.
Christos Fountoukis, Athanasios G. Megaritis, Ksakousti Skyllakou, Panagiotis E. Charalampidis, Hugo A. C. Denier van der Gon, Monica Crippa, André S. H. Prévôt, Friederike Fachinger, Alfred Wiedensohler, Christodoulos Pilinis, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 3727–3741, https://doi.org/10.5194/acp-16-3727-2016, https://doi.org/10.5194/acp-16-3727-2016, 2016
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We use PMCAMx with high grid resolution over Paris to simulate carbonaceous aerosol during the summer and winter MEGAPOLI campaigns. PMCAMx reproduces BC observations well. Addition of cooking organic aerosol emissions of 80 mg per day per capita is needed to reproduce the corresponding observations. While the oxygenated organic aerosol predictions during the summer are encouraging a major wintertime source appears to be missing.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
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We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
J. Thieser, G. Schuster, J. Schuladen, G. J. Phillips, A. Reiffs, U. Parchatka, D. Pöhler, J. Lelieveld, and J. N. Crowley
Atmos. Meas. Tech., 9, 553–576, https://doi.org/10.5194/amt-9-553-2016, https://doi.org/10.5194/amt-9-553-2016, 2016
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We report on the use of thermal dissociation cavity ring-down spectroscopy to detect NO2, peroxy nitrates and alkyl nitrates. We present both laboratory studies that characterise the chemical formation and loss of NO2 in the heated inlets and also result from a first field deployment.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
G. I. Gkatzelis, D. K. Papanastasiou, K. Florou, C. Kaltsonoudis, E. Louvaris, and S. N. Pandis
Atmos. Meas. Tech., 9, 103–114, https://doi.org/10.5194/amt-9-103-2016, https://doi.org/10.5194/amt-9-103-2016, 2016
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A method for the measurement of the nonvolatile atmospheric particle size distribution is developed and tested. The tests include laboratory experiments with biogenic and anthropogenic secondary organic aerosol as well as nucleation experiments with ambient air. The method is then further tested during an ambient campaign.
E. Kostenidou, K. Florou, C. Kaltsonoudis, M. Tsiflikiotou, S. Vratolis, K. Eleftheriadis, and S. N. Pandis
Atmos. Chem. Phys., 15, 11355–11371, https://doi.org/10.5194/acp-15-11355-2015, https://doi.org/10.5194/acp-15-11355-2015, 2015
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The concentration and chemical composition of fine particulate matter were measured during the summer of 2012 in two Greek cities, Patras and Athens. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources. Analysis of the Aerosol Mass Spectrometer data suggested that the contribution of the primary sources to organic aerosol was important (22% in Patras and 35% in Athens) but not dominant.
M. Pikridas, J. Sciare, F. Freutel, S. Crumeyrolle, S.-L. von der Weiden-Reinmüller, A. Borbon, A. Schwarzenboeck, M. Merkel, M. Crippa, E. Kostenidou, M. Psichoudaki, L. Hildebrandt, G. J. Engelhart, T. Petäjä, A. S. H. Prévôt, F. Drewnick, U. Baltensperger, A. Wiedensohler, M. Kulmala, M. Beekmann, and S. N. Pandis
Atmos. Chem. Phys., 15, 10219–10237, https://doi.org/10.5194/acp-15-10219-2015, https://doi.org/10.5194/acp-15-10219-2015, 2015
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Aerosol size distribution measurements from three ground sites, two mobile laboratories, and one airplane are combined to investigate the spatial and temporal variability of ultrafine particles in and around Paris during the summer and winter MEGAPOLI campaigns. The role of nucleation as a particle source and the influence of Paris emissions on their surroundings are examined.
