Articles | Volume 21, issue 8
https://doi.org/10.5194/acp-21-6175-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-6175-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
23 Apr 2021
Research article |
| 23 Apr 2021
| 23 Apr 2021
Non-equilibrium interplay between gas–particle partitioning and multiphase chemical reactions of semi-volatile compounds: mechanistic insights and practical implications for atmospheric modeling of polycyclic aromatic hydrocarbons
Jake Wilson
Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Ulrich Pöschl
Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Department of Chemistry, University of California, Irvine, CA, USA
Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Related authors
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
Short summary
Short summary
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.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
Short summary
Short summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Pourya Shahpoury, Tom Harner, Gerhard Lammel, Steven Lelieveld, Haijie Tong, and Jake Wilson
Atmos. Meas. Tech., 12, 6529–6539, https://doi.org/10.5194/amt-12-6529-2019, https://doi.org/10.5194/amt-12-6529-2019, 2019
Céline Degrendele, Jake Wilson, Petr Kukučka, Jana Klánová, and Gerhard Lammel
Atmos. Chem. Phys., 18, 12877–12890, https://doi.org/10.5194/acp-18-12877-2018, https://doi.org/10.5194/acp-18-12877-2018, 2018
Short summary
Short summary
Polybrominated diphenyl ethers (PBDEs) are persistent organic pollutants present in the global environment. This study, reporting on their atmospheric behaviour in central Europe, has shown that none of the three investigated gas–particle partitioning models provided a satisfactory prediction, highlighting the need for a model that is universally applicable. Finally, this study tends to show that the debromination from high to low brominated congeners, enhanced by photolysis, is important.
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
Short summary
Short summary
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.
Florian Wieland, Nadine Bothen, Ralph Schwidetzky, Teresa M. Seifried, Paul Bieber, Ulrich Pöschl, Konrad Meister, Mischa Bonn, Janine Fröhlich-Nowoisky, and Hinrich Grothe
EGUsphere, https://doi.org/10.5194/egusphere-2024-752, https://doi.org/10.5194/egusphere-2024-752, 2024
Short summary
Short summary
Betula pendula is a widespread birch tree species containing ice nucleation agents that can trigger the freezing of cloud droplets, and thereby alter the evolution of clouds. Our study identifies three distinct ice-nucleating macromolecules (INMs) and aggregates of varying size that can nucleate ice at temperatures of up to -5.4 °C. Our findings suggest that these vegetation-derived particles may influence atmospheric processes, weather, and climate stronger than previously thought.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
Short summary
Short summary
Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Gabriela R. Unfer, Luiz A. T. Machado, Paulo Artaxo, Marco A. Franco, Leslie A. Kremper, Mira L. Pöhlker, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 3869–3882, https://doi.org/10.5194/acp-24-3869-2024, https://doi.org/10.5194/acp-24-3869-2024, 2024
Short summary
Short summary
Amazonian aerosols and their interactions with precipitation were studied by understanding them in a 3D space based on three parameters that characterize the concentration and size distribution of aerosols. The results showed characteristic arrangements regarding seasonal and diurnal cycles, as well as when interacting with precipitation. The use of this 3D space appears to be a promising tool for aerosol population analysis and for model validation and parameterization.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botia, Hella Van Asperen, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosa Ferreira, Hartwig Harder, Sam Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira 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
EGUsphere, https://doi.org/10.5194/egusphere-2023-2901, https://doi.org/10.5194/egusphere-2023-2901, 2024
Short summary
Short summary
Composite analysis of the gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. This analysis helps 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
Marco A. Franco, Rafael Valiati, Bruna A. Holanda, Bruno B. Meller, Leslie A. Kremper, Luciana V. Rizzo, Samara Carbone, Fernando G. Morais, Janaína P. Nascimento, Meinrat O. Andreae, Micael A. Cecchini, Luiz A. T. Machado, Milena Ponczek, Ulrich Pöschl, David Walter, Christopher Pöhlker, and Paulo Artaxo
EGUsphere, https://doi.org/10.5194/egusphere-2023-2607, https://doi.org/10.5194/egusphere-2023-2607, 2024
Short summary
Short summary
The Amazon wet season atmosphere was studied at the Amazon Tall Tower Observatory site, revealing vertical variations (between 60 and 325 m height) in natural aerosols. Daytime mixing contrasted with nighttime stratification, with distinct rain-induced changes in aerosol populations. Notably, optical properties recovery at higher levels was faster, while near-canopy aerosols showed higher scattering efficiency. These findings enhance our understanding of aerosol impacts on climate dynamics.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
Short summary
Short summary
Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
Short summary
Short summary
D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
Short summary
Short summary
Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Najin Kim, Hang Su, Nan Ma, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 16, 2771–2780, https://doi.org/10.5194/amt-16-2771-2023, https://doi.org/10.5194/amt-16-2771-2023, 2023
Short summary
Short summary
We propose a multiple-charging correction algorithm for a broad-supersaturation scanning cloud condensation nuclei (BS2-CCN) system which can obtain high time-resolution aerosol hygroscopicity and CCN activity. The correction algorithm aims at deriving the activation fraction's true value for each particle size. The meaningful differences between corrected and original κ values (single hygroscopicity parameter) emphasize the correction algorithm's importance for ambient aerosol measurement.
