Articles | Volume 20, issue 17
Atmos. Chem. Phys., 20, 10351–10377, 2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
07 Sep 2020
Research article | 07 Sep 2020
Treatment of non-ideality in the SPACCIM multiphase model – Part 2: Impacts on the multiphase chemical processing in deliquesced aerosol particles
Ahmad Jhony Rusumdar et al.
No articles found.
Manuela van Pinxteren, Tiera-Brandy Robinson, Sebastian Zeppenfeld, Xianda Gong, Enno Bahlmann, Khanneh Wadinga Fomba, Nadja Triesch, Frank Stratmann, Oliver Wurl, Anja Engel, Heike Wex, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 5725–5742,Short summary
A class of marine particles (transparent exopolymer particles, TEPs) that is ubiquitously found in the world oceans was measured for the first time in ambient marine aerosol particles and marine cloud waters in the tropical Atlantic Ocean. TEPs are likely to have good properties for influencing clouds. We show that TEPs are transferred from the ocean to the marine atmosphere via sea-spray formation and our results suggest that they can also form directly in aerosol particles and in cloud water.
Kristina Glojek, Griša Močnik, Honey Dawn C. Alas, Andrea Cuesta-Mosquera, Luka Drinovec, Asta Gregorič, Matej Ogrin, Kay Weinhold, Irena Ježek, Thomas Müller, Martin Rigler, Maja Remškar, Dominik van Pinxteren, Hartmut Herrmann, Martina Ristorini, Maik Merkel, Miha Markelj, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 5577–5601,Short summary
A pilot study to determine the emissions of wood burning under
real-world laboratoryconditions was conducted. We found that measured black carbon (eBC) and particulate matter (PM) in rural shallow terrain depressions with residential wood burning could be much greater than predicted by models. The exceeding levels are a cause for concern since similar conditions can be expected in numerous hilly and mountainous regions across Europe, where approximately 20 % of the total population lives.
Nabil Deabji, Khanneh Wadinga Fomba, Souad El Hajjaji, Abdelwahid Mellouki, Laurent Poulain, Sebastian Zeppenfeld, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 18147–18174,Short summary
Mountain and high-altitude sites provide representative data for the lower free troposphere, various pathways for aerosol interactions, and changing boundary layer heights useful in understanding atmospheric composition. However, only few studies exist in African regions despite diversity in both natural and anthropogenic emissions. This study provides detailed atmospheric studies in the northern African high-altitude region.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697,Short summary
This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536,Short summary
Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018,Short summary
The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Markus Hartmann, Xianda Gong, Simonas Kecorius, Manuela van Pinxteren, Teresa Vogl, André Welti, Heike Wex, Sebastian Zeppenfeld, Hartmut Herrmann, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 21, 11613–11636,Short summary
Ice-nucleating particles (INPs) are not well characterized in the Arctic despite their importance for the Arctic energy budget. Little is known about their nature (mineral or biological) and sources (terrestrial or marine, long-range transport or local). We find indications that, at the beginning of the melt season, a local, biogenic, probably marine source is likely, but significant enrichment of INPs has to take place from the ocean to the aerosol phase.
Lady Mateus-Fontecha, Angela Vargas-Burbano, Rodrigo Jimenez, Nestor Y. Rojas, German Rueda-Saa, Dominik van Pinxteren, Manuela van Pinxteren, Khanneh Wadinga Fomba, and Hartmut Herrmann
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study reports the chemical composition of regionally representative PM2.5 in an area densely populated and substantially industrialized, located in the inter-Andean valley with the highest sugarcane yield in the world and where sugarcane is burned and harvested year-round. We found that sugarcane burning did not portrait as a distinguishable sample composition component. Instead, the composition analysis revealed multiple associations among sugarcane burning components and other sources.
Anke Mutzel, Yanli Zhang, Olaf Böge, Maria Rodigast, Agata Kolodziejczyk, Xinming Wang, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 8479–8498,Short summary
This study investigates secondary organic aerosol (SOA) formation and particle growth from α-pinene, limonene, and m-cresol oxidation through NO3 and OH radicals and the effect of relative humidity. The formed SOA is comprehensively characterized with respect to the content of OC / EC, WSOC, SOA-bound peroxides, and SOA marker compounds. The findings present new insights and implications of nighttime chemistry, which can form SOA more efficiently than OH radical reaction during daytime.
Matthias Faust, Ralf Wolke, Steffen Münch, Roger Funk, and Kerstin Schepanski
Geosci. Model Dev., 14, 2205–2220,Short summary
Trajectory dispersion models are powerful and intuitive tools for tracing air pollution through the atmosphere. But the turbulent nature of the atmospheric boundary layer makes it challenging to provide accurate predictions near the surface. To overcome this, we propose an approach using wind and turbulence information at high temporal resolution. Finally, we demonstrate the strength of our approach in a case study on dust emissions from agriculture.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808,Short summary
Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Nadja Triesch, Manuela van Pinxteren, Sanja Frka, Christian Stolle, Tobias Spranger, Erik Hans Hoffmann, Xianda Gong, Heike Wex, Detlef Schulz-Bull, Blaženka Gašparović, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 4267–4283,Short summary
To investigate the source of lipids and their representatives in the marine atmosphere, concerted measurements of seawater and submicrometer aerosol particle sampling were carried out on the Cabo Verde islands. This field study describes the biogenic sources of lipids, their selective transfer from the ocean into the atmosphere and their enrichment as part of organic matter. A strong enrichment of the studied representatives of the lipid classes on submicrometer aerosol particles was observed.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 3667–3684,Short summary
We present results from source apportionment analysis on the carbonaceous aerosol particles, including organic aerosol (OA) and equivalent black carbon (eBC), allowing us to distinguish local emissions from long-range transport for OA and eBC sources. By merging online chemical measurements and considering particle number size distribution, the different air masses reaching the sampling place were described and discussed, based on their respective chemical composition and size distribution.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338,Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Nadja Triesch, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 163–181,Short summary
To investigate the sources of free amino acids (FAAs) in the marine atmosphere, concerted measurements (the simultaneous investigation of seawater, size-segregated aerosol particles and cloud water) were performed at the Cabo Verde islands. This study describes the transfer of FAAs as part of organic matter from the ocean into the atmosphere on a molecular level. In the investigated marine environment, a high enrichment of FAAs in submicron aerosol particles and in cloud droplets was observed.