M. Beekmann, A. S. H. Prévôt, F. Drewnick, J. Sciare, S. N. Pandis, H. A. C. Denier van der Gon, M. Crippa, F. Freutel, L. Poulain, V. Ghersi, E. Rodriguez, S. Beirle, P. Zotter, S.-L. von der Weiden-Reinmüller, M. Bressi, C. Fountoukis, H. Petetin, S. Szidat, J. Schneider, A. Rosso, I. El Haddad, A. Megaritis, Q. J. Zhang, V. Michoud, J. G. Slowik, S. Moukhtar, P. Kolmonen, A. Stohl, S. Eckhardt, A. Borbon, V. Gros, N. Marchand, J. L. Jaffrezo, A. Schwarzenboeck, A. Colomb, A. Wiedensohler, S. Borrmann, M. Lawrence, A. Baklanov, and U. Baltensperger
Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, https://doi.org/10.5194/acp-15-9577-2015, 2015
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A detailed characterization of air quality in the Paris (France) agglomeration, a megacity, during two summer and winter intensive campaigns and from additional 1-year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported into the megacity from upwind regions. Unexpectedly, a major part of organic PM is of modern origin (woodburning and cooking activities, secondary formation from biogenic VOC).
M. Abdelkader, S. Metzger, R. E. Mamouri, M. Astitha, L. Barrie, Z. Levin, and J. Lelieveld
Atmos. Chem. Phys., 15, 9173–9189, https://doi.org/10.5194/acp-15-9173-2015, https://doi.org/10.5194/acp-15-9173-2015, 2015
H. G. Ouwersloot, A. Pozzer, B. Steil, H. Tost, and J. Lelieveld
Geosci. Model Dev., 8, 2435–2445, https://doi.org/10.5194/gmd-8-2435-2015, https://doi.org/10.5194/gmd-8-2435-2015, 2015
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
H. Fischer, A. Pozzer, T. Schmitt, P. Jöckel, T. Klippel, D. Taraborrelli, and J. Lelieveld
Atmos. Chem. Phys., 15, 6971–6980, https://doi.org/10.5194/acp-15-6971-2015, https://doi.org/10.5194/acp-15-6971-2015, 2015
D. Patoulias, C. Fountoukis, I. Riipinen, and S. N. Pandis
Atmos. Chem. Phys., 15, 6337–6350, https://doi.org/10.5194/acp-15-6337-2015, https://doi.org/10.5194/acp-15-6337-2015, 2015
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A new aerosol dynamics model (DMANx) describing the organic vapor condensation on nanoparticles based on the volatility basis set framework is used to simulate typical nucleation events in two contrasting environments in Hyytiälä (Finland) and Finokalia (Greece). The role of semivolatile, low, and extremely low volatility organics and the corresponding surface energies is investigated.
I. Riipinen, N. Rastak, and S. N. Pandis
Atmos. Chem. Phys., 15, 6305–6322, https://doi.org/10.5194/acp-15-6305-2015, https://doi.org/10.5194/acp-15-6305-2015, 2015
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Atmospheric organic aerosol is complex and thus a challenge to model. We introduce a theoretical framework (solubility distributions) to represent the solubility of multicomponent mixtures. Using the framework, we evaluate the commonly made assumptions about the cloud condensation nucleus (CCN) activity of organic mixtures. We find that material with water solubilities larger than 0.1-100 g/L can usually be treated as completely soluble, which simplifies the treatment of organic CCN.
A. Tasoglou and S. N. Pandis
Atmos. Chem. Phys., 15, 6035–6046, https://doi.org/10.5194/acp-15-6035-2015, https://doi.org/10.5194/acp-15-6035-2015, 2015
S. Zheng, A. Pozzer, C. X. Cao, and J. Lelieveld
Atmos. Chem. Phys., 15, 5715–5725, https://doi.org/10.5194/acp-15-5715-2015, https://doi.org/10.5194/acp-15-5715-2015, 2015
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The present study uses aerosol optical depth as proxy to estimate 12 years of PM2.5 data for the Beijing central area and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals/year for the period 2001--2012 in the Beijing central area, and the per capita mortality for all ages due to PM2.5 is around 15 per 10,000 person-years for the period 2010--2012.