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
Short summary
Short summary
We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
Short summary
Short summary
Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
Short summary
Short summary
This paper presents atmospheric particle chemical composition and measurements of aerosol water uptake properties collected at Ragged Point, Barbados, during the winter of 2020. The result of this study indicates the importance of small African smoke particles for cloud droplet formation in the tropical North Atlantic and highlights the large spatial and temporal pervasiveness of smoke over the Atlantic Ocean.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
Short summary
Short summary
The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
Short summary
Short summary
Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Guo Li, Hang Su, Meng Li, Uwe Kuhn, Guangjie Zheng, Lei Han, Fengxia Bao, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 15, 6433–6446, https://doi.org/10.5194/amt-15-6433-2022, https://doi.org/10.5194/amt-15-6433-2022, 2022
Short summary
Short summary
A large fraction of previous work using dynamic flow chambers was to quantify gas exchange in terms of flux or deposition/emission rate. Here, we extended the usage of this technique to examine uptake kinetics on sample surfaces. The good performance of the chamber system was validated. This technique can be further used for liquid samples and real atmospheric aerosol samples without complicated coating procedures, which complements the existing techniques in atmospheric kinetic studies.
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
Short summary
Short summary
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.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
Short summary
Short summary
The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
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
Short summary
Short summary
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
Short summary
Short summary
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 %.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
Short summary
Short summary
EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Marco A. Franco, Florian Ditas, Leslie A. Kremper, Luiz A. T. Machado, Meinrat O. Andreae, Alessandro Araújo, Henrique M. J. Barbosa, Joel F. de Brito, Samara Carbone, Bruna A. Holanda, Fernando G. Morais, Janaína P. Nascimento, Mira L. Pöhlker, Luciana V. Rizzo, Marta Sá, Jorge Saturno, David Walter, Stefan Wolff, Ulrich Pöschl, Paulo Artaxo, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 3469–3492, https://doi.org/10.5194/acp-22-3469-2022, https://doi.org/10.5194/acp-22-3469-2022, 2022
Short summary
Short summary
In Central Amazonia, new particle formation in the planetary boundary layer is rare. Instead, there is the appearance of sub-50 nm aerosols with diameters larger than about 20 nm that eventually grow to cloud condensation nuclei size range. Here, 254 growth events were characterized which have higher predominance in the wet season. About 70 % of them showed direct relation to convective downdrafts, while 30 % occurred partly under clear-sky conditions, evidencing still unknown particle sources.
Kai Tang, Beatriz Sánchez-Parra, Petya Yordanova, Jörn Wehking, Anna T. Backes, Daniel A. Pickersgill, Stefanie Maier, Jean Sciare, Ulrich Pöschl, Bettina Weber, and Janine Fröhlich-Nowoisky
Biogeosciences, 19, 71–91, https://doi.org/10.5194/bg-19-71-2022, https://doi.org/10.5194/bg-19-71-2022, 2022
Short summary
Short summary
Metagenomic sequencing and freezing experiments of aerosol samples collected on Cyprus revealed rain-related short-term changes of bioaerosol and ice nuclei composition. Filtration experiments showed a rain-related enhancement of biological ice nuclei > 5 µm and < 0.1 µm. The observed effects of rainfall on the composition of atmospheric bioaerosols and ice nuclei may influence the hydrological cycle as well as the health effects of air particulate matter (pathogens, allergens).