Jiarong Li, Chao Zhu, Hui Chen, Defeng Zhao, Likun Xue, Xinfeng Wang, Hongyong Li, Pengfei Liu, Junfeng Liu, Chenglong Zhang, Yujing Mu, Wenjin Zhang, Luming Zhang, Hartmut Herrmann, Kai Li, Min Liu, and Jianmin Chen
Atmos. Chem. Phys., 20, 13735–13751,Short summary
Based on a field study at Mt. Tai, China, the simultaneous variations of cloud microphysics, aerosol microphysics and their potential interactions during cloud life cycles were discussed. Results demonstrated that clouds on clean days were more susceptible to the concentrations of particle number, while clouds formed on polluted days might be more sensitive to meteorological parameters. Particles larger than 150 nm played important roles in forming cloud droplets with sizes of 5–10 μm.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519,Short summary
Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Yangang Ren, Bastian Stieger, Gerald Spindler, Benoit Grosselin, Abdelwahid Mellouki, Thomas Tuch, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 13069–13089,Short summary
We present HONO measurements from the TROPOS research site in Melpitz, Germany. Investigations of HONO sources and sinks revealed the nighttime formation by heterogeneous conversion of NO2 to HONO followed by a significant surface deposition at night. The evaporation of dew was identified as the main HONO source in the morning. In the following, dew measurements with a self-made dew collector were performed to estimate the amount of evaporated HONO from dew in the atmospheric HONO distribution.
Laurent Poulain, Gerald Spindler, Achim Grüner, Thomas Tuch, Bastian Stieger, Dominik van Pinxteren, Jean-Eudes Petit, Olivier Favez, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Meas. Tech., 13, 4973–4994,Short summary
The stability and the comparability between ACSM and collocated filter sampling and MPSS measurements was investigated in order to examine the instruments robustness for year-long measurements. Specific attention was paid to the influence of the upper size cutoff diameter to better understand how it might affect the data validation. Recommendations are provided for better on-site quality assurance and quality control of the ACSM, which would be useful for either long-term or intensive campaigns.
Khanneh Wadinga Fomba, Nabil Deabji, Sayf El Islam Barcha, Ibrahim Ouchen, El Mehdi Elbaramoussi, Rajaa Cherkaoui El Moursli, Mimoun Harnafi, Souad El Hajjaji, Abdelwahid Mellouki, and Hartmut Herrmann
Atmos. Meas. Tech., 13, 4773–4790,Short summary
As air quality monitoring networks often sample aerosol particles on quartz filters, the development and applicability of analytical methods with quartz filters are becoming important. In this study different filter preparation methods (e.g., baking, acid digestion) were investigated for quantifying trace metals on quartz and polycarbonate filters, and cloud water using the total reflection X-Ray fluorescence (TXRF) technique, with low detection limits of about 0.3 ng cm−3 for some elements.
Sebastian Zeppenfeld, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Ocean Sci., 16, 817–830,Short summary
An analytical method combining electro-dialysis with high-performance anionic exchange chromatography coupled to pulsed amperometric detection was developed and optimized for analyzing free and combined carbohydrates in seawater and other saline environmental samples.
Manuela van Pinxteren, Khanneh Wadinga Fomba, Nadja Triesch, Christian Stolle, Oliver Wurl, Enno Bahlmann, Xianda Gong, Jens Voigtländer, Heike Wex, Tiera-Brandy Robinson, Stefan Barthel, Sebastian Zeppenfeld, Erik Hans Hoffmann, Marie Roveretto, Chunlin Li, Benoit Grosselin, Veronique Daële, Fabian Senf, Dominik van Pinxteren, Malena Manzi, Nicolás Zabalegui, Sanja Frka, Blaženka Gašparović, Ryan Pereira, Tao Li, Liang Wen, Jiarong Li, Chao Zhu, Hui Chen, Jianmin Chen, Björn Fiedler, Wolf von Tümpling, Katie Alana Read, Shalini Punjabi, Alastair Charles Lewis, James Roland Hopkins, Lucy Jane Carpenter, Ilka Peeken, Tim Rixen, Detlef Schulz-Bull, María Eugenia Monge, Abdelwahid Mellouki, Christian George, Frank Stratmann, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 6921–6951,Short summary
An introduction to a comprehensive field campaign performed at the Cape Verde Atmospheric Observatory regarding ocean–atmosphere interactions is given. Chemical, physical, biological and meteorological techniques were applied, and measurements of bulk water, the sea surface microlayer, cloud water and ambient aerosol particles took place. Oceanic compounds were found to be transferred to atmospheric aerosol and to the cloud level; however, sea spray contributions to CCN and INPs were limited.
Yanhong Zhu, Andreas Tilgner, Erik Hans Hoffmann, Hartmut Herrmann, Kimitaka Kawamura, Lingxiao Yang, Likun Xue, and Wenxing Wang
Atmos. Chem. Phys., 20, 6725–6747,Short summary
The formation and processing of secondary inorganic and organic compounds at Mt. Tai, the highest mountain on the North China Plain, are modeled using a multiphase chemical model. The concentrations of key radical and non-radical oxidations in the formation processes are investigated. Sensitivity tests assess the impacts of emission data and glyoxal partitioning constants on modeled results. The key precursors of secondary organic compounds are also identified.
Erik H. Hoffmann, Roland Schrödner, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Geosci. Model Dev., 13, 2587–2609,Short summary
A condensed multiphase halogen and DMS chemistry mechanism for application in chemical transport models has been developed and applied by 2D simulations to explore multiphase marine chemistry above the pristine open ocean. The model simulations have demonstrated the ability of the mechanism in studying aerosol cloud processing effects in the marine atmosphere. First 2D simulations have shown significant differences in the DMS processing under convective and stratiform cloud conditions.
Nicolás Zabalegui, Malena Manzi, Antoine Depoorter, Nathalie Hayeck, Marie Roveretto, Chunlin Li, Manuela van Pinxteren, Hartmut Herrmann, Christian George, and María Eugenia Monge
Atmos. Chem. Phys., 20, 6243–6257,Short summary
A new approach to bridging different fields of science by studying the air–sea interface is described. An untargeted ambient mass-spectrometry-based metabolomics method enables the study of enriched organic compounds found on the sea surface for air–water transfer processes. Results from the metabolomics experiments and a lab-to-field approach provide new opportunities for characterizing the seawater organic-matter content and discovering compounds involved in aerosol-formation processes.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888,Short summary
Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Xianda Gong, Heike Wex, Jens Voigtländer, Khanneh Wadinga Fomba, Kay Weinhold, Manuela van Pinxteren, Silvia Henning, Thomas Müller, Hartmut Herrmann, and Frank Stratmann
Atmos. Chem. Phys., 20, 1431–1449,Short summary
We characterized the aerosol particles in Cabo Verde at sea and cloud levels. We found four well-separable types of PNSDs, with the strongest differences between air masses coming from the ocean compared to from the African continent. During the strongest observed dust periods, CCN concentrations were 2.5 higher than during clean marine periods. The hygroscopicity of the particles did not vary much between different periods. Aerosol at sea level and on the mountaintop was well in agreement.