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
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A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
K. Klingmüller, B. Steil, C. Brühl, H. Tost, and J. Lelieveld
Geosci. Model Dev., 7, 2503–2516, https://doi.org/10.5194/gmd-7-2503-2014, https://doi.org/10.5194/gmd-7-2503-2014, 2014
A. Novelli, K. Hens, C. Tatum Ernest, D. Kubistin, E. Regelin, T. Elste, C. Plass-Dülmer, M. Martinez, J. Lelieveld, and H. Harder
Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, https://doi.org/10.5194/amt-7-3413-2014, 2014
A. G. Megaritis, C. Fountoukis, P. E. Charalampidis, H. A. C. Denier van der Gon, C. Pilinis, and S. N. Pandis
Atmos. Chem. Phys., 14, 10283–10298, https://doi.org/10.5194/acp-14-10283-2014, https://doi.org/10.5194/acp-14-10283-2014, 2014
E. Karnezi, I. Riipinen, and S. N. Pandis
Atmos. Meas. Tech., 7, 2953–2965, https://doi.org/10.5194/amt-7-2953-2014, https://doi.org/10.5194/amt-7-2953-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
H. Bozem, H. Fischer, C. Gurk, C. L. Schiller, U. Parchatka, R. Koenigstedt, A. Stickler, M. Martinez, H. Harder, D. Kubistin, J. Williams, G. Eerdekens, and J. Lelieveld
Atmos. Chem. Phys., 14, 8917–8931, https://doi.org/10.5194/acp-14-8917-2014, https://doi.org/10.5194/acp-14-8917-2014, 2014
D. Y. Chang, H. Tost, B. Steil, and J. Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-21975-2014, https://doi.org/10.5194/acpd-14-21975-2014, 2014
Preprint withdrawn
K. Hens, A. Novelli, M. Martinez, J. Auld, R. Axinte, B. Bohn, H. Fischer, P. Keronen, D. Kubistin, A. C. Nölscher, R. Oswald, P. Paasonen, T. Petäjä, E. Regelin, R. Sander, V. Sinha, M. Sipilä, D. Taraborrelli, C. Tatum Ernest, J. Williams, J. Lelieveld, and H. Harder
Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, https://doi.org/10.5194/acp-14-8723-2014, 2014
A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren
Atmos. Chem. Phys., 14, 7213–7231, https://doi.org/10.5194/acp-14-7213-2014, https://doi.org/10.5194/acp-14-7213-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
B. N. Murphy, N. M. Donahue, A. L. Robinson, and S. N. Pandis
Atmos. Chem. Phys., 14, 5825–5839, https://doi.org/10.5194/acp-14-5825-2014, https://doi.org/10.5194/acp-14-5825-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
T. Christoudias, Y. Proestos, and J. Lelieveld
Atmos. Chem. Phys., 14, 4607–4616, https://doi.org/10.5194/acp-14-4607-2014, https://doi.org/10.5194/acp-14-4607-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
K. Skyllakou, B. N. Murphy, A. G. Megaritis, C. Fountoukis, and S. N. Pandis
Atmos. Chem. Phys., 14, 2343–2352, https://doi.org/10.5194/acp-14-2343-2014, https://doi.org/10.5194/acp-14-2343-2014, 2014
J. A. Adame, M. Martínez, M. Sorribas, P. J. Hidalgo, H. Harder, J.-M. Diesch, F. Drewnick, W. Song, J. Williams, V. Sinha, M. A. Hernández-Ceballos, J. Vilà-Guerau de Arellano, R. Sander, Z. Hosaynali-Beygi, H. Fischer, J. Lelieveld, and B. De la Morena
Atmos. Chem. Phys., 14, 2325–2342, https://doi.org/10.5194/acp-14-2325-2014, https://doi.org/10.5194/acp-14-2325-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Y. F. Elshorbany, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld
Atmos. Chem. Phys., 14, 1167–1184, https://doi.org/10.5194/acp-14-1167-2014, https://doi.org/10.5194/acp-14-1167-2014, 2014
D. Giannadaki, A. Pozzer, and J. Lelieveld
Atmos. Chem. Phys., 14, 957–968, https://doi.org/10.5194/acp-14-957-2014, https://doi.org/10.5194/acp-14-957-2014, 2014
P. Zanis, P. Hadjinicolaou, A. Pozzer, E. Tyrlis, S. Dafka, N. Mihalopoulos, and J. Lelieveld
Atmos. Chem. Phys., 14, 115–132, https://doi.org/10.5194/acp-14-115-2014, https://doi.org/10.5194/acp-14-115-2014, 2014
J. Yoon, A. Pozzer, P. Hoor, D. Y. Chang, S. Beirle, T. Wagner, S. Schloegl, J. Lelieveld, and H. M. Worden
Atmos. Chem. Phys., 13, 11307–11316, https://doi.org/10.5194/acp-13-11307-2013, https://doi.org/10.5194/acp-13-11307-2013, 2013
E. Regelin, H. Harder, M. Martinez, D. Kubistin, C. Tatum Ernest, H. Bozem, T. Klippel, Z. Hosaynali-Beygi, H. Fischer, R. Sander, P. Jöckel, R. Königstedt, and J. Lelieveld
Atmos. Chem. Phys., 13, 10703–10720, https://doi.org/10.5194/acp-13-10703-2013, https://doi.org/10.5194/acp-13-10703-2013, 2013
L. Ahlm, J. Julin, C. Fountoukis, S. N. Pandis, and I. Riipinen
Atmos. Chem. Phys., 13, 10271–10283, https://doi.org/10.5194/acp-13-10271-2013, https://doi.org/10.5194/acp-13-10271-2013, 2013
E. Kostenidou, C. Kaltsonoudis, M. Tsiflikiotou, E. Louvaris, L. M. Russell, and S. N. Pandis