Luiz A. T. Machado, Marco A. Franco, Leslie A. Kremper, Florian Ditas, Meinrat O. Andreae, Paulo Artaxo, Micael A. Cecchini, Bruna A. Holanda, Mira L. Pöhlker, Ivan Saraiva, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 21, 18065–18086, https://doi.org/10.5194/acp-21-18065-2021, https://doi.org/10.5194/acp-21-18065-2021, 2021
Short summary
Short summary
Several studies evaluate aerosol–cloud interactions, but only a few attempted to describe how clouds modify aerosol properties. This study evaluates the effect of weather events on the particle size distribution at the ATTO, combining remote sensing and in situ data. Ultrafine, Aitken and accumulation particles modes have different behaviors for the diurnal cycle and for rainfall events. This study opens up new scientific questions that need to be pursued in detail in new field campaigns.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
Short summary
Short summary
Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Najin Kim, Yafang Cheng, Nan Ma, Mira L. Pöhlker, Thomas Klimach, Thomas F. Mentel, Ovid O. Krüger, Ulrich Pöschl, and Hang Su
Atmos. Meas. Tech., 14, 6991–7005, https://doi.org/10.5194/amt-14-6991-2021, https://doi.org/10.5194/amt-14-6991-2021, 2021
Short summary
Short summary
A broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of supersaturation simultaneously, can measure a broad range of CCN activity distribution with a high time resolution. We describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve. Intercomparison experiments between typical DMA-CCN and BS2-CCN measurements to evaluate the BS2-CCN system showed high correlation and good agreement.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
Short summary
Short summary
Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
Short summary
Short summary
Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
Bjorn Stevens, Sandrine Bony, David Farrell, Felix Ament, Alan Blyth, Christopher Fairall, Johannes Karstensen, Patricia K. Quinn, Sabrina Speich, Claudia Acquistapace, Franziska Aemisegger, Anna Lea Albright, Hugo Bellenger, Eberhard Bodenschatz, Kathy-Ann Caesar, Rebecca Chewitt-Lucas, Gijs de Boer, Julien Delanoë, Leif Denby, Florian Ewald, Benjamin Fildier, Marvin Forde, Geet George, Silke Gross, Martin Hagen, Andrea Hausold, Karen J. Heywood, Lutz Hirsch, Marek Jacob, Friedhelm Jansen, Stefan Kinne, Daniel Klocke, Tobias Kölling, Heike Konow, Marie Lothon, Wiebke Mohr, Ann Kristin Naumann, Louise Nuijens, Léa Olivier, Robert Pincus, Mira Pöhlker, Gilles Reverdin, Gregory Roberts, Sabrina Schnitt, Hauke Schulz, A. Pier Siebesma, Claudia Christine Stephan, Peter Sullivan, Ludovic Touzé-Peiffer, Jessica Vial, Raphaela Vogel, Paquita Zuidema, Nicola Alexander, Lyndon Alves, Sophian Arixi, Hamish Asmath, Gholamhossein Bagheri, Katharina Baier, Adriana Bailey, Dariusz Baranowski, Alexandre Baron, Sébastien Barrau, Paul A. Barrett, Frédéric Batier, Andreas Behrendt, Arne Bendinger, Florent Beucher, Sebastien Bigorre, Edmund Blades, Peter Blossey, Olivier Bock, Steven Böing, Pierre Bosser, Denis Bourras, Pascale Bouruet-Aubertot, Keith Bower, Pierre Branellec, Hubert Branger, Michal Brennek, Alan Brewer, Pierre-Etienne Brilouet, Björn Brügmann, Stefan A. Buehler, Elmo Burke, Ralph Burton, Radiance Calmer, Jean-Christophe Canonici, Xavier Carton, Gregory Cato Jr., Jude Andre Charles, Patrick Chazette, Yanxu Chen, Michal T. Chilinski, Thomas Choularton, Patrick Chuang, Shamal Clarke, Hugh Coe, Céline Cornet, Pierre Coutris, Fleur Couvreux, Susanne Crewell, Timothy Cronin, Zhiqiang Cui, Yannis Cuypers, Alton