Xianda Gong, Heike Wex, Manuela van Pinxteren, Nadja Triesch, Khanneh Wadinga Fomba, Jasmin Lubitz, Christian Stolle, Tiera-Brandy Robinson, Thomas Müller, Hartmut Herrmann, and Frank Stratmann
Atmos. Chem. Phys., 20, 1451–1468,Short summary
In this study, we examined number concentrations of ice nucleating particles (INPs) at Cabo Verde in the oceanic sea surface microlayer and underlying seawater, in the air close to both sea level and cloud level, and in cloud water. The results show that most INPs are supermicron in size, that INP number concentrations in air fit well to those in cloud water and that sea spray aerosols at maximum contributed a small fraction of all INPs in the air at Cabo Verde.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254,Short summary
Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
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,Short summary
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.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407,Short summary
This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
Marco Pandolfi, Dennis Mooibroek, Philip Hopke, Dominik van Pinxteren, Xavier Querol, Hartmut Herrmann, Andrés Alastuey, Olivier Favez, Christoph Hüglin, Esperanza Perdrix, Véronique Riffault, Stéphane Sauvage, Eric van der Swaluw, Oksana Tarasova, and Augustin Colette
Atmos. Chem. Phys., 20, 409–429,Short summary
In the last scientific assessment report from the LRTAP Convention, it is stated that because non-urban sources are often major contributors to urban pollution, many cities will be unable to meet WHO guideline levels for air pollutants through local action alone. Consequently, it is very important to estimate how much the local and non-local sources contribute to urban pollution in order to design global strategies to reduce the levels of pollutants in European cities.
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364,Short summary
Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Peter Bräuer, Camille Mouchel-Vallon, Andreas Tilgner, Anke Mutzel, Olaf Böge, Maria Rodigast, Laurent Poulain, Dominik van Pinxteren, Ralf Wolke, Bernard Aumont, and Hartmut Herrmann
Atmos. Chem. Phys., 19, 9209–9239,Short summary
The article presents a new protocol for computer-assisted automated aqueous-phase chemistry mechanism generation, which has been validated against chamber experiments. Together with a large kinetics database and improved prediction methods for kinetic data, the novel protocol provides an unmatched tool for detailed studies of tropospheric aqueous-phase chemistry in complex model studies and for the design and analysis of chamber experiments.
Bastian Stieger, Gerald Spindler, Dominik van Pinxteren, Achim Grüner, Markus Wallasch, and Hartmut Herrmann
Atmos. Meas. Tech., 12, 281–298,Short summary
A MARGA was combined with an additional IC system specialized for the 2 h interval online quantification of 12 low-molecular-weight organic acids in the gas and particle phases. Low limits of detection and good precision were achieved. The suitability for field measurements was shown. This setup reduces laboratory work and filter sampling artifacts. Diurnal profiles, sources and phase distributions of these compounds will improve the knowledge of the tropospheric multiphase chemistry.
Shan Huang, Zhijun Wu, Laurent Poulain, Manuela van Pinxteren, Maik Merkel, Denise Assmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 18043–18062,Short summary
The Atlantic aerosols are characterized based on high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements during four open-ocean cruises. This unique data set provides the latitudinal distribution of source contributions of organic aerosols (OAs) over the Atlantic Ocean, showing that marine sources could control the OA formation over the South Atlantic, while strong continental influence was found near Africa and Europe.
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,Short summary
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.
Yanhong Zhu, Lingxiao Yang, Jianmin Chen, Kimitaka Kawamura, Mamiko Sato, Andreas Tilgner, Dominik van Pinxteren, Ying Chen, Likun Xue, Xinfeng Wang, Isobel J. Simpson, Hartmut Herrmann, Donald R. Blake, and Wenxing Wang
Atmos. Chem. Phys., 18, 10741–10758,Short summary
Molecular distributions of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in the free troposphere are identified, and their concentration variations between 2014 and 2006 are presented. High nighttime concentrations were probably due to precursor emissions and aqueous-phase oxidation. Biomass burning was significant, but its tracer levoglucosan in 2014 was 5 times lower than 2006 concentrations. Finally, regional emission from anthropogenic activities was identified as a major source.
Laura Palacios-Peña, Rocío Baró, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, José María López-Romero, Juan Pedro Montávez, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 18, 5021–5043,Short summary
Atmospheric aerosols modify the radiative budget of the Earth, and it is therefore mandatory to have an accurate representation of their optical properties for understanding their climatic role. This work therefore evaluates the skill in the representation of optical properties by different remote-sensing sensors and regional online coupled chemistry–climate models over Europe.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881,Short summary
Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Ying Chen, Ralf Wolke, Liang Ran, Wolfram Birmili, Gerald Spindler, Wolfram Schröder, Hang Su, Yafang Cheng, Ina Tegen, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 673–689,Short summary
The heterogeneous hydrolysis of N2O5 on particle surfaces is crucial for the nitrogen cycle in the atmosphere. The reaction rate is determined by meteorological and particle properties, but its parameterization in previous 3-D modelling studies did not comprehensively consider these parameters. We propose a parameterization to take these into account and improve nitrate prediction; we report that the organic coating suppression on the N2O5 reaction is not as important as expected in the EU.
Kathrin Gatzsche, Yoshiteru Iinuma, Andreas Tilgner, Anke Mutzel, Torsten Berndt, and Ralf Wolke
Atmos. Chem. Phys., 17, 13187–13211,Short summary
Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and, thus, an advanced treatment of SOA processes in models is necessary. Therefore, this investigation aims at sensitivity studies of a kinetic description of SOA formation. The results reveal that the particle-phase state and the reactivity of the organic solutes are key parameters in the SOA formation. Overall, the results show that an advanced kinetic treatment enables improved model predictions.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267,Short summary
Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Jiarong Li, Xinfeng Wang, Jianmin Chen, Chao Zhu, Weijun Li, Chengbao Li, Lu Liu, Caihong Xu, Liang Wen, Likun Xue, Wenxing Wang, Aijun Ding, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 9885–9896,Short summary
Cloud events at Mt. Tai were investigated for the chemical composition and size distribution of cloud droplets. An obvious rise in pH was found for elevated NH+4 during the last decade. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions, smaller sizes and higher numbers of cloud droplets. The mechanism of cloud-droplet formation and the mass transfer between aerosol–gas–cloud phases were summarized to enrich the knowledge of cloud chemical and microphysical properties.