Atmos. Chem. Phys., 13, 8797–8811, https://doi.org/10.5194/acp-13-8797-2013, https://doi.org/10.5194/acp-13-8797-2013, 2013
J. Lelieveld, C. Barlas, D. Giannadaki, and A. Pozzer
Atmos. Chem. Phys., 13, 7023–7037, https://doi.org/10.5194/acp-13-7023-2013, https://doi.org/10.5194/acp-13-7023-2013, 2013
A.C. Nölscher, E. Bourtsoukidis, B. Bonn, J. Kesselmeier, J. Lelieveld, and J. Williams
Biogeosciences, 10, 4241–4257, https://doi.org/10.5194/bg-10-4241-2013, https://doi.org/10.5194/bg-10-4241-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
C. Brühl, J. Lelieveld, M. Höpfner, and H. Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-11395-2013, https://doi.org/10.5194/acpd-13-11395-2013, 2013
Revised manuscript not accepted
G. J. Phillips, N. Pouvesle, J. Thieser, G. Schuster, R. Axinte, H. Fischer, J. Williams, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 13, 1129–1139, https://doi.org/10.5194/acp-13-1129-2013, https://doi.org/10.5194/acp-13-1129-2013, 2013
E. Athanasopoulou, H. Vogel, B. Vogel, A. P. Tsimpidi, S. N. Pandis, C. Knote, and C. Fountoukis
Atmos. Chem. Phys., 13, 625–645, https://doi.org/10.5194/acp-13-625-2013, https://doi.org/10.5194/acp-13-625-2013, 2013
J. Lelieveld, M. G. Lawrence, and D. Kunkel
Atmos. Chem. Phys., 13, 31–34, https://doi.org/10.5194/acp-13-31-2013, https://doi.org/10.5194/acp-13-31-2013, 2013
A. Jugold, F. Althoff, M. Hurkuck, M. Greule, K. Lenhart, J. Lelieveld, and F. Keppler
Biogeosciences, 9, 5291–5301, https://doi.org/10.5194/bg-9-5291-2012, https://doi.org/10.5194/bg-9-5291-2012, 2012
V.-M. Kerminen, M. Paramonov, T. Anttila, I. Riipinen, C. Fountoukis, H. Korhonen, E. Asmi, L. Laakso, H. Lihavainen, E. Swietlicki, B. Svenningsson, A. Asmi, S. N. Pandis, M. Kulmala, and T. Petäjä
Atmos. Chem. Phys., 12, 12037–12059, https://doi.org/10.5194/acp-12-12037-2012, https://doi.org/10.5194/acp-12-12037-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the Long-term Trend of Organic Aerosol and the Influences from Anthropogenic Emission and Regional Climate Change in China
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Trends and Drivers of Soluble Iron Deposition from East Asian Dust to the Northwest Pacific: A Springtime Analysis (2001–2017)
Impacts of Sea Ice Leads on Sea Salt Aerosols and Atmospheric Chemistry in the Arctic
Implications of Reduced-Complexity Aerosol Thermodynamics on Organic Aerosol Mass Concentration and Composition over North America
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Population exposure to outdoor NO2, black carbon, particle mass, and number concentrations over Paris with multi-scale modelling down to the street scale
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
Modelling of atmospheric variability of gas and aerosols during the ACROSS campaign 2022 in the greater Paris area: evaluation of the meteorology, dynamics and chemistry
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Long-term trends in aerosol properties derived from AERONET measurements
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Critical Load Exceedances for North America and Europe using an Ensemble of Models and an Investigation of Causes for Environmental Impact Estimate Variability: An AQMEII4 Study
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
AERO-MAP: A data compilation and modelling approach to understand spatial variability in fine and coarse mode aerosol composition
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Spatial-temporal patterns of anthropogenic and biomass burning contributions on air pollution and mortality burden changes in India from 1995 to 2014
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
EGUsphere, https://doi.org/10.5194/egusphere-2024-3584, https://doi.org/10.5194/egusphere-2024-3584, 2024
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different time scales. Its application in Changzhou, China revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residues.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3420, https://doi.org/10.5194/egusphere-2024-3420, 2024
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Understanding long-term organic aerosols (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6% from 1990 to 2019, primarily due to a 32.3% increase in secondary organic aerosols (SOA) and an 8.1% decrease in primary organic aerosols (POA), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2293, https://doi.org/10.5194/egusphere-2024-2293, 2024