Daley, Gillian M. Damerell, Thibaut Dauhut, Hartwig Deneke, Jean-Philippe Desbios, Steffen Dörner, Sebastian Donner, Vincent Douet, Kyla Drushka, Marina Dütsch, André Ehrlich, Kerry Emanuel, Alexandros Emmanouilidis, Jean-Claude Etienne, Sheryl Etienne-Leblanc, Ghislain Faure, Graham Feingold, Luca Ferrero, Andreas Fix, Cyrille Flamant, Piotr Jacek Flatau, Gregory R. Foltz, Linda Forster, Iulian Furtuna, Alan Gadian, Joseph Galewsky, Martin Gallagher, Peter Gallimore, Cassandra Gaston, Chelle Gentemann, Nicolas Geyskens, Andreas Giez, John Gollop, Isabelle Gouirand, Christophe Gourbeyre, Dörte de Graaf, Geiske E. de Groot, Robert Grosz, Johannes Güttler, Manuel Gutleben, Kashawn Hall, George Harris, Kevin C. Helfer, Dean Henze, Calvert Herbert, Bruna Holanda, Antonio Ibanez-Landeta, Janet Intrieri, Suneil Iyer, Fabrice Julien, Heike Kalesse, Jan Kazil, Alexander Kellman, Abiel T. Kidane, Ulrike Kirchner, Marcus Klingebiel, Mareike Körner, Leslie Ann Kremper, Jan Kretzschmar, Ovid Krüger, Wojciech Kumala, Armin Kurz, Pierre L'Hégaret, Matthieu Labaste, Tom Lachlan-Cope, Arlene Laing, Peter Landschützer, Theresa Lang, Diego Lange, Ingo Lange, Clément Laplace, Gauke Lavik, Rémi Laxenaire, Caroline Le Bihan, Mason Leandro, Nathalie Lefevre, Marius Lena, Donald Lenschow, Qiang Li, Gary Lloyd, Sebastian Los, Niccolò Losi, Oscar Lovell, Christopher Luneau, Przemyslaw Makuch, Szymon Malinowski, Gaston Manta, Eleni Marinou, Nicholas Marsden, Sebastien Masson, Nicolas Maury, Bernhard Mayer, Margarette Mayers-Als, Christophe Mazel, Wayne McGeary, James C. McWilliams, Mario Mech, Melina Mehlmann, Agostino Niyonkuru Meroni, Theresa Mieslinger, Andreas Minikin, Peter Minnett, Gregor Möller, Yanmichel Morfa Avalos, Caroline Muller, Ionela Musat, Anna Napoli, Almuth Neuberger, Christophe Noisel, David Noone, Freja Nordsiek, Jakub L. Nowak, Lothar Oswald, Douglas J. Parker, Carolyn Peck, Renaud Person, Miriam Philippi, Albert Plueddemann, Christopher Pöhlker, Veronika Pörtge, Ulrich Pöschl, Lawrence Pologne, Michał Posyniak, Marc Prange, Estefanía Quiñones Meléndez, Jule Radtke, Karim Ramage, Jens Reimann, Lionel Renault, Klaus Reus, Ashford Reyes, Joachim Ribbe, Maximilian Ringel, Markus Ritschel, Cesar B. Rocha, Nicolas Rochetin, Johannes Röttenbacher, Callum Rollo, Haley Royer, Pauline Sadoulet, Leo Saffin, Sanola Sandiford, Irina Sandu, Michael Schäfer, Vera Schemann, Imke Schirmacher, Oliver Schlenczek, Jerome Schmidt, Marcel Schröder, Alfons Schwarzenboeck, Andrea Sealy, Christoph J. Senff, Ilya Serikov, Samkeyat Shohan, Elizabeth Siddle, Alexander Smirnov, Florian Späth, Branden Spooner, M. Katharina Stolla, Wojciech Szkółka, Simon P. de Szoeke, Stéphane Tarot, Eleni Tetoni, Elizabeth Thompson, Jim Thomson, Lorenzo Tomassini, Julien Totems, Alma Anna Ubele, Leonie Villiger, Jan von Arx, Thomas Wagner, Andi Walther, Ben Webber, Manfred Wendisch, Shanice Whitehall, Anton Wiltshire, Allison A. Wing, Martin Wirth, Jonathan Wiskandt, Kevin Wolf, Ludwig Worbes, Ethan Wright, Volker Wulfmeyer, Shanea Young, Chidong Zhang, Dongxiao Zhang, Florian Ziemen, Tobias Zinner, and Martin Zöger
Earth Syst. Sci. Data, 13, 4067–4119, https://doi.org/10.5194/essd-13-4067-2021, https://doi.org/10.5194/essd-13-4067-2021, 2021
Short summary
Short summary
The EUREC4A field campaign, designed to test hypothesized mechanisms by which clouds respond to warming and benchmark next-generation Earth-system models, is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. It was the first campaign that attempted to characterize the full range of processes and scales influencing trade wind clouds.