Rocío Baró, Laura Palacios-Peña, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 17, 9677–9696,Short summary
The influence on modeled max., mean and min. temperature over Europe of including aerosol–radiation–cloud interactions has been assessed for two case studies in 2010. Data were taken from an ensemble of online regional chemistry–climate models from EuMetChem COST Action. The results indicate that including these interactions clearly improves the spatiotemporal variability in the temperature signal simulated by the models, with implications for reducing the uncertainty in climate projections.
Sudhakar Dipu, Johannes Quaas, Ralf Wolke, Jens Stoll, Andreas Mühlbauer, Odran Sourdeval, Marc Salzmann, Bernd Heinold, and Ina Tegen
Geosci. Model Dev., 10, 2231–2246,
Maria Rodigast, Anke Mutzel, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 3929–3943,Short summary
The study presents, for the first time, a quantification method for methylglyoxal oligomers and highlights their importance for SOA formation. The method was applied to determine the fraction of methylglyoxal oligomers of 1,3,5-trimethylbenzene SOA dependent on relative humidity and seed particle acidity. An oligomer contribution of up to 8 % was calculated varying with experimental conditions and thus further hints for the dependency of the oligomer formation mechanism on conditions were found.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162,Short summary
Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic and natural emissions. This review results from a June 2015 workshop and includes the recent literature on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for future research in modeling, field observations, and laboratory studies.
Monique Teich, Dominik van Pinxteren, Michael Wang, Simonas Kecorius, Zhibin Wang, Thomas Müller, Griša Močnik, and Hartmut Herrmann
Atmos. Chem. Phys., 17, 1653–1672,Short summary
This study provides a large data set on concentrations of individual brown carbon constituents, i.e., nitrated aromatic compounds, in diverse atmospheric environments and their relative contribution to water-soluble and particulate light absorption. It extends the existing knowledge on the abundance of brown carbon and its molecular composition and provides scientific motivation for further studies on ambient brown carbon constituents.
Martin Brüggemann, Laurent Poulain, Andreas Held, Torsten Stelzer, Christoph Zuth, Stefanie Richters, Anke Mutzel, Dominik van Pinxteren, Yoshiteru Iinuma, Sarmite Katkevica, René Rabe, Hartmut Herrmann, and Thorsten Hoffmann
Atmos. Chem. Phys., 17, 1453–1469,Short summary
Using complementary mass spectrometric techniques during a field study in central Europe, characteristic contributors to the organic aerosol mass were identified. Besides common marker compounds for biogenic secondary organic aerosol, highly oxidized sulfur species were detected in the particle phase. High-time-resolution measurements revealed correlations between these organosulfates and particulate sulfate as well as gas-phase peroxyradicals, giving hints to underlying formation mechanisms.
Johannes Schneider, Stephan Mertes, Dominik van Pinxteren, Hartmut Herrmann, and Stephan Borrmann
Atmos. Chem. Phys., 17, 1571–1593,Short summary
We analyzed the composition of cloud droplet residuals and of aerosol particles sampled on a mountaintop site. The data show that about 85 % of the submicron aerosol mass partitions into the cloud phase, and that the uptake of soluble compounds (nitric acid, ammonia, and organic gases) from the gas phase into the cloud droplets is very effective. This will lead to a redistribution of these compounds among the aerosol particles and thereby to a more uniform aerosol after cloud evaporation.
Ying Chen, Yafang Cheng, Nan Ma, Ralf Wolke, Stephan Nordmann, Stephanie Schüttauf, Liang Ran, Birgit Wehner, Wolfram Birmili, Hugo A. C. Denier van der Gon, Qing Mu, Stefan Barthel, Gerald Spindler, Bastian Stieger, Konrad Müller, Guang-Jie Zheng, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 12081–12097,Short summary
Sea salt aerosol (SSA) is important for primary and secondary aerosols on a global scale. During 10–20 September 2013, the SSA mass concentration was overestimated by a factor of 8–20 over central Europe by WRF-Chem model, stem from the uncertainty of its emission scheme. This could facilitate the coarse-mode nitrate formation (~ 140 % but inhibit the fine-mode nitrate formation (~−20 %). A special long-range transport mechanism could broaden this influence of SSA to a larger downwind region.
Silvia Sandrini, Dominik van Pinxteren, Lara Giulianelli, Hartmut Herrmann, Laurent Poulain, Maria Cristina Facchini, Stefania Gilardoni, Matteo Rinaldi, Marco Paglione, Barbara J. Turpin, Francesca Pollini, Silvia Bucci, Nicola Zanca, and Stefano Decesari
Atmos. Chem. Phys., 16, 10879–10897,Short summary
This paper deals with impactor measurements performed in the summer 2012 during the EU project PEGASOS campaign in the Po Valley, at an urban and a rural site. The paper tries to disentangle the effects of weather anomalies (temporal and spatial) from those of diverse emissions (NH3) and chemical processes on the formation of secondary aerosols in the region, with special focus on nocturnal ammonium nitrate formation and its implications (aqueous formation of secondary organic aerosol).
Stefanie Richters, Hartmut Herrmann, and Torsten Berndt
Atmos. Chem. Phys., 16, 9831–9845,Short summary
New reaction pathways of highly oxidized multifunctional organic compounds (HOMs) from the ozonolysis of the sesquiterpene (C15H24) beta-caryophyllene were elucidated based on experiments using isotopically labelled ozone and H/D exchange experiments. These new insights in reaction pathways of unsaturated RO2 radicals are responsible for the production of about two-thirds of the detected HOMs from beta-caryophyllene and extend the knowledge of HOM formation mechanisms in the atmosphere.