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Dust soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust, but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. It underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Erin Emme and Hannah Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-3147, https://doi.org/10.5194/egusphere-2024-3147, 2024
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There is uncertainty in the sources of Arctic cold season (November-April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-2712, https://doi.org/10.5194/egusphere-2024-2712, 2024
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Organic aerosol water content impacts the gas–particle partitioning of semivolatile organics. We used an aerosol thermodynamic model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake and nonideal mixing. This led to a substantial enhancement in mean organic aerosol mass concentration with respect to GEOS-Chem's most advanced scheme. The water-sensitive scheme could be a valuable tool for reconciling model estimations and field measurements.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D’Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2024-2120, https://doi.org/10.5194/egusphere-2024-2120, 2024
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To accurately represent the population exposure to outdoor concentrations of pollutants of health interest (NO2, black carbon, PM2.5, ultrafine particles), multi-scale modelling down to the street scale is setup and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing to correct regional-scale simulations to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon and ultrafine particles, but less PM2.5.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Rubén Soussé-Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2024-2310, https://doi.org/10.5194/egusphere-2024-2310, 2024
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
EGUsphere, https://doi.org/10.5194/egusphere-2024-2175, https://doi.org/10.5194/egusphere-2024-2175, 2024
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Summer 2022 has been considered a proxy for future climate scenarios, given the registered hot and dry conditions. In this paper, we used the measurements from the ACROSS campaign, occurred over the Paris area in June–July 2022, in addition to observations from existing networks, to evaluate the WRF–CHIMERE model simulation over France and the Ile-de-France regions. Results over the Ile–de–France show to be satisfactory, allowing to explain the gas and aerosol variability at the ACROSS sites.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
EGUsphere, https://doi.org/10.5194/egusphere-2024-2533, https://doi.org/10.5194/egusphere-2024-2533, 2024
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America, increased anthropogenic source over North India, increased dust activities over the Arabian Peninsula, etc.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz-Ozdemir, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Iannis Koutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark Shephard, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2024-2226, https://doi.org/10.5194/egusphere-2024-2226, 2024
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The large range of sulphur and nitrogen deposition estimates from air-quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulphur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by droplets, rain, snow, etc., aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, and gas deposition via plant cuticles and soil.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-1617, https://doi.org/10.5194/egusphere-2024-1617, 2024
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
EGUsphere, https://doi.org/10.5194/egusphere-2024-974, https://doi.org/10.5194/egusphere-2024-974, 2024
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India is facing a severe air pollution crisis that poses significant health risks, particularly from PM2.5 and O3. Our study reveals rising levels of both pollutants from 1995 to 2014, leading to increased premature mortality. While anthropogenic emissions play a significant role, biomass burning also impacts air quality, in particular seasons and regions in India. This study highlights the urgent need for localized policies to protect public health amid escalating environmental challenges.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Cited articles
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Short summary
We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions...
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