Mira L. Pöhlker, Minghui Zhang, Ramon Campos Braga, Ovid O. Krüger, Ulrich Pöschl, and Barbara Ervens
Atmos. Chem. Phys., 21, 11723–11740, https://doi.org/10.5194/acp-21-11723-2021, https://doi.org/10.5194/acp-21-11723-2021, 2021
Short summary
Short summary
Clouds cool our atmosphere. The role of small aerosol particles in affecting them represents one of the largest uncertainties in current estimates of climate change. Traditionally it is assumed that cloud droplets only form particles of diameters ~ 100 nm (
accumulation mode). Previous studies suggest that this can also occur in smaller particles (
Aitken mode). Our study provides a general framework to estimate under which aerosol and cloud conditions Aitken mode particles affect clouds.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
Short summary
Short summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
Short summary
Short summary
We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Eugene F. Mikhailov, Mira L. Pöhlker, Kathrin Reinmuth-Selzle, Sergey S. Vlasenko, Ovid O. Krüger, Janine Fröhlich-Nowoisky, Christopher Pöhlker, Olga A. Ivanova, Alexey A. Kiselev, Leslie A. Kremper, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 6999–7022, https://doi.org/10.5194/acp-21-6999-2021, https://doi.org/10.5194/acp-21-6999-2021, 2021
Short summary
Short summary
Subpollen particles are a relatively new subset of atmospheric aerosol particles. When pollen grains rupture, they release cytoplasmic fragments known as subpollen particles (SPPs). We found that SPPs, containing a broad spectrum of biopolymers and hydrocarbons, exhibit abnormally high water uptake. This effect may influence the life cycle of SPPs and the related direct and indirect impacts on radiation budget as well as reinforce their allergic potential.
Patricia K. Quinn, Elizabeth J. Thompson, Derek J. Coffman, Sunil Baidar, Ludovic Bariteau, Timothy S. Bates, Sebastien Bigorre, Alan Brewer, Gijs de Boer, Simon P. de Szoeke, Kyla Drushka, Gregory R. Foltz, Janet Intrieri, Suneil Iyer, Chris W. Fairall, Cassandra J. Gaston, Friedhelm Jansen, James E. Johnson, Ovid O. Krüger, Richard D. Marchbanks, Kenneth P. Moran, David Noone, Sergio Pezoa, Robert Pincus, Albert J. Plueddemann, Mira L. Pöhlker, Ulrich Pöschl, Estefania Quinones Melendez, Haley M. Royer, Malgorzata Szczodrak, Jim Thomson, Lucia M. Upchurch, Chidong Zhang, Dongxiao Zhang, and Paquita Zuidema
Earth Syst. Sci. Data, 13, 1759–1790, https://doi.org/10.5194/essd-13-1759-2021, https://doi.org/10.5194/essd-13-1759-2021, 2021
Short summary
Short summary
ATOMIC took place in the northwestern tropical Atlantic during January and February of 2020 to gather information on shallow atmospheric convection, the effects of aerosols and clouds on the ocean surface energy budget, and mesoscale oceanic processes. Measurements made from the NOAA RV Ronald H. Brown and assets it deployed (instrumented mooring and uncrewed seagoing vehicles) are described herein to advance widespread use of the data by the ATOMIC and broader research communities.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
Short summary
Short summary
Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Chuchu Chen, Xiaoxiang Wang, Kurt Binder, Mohammad Mehdi Ghahremanpour, David van der Spoel, Ulrich Pöschl, Hang Su, and Yafang Cheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1329, https://doi.org/10.5194/acp-2020-1329, 2021
Publication in ACP not foreseen
Short summary
Short summary
Size dependence of succinic acid solvation in the nanoparticles is investigated based on the molecular dynamics (MD) simulation and energetic analysis. The results show a stronger surface preference and a weaker internal bulk volume solvation of succinic acid in the smaller droplets, which may explain the previously observed size-dependent phase-state of aerosol nanoparticles containing organic molecules, fundamentally promoting a better understanding of atmospheric aerosols.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
Short summary
Short summary
Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
Short summary
Short summary
This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Guo Li, Hang Su, Nan Ma, Guangjie Zheng, Uwe Kuhn, Meng Li, Thomas Klimach, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 13, 6053–6065, https://doi.org/10.5194/amt-13-6053-2020, https://doi.org/10.5194/amt-13-6053-2020, 2020
Short summary
Short summary
Aerosol acidity plays an important role in regulating the chemistry, health, and ecological effect of aerosol particles. However, a direct measurement of aerosol pH is very challenging because of its fast transition and equilibrium with adjacent environments. Therefore, most early studies have to use modeled pH, resulting in intensive debates about model uncertainties. Here we developed an optimized approach to measure aerosol pH by using pH-indicator papers combined with RGB-based colorimetry.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