Nan Ma, Chunsheng Zhao, Jiangchuan Tao, Zhijun Wu, Simonas Kecorius, Zhibin Wang, Johannes Größ, Hongjian Liu, Yuxuan Bian, Ye Kuang, Monique Teich, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Hartmut Herrmann, Min Hu, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 8593–8607,Short summary
New particle formation (NPF) is one of main sources of cloud condensation nuclei (CCN) in the atmosphere. Based on in situ measurements, we found that CCN activity of newly formed particles largely differs in different NPF events. It is therefore difficult to find a simple parameterization of CCN activity for NPF events. Using a fixed size-resolved activation ratio curve or critical diameter is very likely to result in large biases up to 50 % in the calculated NCCN during NPF events.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108,Short summary
This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
James W. Grayson, Yue Zhang, Anke Mutzel, Lindsay Renbaum-Wolff, Olaf Böge, Saeid Kamal, Hartmut Herrmann, Scot T. Martin, and Allan K. Bertram
Atmos. Chem. Phys., 16, 6027–6040,Short summary
The effect of several experimental parameters on the viscosity of secondary organic material (SOM) generated from the ozonolysis of α-pinene has been studied. The results demonstrate that the viscosity of SOM depends on the particle mass concentration at which SOM is produced, and the relative humidity (RH) at which the SOM is studied. Hence, particle mass concentration and RH should be considered when comparing experimental results for SOM, or extrapolating laboratory results to the atmosphere.
Dominik van Pinxteren, Khanneh Wadinga Fomba, Stephan Mertes, Konrad Müller, Gerald Spindler, Johannes Schneider, Taehyoung Lee, Jeffrey L. Collett, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 3185–3205,
Yan Lv, Xiang Li, Ting Ting Xu, Tian Tao Cheng, Xin Yang, Jian Min Chen, Yoshiteru Iinuma, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 2971–2983,Short summary
The study focused on size-resolved PAHs in urban aerosols at a megacity Shanghai site. The results provide us with a mechanistic understanding of the particle size distribution of PAHs and their transport in the human respiratory system; this can help develop better source control strategies.
Maria Rodigast, Anke Mutzel, Janine Schindelka, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 2689–2702,Short summary
The study highlights methyl ethyl ketone as a new and unknown source for methylglyoxal in the aqueous phase that is important for aqueous secondary organic aerosol (aqSOA) formation. Besides 2,3-butanedione (29.5 %) and hydroxyacetone (3.0 %), methylglyoxal was formed with a molar yield of 9.5 %. According to the detected products a reaction mechanism was developed and evaluated. The comparison of the model and experimental data showed excellent agreements, in particular for methylglyoxal.
Ying Chen, Ya-Fang Cheng, Stephan Nordmann, Wolfram Birmili, Hugo A. C. Denier van der Gon, Nan Ma, Ralf Wolke, Birgit Wehner, Jia Sun, Gerald Spindler, Qing Mu, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 1823–1835,Short summary
We evaluated the EC point sources in Germany with high-resolution simulation by WRF-Chem, and find out that point sources contribute too much EC in the coarse mode aerosol mass. The area emissions in Eastern Europe and Russia also allocate too much EC emission in coarse mode in the EUCAARI EC emission inventory. Because of the shorter life time of coarse mode EC, about 20–40 % less EC can be transported to Melpitz from Eastern Europe. Size segregation information is important for EC inventories.
A. J. Rusumdar, R. Wolke, A. Tilgner, and H. Herrmann
Geosci. Model Dev., 9, 247–281,Short summary
The present paper was aimed at the further development of SPACCIM to treat both complex multiphase chemistry and phase transfer processes considering new non-ideality properties of concentrated solutions. Model studies showed the applicability of the new kinetic model approach for complex aerosol mixtures and detailed chemical mechanisms. Simulations have implied that the treatment of non-ideality should be mandatory for modeling multiphase chemical processes in deliquesced particles.
A. Roth, J. Schneider, T. Klimach, S. Mertes, D. van Pinxteren, H. Herrmann, and S. Borrmann
Atmos. Chem. Phys., 16, 505–524,Short summary
This paper reports on single-particle measurements of ambient aerosol particles and cloud residues sampled from orographic clouds on a mountain site in central Germany. The results show that soot particles can get efficiently activated in cloud droplets when they are mixed with or coated by sulfate and nitrate. Cloud processing leads to addition of nitrate and sulfate to the particles, thereby increasing the hygroscopicity of these particles when they remain in the air after cloud evaporation.
K. W. Fomba, D. van Pinxteren, K. Müller, Y. Iinuma, T. Lee, J. L. Collett Jr., and H. Herrmann
Atmos. Chem. Phys., 15, 8751–8765,
M. Rodigast, A. Mutzel, Y. Iinuma, S. Haferkorn, and H. Herrmann
Atmos. Meas. Tech., 8, 2409–2416,Short summary
An optimised method for derivatisation of carbonyl compounds with o-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine (PFBHA) in aqueous samples is described. The comprehensive optimisation of the method leads to an improvement of the detection limit up to a factor of 10 highlighting the good sensitivity of the optimised method for atmospherically relevant carbonyl compounds. The optimised method was successfully applied to detect carbonyl compounds from the aqueous phase oxidation of 3-methylbutanone.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301,
L. Poulain, W. Birmili, F. Canonaco, M. Crippa, Z. J. Wu, S. Nordmann, G. Spindler, A. S. H. Prévôt, A. Wiedensohler, and H. Herrmann
Atmos. Chem. Phys., 14, 10145–10162,
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128,
K. W. Fomba, K. Müller, D. van Pinxteren, L. Poulain, M. van Pinxteren, and H. Herrmann
Atmos. Chem. Phys., 14, 8883–8904,
S. Henning, K. Dieckmann, K. Ignatius, M. Schäfer, P. Zedler, E. Harris, B. Sinha, D. van Pinxteren, S. Mertes, W. Birmili, M. Merkel, Z. Wu, A. Wiedensohler, H. Wex, H. Herrmann, and F. Stratmann
Atmos. Chem. Phys., 14, 7859–7868,
L. Schöne and H. Herrmann
Atmos. Chem. Phys., 14, 4503–4514,
S. Scheinhardt, D. van Pinxteren, K. Müller, G. Spindler, and H. Herrmann
Atmos. Chem. Phys., 14, 4531–4538,
E. Harris, B. Sinha, D. van Pinxteren, J. Schneider, L. Poulain, J. Collett, B. D'Anna, B. Fahlbusch, S. Foley, K. W. Fomba, C. George, T. Gnauk, S. Henning, T. Lee, S. Mertes, A. Roth, F. Stratmann, S. Borrmann, P. Hoppe, and H. Herrmann
Atmos. Chem. Phys., 14, 4219–4235,
D. van Pinxteren, C. Neusüß, and H. Herrmann
Atmos. Chem. Phys., 14, 3913–3928,
N. Niedermeier, A. Held, T. Müller, B. Heinold, K. Schepanski, I. Tegen, K. Kandler, M. Ebert, S. Weinbruch, K. Read, J. Lee, K. W. Fomba, K. Müller, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 14, 2245–2266,
A. Kahnt, Y. Iinuma, A. Mutzel, O. Böge, M. Claeys, and H. Herrmann
Atmos. Chem. Phys., 14, 719–736,
S. Barthel, I. Tegen, R. Wolke, and M. van Pinxteren
Atmos. Chem. Phys. Discuss.,
Revised manuscript not accepted
M. van Pinxteren and H. Herrmann
Atmos. Chem. Phys., 13, 11791–11802,
Z. J. Wu, L. Poulain, S. Henning, K. Dieckmann, W. Birmili, M. Merkel, D. van Pinxteren, G. Spindler, K. Müller, F. Stratmann, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 13, 7983–7996,
Z. Wu, W. Birmili, L. Poulain, Z. Wang, M. Merkel, B. Fahlbusch, D. van Pinxteren, H. Herrmann, and A. Wiedensohler
Atmos. Chem. Phys., 13, 6637–6646,
K. W. Fomba, K. Müller, D. van Pinxteren, and H. Herrmann
Atmos. Chem. Phys., 13, 4801–4814,
C. Mouchel-Vallon, P. Bräuer, M. Camredon, R. Valorso, S. Madronich, H. Herrmann, and B. Aumont
Atmos. Chem. Phys., 13, 1023–1037,
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Molecular-level nucleation mechanism of iodic acid and methanesulfonic acidEstimation of secondary PM2.5 in China and the United States using a multi-tracer approachTwo-way coupled meteorology and air quality models in Asia: a systematic review and meta-analysis of impacts of aerosol feedbacks on meteorology and air qualityOCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on cloudsThe pathway of impacts of aerosol direct effects on secondary inorganic aerosol formationThe impact of molecular self-organisation on the atmospheric fate of a cooking aerosol proxyThe formation and mitigation of nitrate pollution: comparison between urban and suburban environmentsImpacts of aerosol–photolysis interaction and aerosol–radiation feedback on surface-layer ozone in North China during multi-pollutant air pollution episodesReducing future air-pollution-related premature mortality over Europe by mitigating emissions from the energy sector: assessing an 80 % renewable energies scenarioThe impact of chlorine chemistry combined with heterogeneous N2O5 reactions on air quality in ChinaOH-initiated atmospheric degradation of hydroxyalkyl hydroperoxides: mechanism, kinetics, and structure–activity relationshipA predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phasesThe role of organic acids in new particle formation from methanesulfonic acid and methylamineElucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formationSecondary PM decreases significantly less than NO2 emission reductions during COVID lockdown in GermanyThe number fraction of iron-containing particles affects OH, HO2 and H2O2 budgets in the atmospheric aqueous phaseSource-resolved variability of fine particulate matter and human exposure in an urban areaThe impact of atmospheric blocking on the compounding effect of ozone pollution and temperature: a copula-based approachExploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcingModelling changes in secondary inorganic aerosol formation and nitrogen deposition in Europe from 2005 to 2030Climate impacts of emission reductions in China during 2013–2017Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activationA numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particlesPrediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility–reactivity base lumpingModelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidityLimitations in representation of physical processes prevent successful simulation of PM2.5 during KORUS-AQModeling secondary organic aerosol formation from volatile chemical productsWhy is the city's responsibility for its air pollution often underestimated? A focus on PM2.5Eurodelta multi-model simulated and observed PM trends in Europe in the period of 1990–2010Quantifying the structural uncertainty of the aerosol mixing state representation in a modal modelChanges in PM2.5 concentrations and their sources in the US from 1990 to 2010A predictive thermodynamic framework of cloud droplet activation for chemically unresolved aerosol mixtures, including surface tension, non-ideality, and bulk–surface partitioningProcess-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levelsImpacts of emission changes in China from 2010 to 2017 on domestic and intercontinental air quality and health effectExploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified ModelImproving the representation of HONO chemistry in CMAQ and examining its impact on haze over ChinaHow alkaline compounds control atmospheric aerosol particle acidityAerosol transport pathways and source attribution in China during the COVID-19 outbreakNonlinear responses of particulate nitrate to NOx emission controls in the megalopolises of ChinaInsight into PM2.5 sources by applying positive matrix factorization (PMF) at urban and rural sites of BeijingEvaluation and intercomparison of wildfire smoke forecasts from multiple modeling systems for the 2019 Williams Flats fireA comprehensive observation-based multiphase chemical model analysis of sulfur dioxide oxidations in both summer and winterPredicting gas–particle partitioning coefficients of atmospheric molecules with machine learningDevelopment of a new emission reallocation method for industrial sources in ChinaProjections of shipping emissions and the related impact on air pollution and human health in the Nordic regionA predictive model for salt nanoparticle formation using heterodimer stability calculationsUsing GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied campheneSeasonal distribution and drivers of surface fine particulate matter and organic aerosol over the Indo-Gangetic PlainIntensified modulation of winter aerosol pollution in China by El Niño with short durationForest-fire aerosol–weather feedbacks over western North America using a high-resolution, online coupled air-quality model
An Ning, Ling Liu, Lin Ji, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 6103–6114,Short summary
Iodic acid (IA) and methanesulfonic acid (MSA) were previously proved to be significant nucleation precursors in marine areas. However, the nucleation process involved in IA and MSA remains unclear. We show the enhancement of MSA on IA cluster formation and reveal the IAM-SA nucleating mechanism using a theoretical approach. This study helps to understand the clustering process in which marine sulfur- and iodine-containing species are jointly involved and its impact on new particle formation.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514,Short summary
We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Chao Gao, Aijun Xiu, Xuelei Zhang, Qingqing Tong, Hongmei Zhao, Shichun Zhang, Guangyi Yang, and Mengduo Zhang
Atmos. Chem. Phys., 22, 5265–5329,Short summary
With ever-growing applications of two-way coupled meteorology and air quality models in Asia over the past decade, this paper summarizes the current status and research focuses, as well as how aerosol effects impact model performance, meteorology, and air quality. These models enable investigations of ARI and ACI effects induced by natural and anthropogenic aerosols in Asia, which has serious air pollution problems. The current gaps and perspectives are also presented and discussed.