Short summary
Short summary
This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Ting Lei, Nan Ma, Juan Hong, Thomas Tuch, Xin Wang, Zhibin Wang, Mira Pöhlker, Maofa Ge, Weigang Wang, Eugene Mikhailov, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Alfred Wiedensohler, and Yafang Cheng
Atmos. Meas. Tech., 13, 5551–5567, https://doi.org/10.5194/amt-13-5551-2020, https://doi.org/10.5194/amt-13-5551-2020, 2020
Short summary
Short summary
We present the design of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. We further introduce comprehensive methods for system calibration and validation of the performance of the system. We then study the size dependence of the deliquescence and the efflorescence of aerosol nanoparticles for sizes down to 6 nm.
Wei Tao, Hang Su, Guangjie Zheng, Jiandong Wang, Chao Wei, Lixia Liu, Nan Ma, Meng Li, Qiang Zhang, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 20, 11729–11746, https://doi.org/10.5194/acp-20-11729-2020, https://doi.org/10.5194/acp-20-11729-2020, 2020
Short summary
Short summary
We simulated the thermodynamic and multiphase reactions in aerosol water during a wintertime haze event over the North China Plain. It was found that aerosol pH exhibited a strong spatiotemporal variability, and multiple oxidation pathways were predominant for particulate sulfate formation in different locations. Sensitivity tests further showed that ammonia, crustal particles, and dissolved transition metal ions were important factors for multiphase chemistry during haze episodes.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
Short summary
Short summary
Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Meas. Tech., 13, 3717–3729, https://doi.org/10.5194/amt-13-3717-2020, https://doi.org/10.5194/amt-13-3717-2020, 2020
Short summary
Short summary
A gas flow system coupled with a microreactor for X-ray microspectroscopy is presented. Its core objective is to mimic the atmospheric processing of aerosol particles under laboratory conditions in a controlled gas-phase environment and allow in situ observations with high spatial and chemical resolution. We here emphasize its analytical capabilities and show initial results from hydration–dehydration experiments and the observation of water ice at low temperature and high relative humidity.
Bruna A. Holanda, Mira L. Pöhlker, David Walter, Jorge Saturno, Matthias Sörgel, Jeannine Ditas, Florian Ditas, Christiane Schulz, Marco Aurélio Franco, Qiaoqiao Wang, Tobias Donth, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Ramon Braga, Joel Brito, Yafang Cheng, Maximilian Dollner, Johannes W. Kaiser, Thomas Klimach, Christoph Knote, Ovid O. Krüger, Daniel Fütterer, Jošt V. Lavrič, Nan Ma, Luiz A. T. Machado, Jing Ming, Fernando G. Morais, Hauke Paulsen, Daniel Sauer, Hans Schlager, Johannes Schneider, Hang Su, Bernadett Weinzierl, Adrian Walser, Manfred Wendisch, Helmut Ziereis, Martin Zöger, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 20, 4757–4785, https://doi.org/10.5194/acp-20-4757-2020, https://doi.org/10.5194/acp-20-4757-2020, 2020
Short summary
Short summary
Biomass burning smoke from African savanna and grassland is transported across the South Atlantic Ocean in defined layers within the free troposphere. The combination of in situ aircraft and ground-based measurements aided by satellite observations showed that these layers are transported into the Amazon Basin during the early dry season. The influx of aged smoke, enriched in black carbon and cloud condensation nuclei, has important implications for the Amazonian aerosol and cloud cycling.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
Short summary
Short summary
In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
Pascal Polonik, Christoph Knote, Tobias Zinner, Florian Ewald, Tobias Kölling, Bernhard Mayer, Meinrat O. Andreae, Tina Jurkat-Witschas, Thomas Klimach, Christoph Mahnke, Sergej Molleker, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Ralf Weigel, and Manfred Wendisch
Atmos. Chem. Phys., 20, 1591–1605, https://doi.org/10.5194/acp-20-1591-2020, https://doi.org/10.5194/acp-20-1591-2020, 2020
Short summary
Short summary
A realistic representation of cloud–aerosol interactions is central to accurate climate projections. Here we combine observations collected during the ACRIDICON-CHUVA campaign with chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysics. We find an upper limit for the model sensitivity on cloud condensation nuclei concentrations well below the levels reached during the burning season in the Amazon Basin.