Susannah M. Burrows, Richard C. Easter, Xiaohong Liu, Po-Lun Ma, Hailong Wang, Scott M. Elliott, Balwinder Singh, Kai Zhang, and Philip J. Rasch
Atmos. Chem. Phys., 22, 5223–5251,Short summary
Sea spray particles are composed of a mixture of salts and organic substances from oceanic microorganisms. In prior work, our team developed an approach connecting sea spray chemistry to ocean biology, called OCEANFILMS. Here we describe its implementation within an Earth system model, E3SM. We show that simulated sea spray chemistry is consistent with observed seasonal cycles and that sunlight reflected by simulated Southern Ocean clouds increases, consistent with analysis of satellite data.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156,Short summary
Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Adam Milsom, Adam M. Squires, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 22, 4895–4907,Short summary
Cooking emissions can self-organise into nanostructured lamellar bilayers, and this can influence reaction kinetics. We developed a kinetic multi-layer model-based description of decay data we obtained from laboratory experiments of the ozonolysis of coated films of such a self-organised system, demonstrating a decreased diffusivity for both oleic acid and ozone. Nanostructure formation can thus increase the reactive half-life of oleic acid by days under typical indoor and outdoor conditions.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556,Short summary
We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 22, 4101–4116,Short summary
Aerosols can influence O3 through aerosol–radiation interactions, including aerosol–photolysis interaction (API) and aerosol–radiation feedback (ARF). The weakened photolysis rates and changed meteorological conditions reduce surface-layer O3 concentrations by up to 9.3–11.4 ppb, with API and ARF contributing 74.6 %–90.0 % and 10.0 %–25.4 % of the O3 decrease in three episodes, respectively, which indicates that API is the dominant way for O3 reduction related to aerosol–radiation interactions.
Patricia Tarín-Carrasco, Ulas Im, Camilla Geels, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 22, 3945–3965,Short summary
The evidence of the effects of atmospheric pollution (and particularly fine particulate matter, PM2.5) on human mortality is now unquestionable. Here, 895 000 annual premature deaths (PD) are estimated for the present (1991–2010), which increases to 1 540 000 in the year 2050 due to the ageing of the European population. The implementation of a mitigation scenario (80 % of the energy production in Europe from renewable sources) could lead to a decrease of over 60 000 annual PD for the year 2050.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762,Short summary
We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 ＋ Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 ＋ Cl chemistry to the impact of chlorine chemistry in China.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 3693–3711,Short summary
Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233,Short summary
Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650,Short summary
Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
Yuemeng Ji, Qiuju Shi, Xiaohui Ma, Lei Gao, Jiaxin Wang, Yixin Li, Yanpeng Gao, Guiying Li, Renyi Zhang, and Taicheng An
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Formation mechanism of secondary organic aerosol (SOA) and brown carbon (BrC) from small α-carbonyls are still unclear. Thus, the mechanisms and kinetics of aqueous-phase reaction of glyoxal were investigated using quantum chemical and kinetic rate calculations. Several essential isomeric processes were identified, including protonation to yield diol/tetrol and carbenium ions, nucleophilic addition of carbenium ions to diol/tetrol and free methylamine/ammonia.
Vigneshkumar Balamurugan, Jia Chen, Zhen Qu, Xiao Bi, and Frank N. Keutsch
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
In this study, we investigated the response of secondary pollutants to changes in precursors emissions, focusing on the formation of secondary PM, during COVID-19 lockdown period. We show that, due to the decrease in primary NOX emissions, atmospheric oxidizing capacity is increased. The night-time increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
Amina Khaled, Minghui Zhang, and Barbara Ervens
Atmos. Chem. Phys., 22, 1989–2009,Short summary
Chemical reactions with iron in clouds and aerosol form and cycle reactive oxygen species (ROS). Previous model studies assumed that all cloud droplets (particles) contain iron, while single-particle analyses showed otherwise. By means of a model, we explore the bias in predicted ROS budgets by distributing a given iron mass to either all or only a few droplets (particles). Implications for oxidation potential, radical loss and iron oxidation state are discussed.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027,Short summary
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.
Noelia Otero, Oscar E. Jurado, Tim Butler, and Henning W. Rust
Atmos. Chem. Phys., 22, 1905–1919,Short summary
Surface ozone and temperature are strongly dependent and their extremes might be exacerbated by underlying climatological drivers, such as atmospheric blocking. Using an observational data set, we measure the dependence structure between ozone and temperature under the influence of atmospheric blocking. Blocks enhanced the probability of occurrence of compound ozone and temperature extremes over northwestern and central Europe, leading to greater health risks.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573,Short summary
Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Jan Eiof Jonson, Hilde Fagerli, Thomas Scheuschner, and Svetlana Tsyro
Atmos. Chem. Phys., 22, 1311–1331,Short summary
Ammonia emissions are expected to decrease less than SOx and NOx emissions between 2005 and 2030. As the formation of PM2.5 particles from ammonia depends on the ratio between ammonia on one hand and sulfate (from SOx) and HNO3 (from NOx) on the other hand, the efficiency of particle formation from ammonia is decreasing. Depositions of reduced nitrogen are decreasing much less than oxidized nitrogen. The critical loads for nitrogen deposition will also be exceeded in much of Europe in 2030.
Jiyuan Gao, Yang Yang, Hailong Wang, Pinya Wang, Huimin Li, Mengyun Li, Lili Ren, Xu Yue, and Hong Liao
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The aerosol decline produced a 0.09 ± 0.10 °C warming estimated in this study and the increase of ozone in the lower troposphere accelerated the warming, leading to a total 0.16 ± 0.15 °C temperature increase in eastern China during 2013–2017. Residential emissions reductions led to a cooling effect because a substantial decrease in light-absorbing aerosols.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013,Short summary
Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Isabelle Steinke, Paul J. DeMott, Grant B. Deane, Thomas C. J. Hill, Mathew Maltrud, Aishwarya Raman, and Susannah M. Burrows
Atmos. Chem. Phys., 22, 847–859,Short summary
Over the oceans, sea spray aerosol is an important source of particles that may initiate the formation of cloud ice, which then has implications for the radiative properties of marine clouds. In our study, we focus on marine biogenic particles that are emitted episodically and develop a numerical framework to describe these emissions. We find that further cloud-resolving model studies and targeted observations are needed to fully understand the climate impacts from marine biogenic particles.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 22, 625–639,Short summary
The gasoline SOA formation potential was simulated by using the UNIPAR model coupled with CB6r3 mechanism under varying NOx levels, aerosol acidity, humidity, temperature, and concentrations of aqueous salts and gasoline vapor. The model predicts SOA formation via multiphase reactions in the absence of wall bias. The simulation shows that both heterogeneous reactions in the aqueous phase and the implementation of model parameters corrected for GWP are critical to accurately predict SOA mass.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244,Short summary
We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The 2016 Korea United States-Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261,Short summary
Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212,Short summary
Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741,Short summary
Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
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,Short summary
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.
Nønne L. Prisle
Atmos. Chem. Phys., 21, 16387–16411,Short summary
A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of droplet growth and activation with considerations of surface partitioning, surface tension, and non-ideal water activity for chemically complex and unresolved surface active aerosol mixtures, including actual atmospheric samples. The model is used to calculate cloud condensation nuclei (CCN) activity of aerosol particles comprising strongly surface-active model atmospheric humic-like substances (HULIS).
Ruqian Miao, Qi Chen, Manish Shrivastava, Youfan Chen, Lin Zhang, Jianlin Hu, Yan Zheng, and Keren Liao
Atmos. Chem. Phys., 21, 16183–16201,Short summary
We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys., 21, 16051–16065,Short summary
In this study, we use a global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927,Short summary
Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys., 21, 15809–15826,Short summary
Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001,Short summary
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).
Lili Ren, Yang Yang, Hailong Wang, Pinya Wang, Lei Chen, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 21, 15431–15445,Short summary
Due to the COVID-19 pandemic, human activities were strictly restricted in China. Even though anthropogenic aerosol emissions largely decreased, haze events still occurred. Our results shows that PM2.5 over the North China Plain is largely contributed by local sources. For other regions in China, PM2.5 is largely contributed from nonlocal sources. As emission reduction is a future goal, aerosol long-range transport and unfavorable meteorology are increasingly important to air quality.
Mengmeng Li, Zihan Zhang, Quan Yao, Tijian Wang, Min Xie, Shu Li, Bingliang Zhuang, and Yong Han
Atmos. Chem. Phys., 21, 15135–15152,Short summary
We establish the nonlinear responses between nitrate and NOx in China. Reduction of NOx results in linearly lower nitrate in summer–autumn whereas an increase of winter nitrate until an inflexion point at 40–50 % reduction due to the excess oxidants. NH3 and VOCs are effective in controlling nitrate pollution, whereas decreasing the SO2 and NOx emissions may have counterintuitive effects on nitrate aerosols. This paper helps understand the nonlinear aerosol and photochemistry feedback.
Deepchandra Srivastava, Jingsha Xu, Tuan V. Vu, Di Liu, Linjie Li, Pingqing Fu, Siqi Hou, Natalia Moreno Palmerola, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 21, 14703–14724,Short summary
This study presents the source apportionment of PM2.5 performed by positive matrix factorization (PMF) at urban and rural sites in Beijing. These factors are interpreted as traffic emissions, biomass burning, road and soil dust, coal and oil combustion, and secondary inorganics. PMF failed to resolve some sources identified by CMB and AMS and appears to overestimate the dust sources. Comparison with earlier PMF studies from the Beijing area highlights inconsistent findings using this method.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469,Short summary
Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727,Short summary
Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246,Short summary
The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Yun Fat Lam, Chi Chiu Cheung, Xuguo Zhang, Joshua S. Fu, and Jimmy Chi Hung Fung
Atmos. Chem. Phys., 21, 12895–12908,Short summary
In recent years, air pollution forecasting has become an important municipal service of the government. In this study, a new spatial allocation method based on satellite remote sensing and GIS techniques was developed to address the spatial deficiency of industrial source emissions in China, providing a substantial improvement on NO2 and PM2.5 forecast for the Pearl River Delta/Greater Bay Area.
Camilla Geels, Morten Winther, Camilla Andersson, Jukka-Pekka Jalkanen, Jørgen Brandt, Lise M. Frohn, Ulas Im, Wing Leung, and Jesper H. Christensen
Atmos. Chem. Phys., 21, 12495–12519,Short summary
In this study, we set up new shipping emissions scenarios and use two chemistry transport models and a health assessment model to assess the development of air quality and related health impacts in the Nordic region. Shipping alone is associated with about 850 premature deaths during present-day conditions, decreasing to approximately 550–600 cases in the 2050 scenarios.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys., 21, 11637–11654,Short summary
We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487,Short summary
This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
Caterina Mogno, Paul I. Palmer, Christoph Knote, Fei Yao, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 10881–10909,Short summary
We use a 3-D atmospheric chemistry model to investigate how seasonal emissions sources and meteorological conditions affect the surface distribution of fine particulate matter (PM2.5) and organic aerosol (OA) over the Indo-Gangetic Plain. We find that all seasonal mean values of PM2.5 still exceed safe air quality levels, with human emissions contributing to PM2.5 all year round, open fires during post- and pre-monsoon, and biogenic emissions during monsoon. OA contributes up to 30 % to PM2.5.
Liangying Zeng, Yang Yang, Hailong Wang, Jing Wang, Jing Li, Lili Ren, Huimin Li, Yang Zhou, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 21, 10745–10761,Short summary
Using an aerosol–climate model, the impacts of El Niño with different durations on aerosols in China are examined. The modulation on aerosol concentrations and haze days by short-duration El Niño events is 2–3 times more than that by long-duration El Niño events in China. The frequency of short-duration El Niño has been increasing significantly in recent decades, suggesting that El Niño events have exerted increasingly intense modulation on aerosol pollution in China over the past few decades.
Paul A. Makar, Ayodeji Akingunola, Jack Chen, Balbir Pabla, Wanmin Gong, Craig Stroud, Christopher Sioris, Kerry Anderson, Philip Cheung, Junhua Zhang, and Jason Milbrandt
Atmos. Chem. Phys., 21, 10557–10587,Short summary
We have examined the effects of airborne particles on absorption and scattering of incoming sunlight by the particles themselves via cloud formation. We used an advanced, combined high-resolution weather forecast and chemical transport computer model, for western North America, and simulations with and without the connections between particles and weather enabled. Feedbacks improved weather and air pollution forecasts and changed cloud behaviour and forest-fire pollutant amount and height.
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In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are performed. The investigations aim at assessing the impact of a detailed treatment of non-ideality in multiphase models dealing with aqueous aerosol chemistry. The model studies demonstrate that the inclusion of non-ideality considerably affects the multiphase chemical processing of transition metal ions, oxidants, and related chemical subsystems such as organic chemistry in aqueous aerosols.
In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are...