Nina Löbs, Cybelli G. G. Barbosa, Sebastian Brill, David Walter, Florian Ditas, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Ricardo H. M. Godoi, Stefan Wolff, Meike Piepenbring, Jürgen Kesselmeier, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, Christopher Pöhlker, and Bettina Weber
Atmos. Meas. Tech., 13, 153–164, https://doi.org/10.5194/amt-13-153-2020, https://doi.org/10.5194/amt-13-153-2020, 2020
Short summary
Short summary
Bioaerosols are considered to play a relevant role in atmospheric processes, but their sources, properties, and spatiotemporal distribution in the atmosphere are not yet well characterized. Measurement data on the release of fungal spores under natural conditions are also sparse. Here, we present an experimental approach to analyze and quantify the spore release from fungi and other spore-producing organisms under natural and laboratory conditions.
Pourya Shahpoury, Tom Harner, Gerhard Lammel, Steven Lelieveld, Haijie Tong, and Jake Wilson
Atmos. Meas. Tech., 12, 6529–6539, https://doi.org/10.5194/amt-12-6529-2019, https://doi.org/10.5194/amt-12-6529-2019, 2019
Anna T. Kunert, Mira L. Pöhlker, Kai Tang, Carola S. Krevert, Carsten Wieder, Kai R. Speth, Linda E. Hanson, Cindy E. Morris, David G. Schmale III, Ulrich Pöschl, and Janine Fröhlich-Nowoisky
Biogeosciences, 16, 4647–4659, https://doi.org/10.5194/bg-16-4647-2019, https://doi.org/10.5194/bg-16-4647-2019, 2019
Short summary
Short summary
A screening of more than 100 strains from 65 different species revealed that the ice nucleation activity within the fungal genus Fusarium is more widespread than previously assumed. Filtration experiments suggest that the single cell-free Fusarium IN is smaller than 100 kDa (~ 6 nm) and that aggregates can be formed in solution. Exposure experiments, freeze–thaw cycles, and long-term storage tests demonstrate a high stability of Fusarium IN under atmospherically relevant conditions.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Meng Li, Hang Su, Guo Li, Nan Ma, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 19, 10981–11011, https://doi.org/10.5194/acp-19-10981-2019, https://doi.org/10.5194/acp-19-10981-2019, 2019
Short summary
Short summary
Aerosols and the ground provide two kinds of surfaces for multiphase reactions in the planetary boundary layer. However, the relative importance of these two surfaces for gas uptake has not been quantified. We compare the uptake fluxes of aerosols and the ground surface for reactive trace gases under various conditions. More studies regarding O3 uptake on liquid organic aerosols and H2O2 uptakes on various aerosols are needed considering their potential important roles in atmospheric chemistry.
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
Short summary
Short summary
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.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
Short summary
Short summary
We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Christopher Pöhlker, David Walter, Hauke Paulsen, Tobias Könemann, Emilio Rodríguez-Caballero, Daniel Moran-Zuloaga, Joel Brito, Samara Carbone, Céline Degrendele, Viviane R. Després, Florian Ditas, Bruna A. Holanda, Johannes W. Kaiser, Gerhard Lammel, Jošt V. Lavrič, Jing Ming, Daniel Pickersgill, Mira L. Pöhlker, Maria Praß, Nina Löbs, Jorge Saturno, Matthias Sörgel, Qiaoqiao Wang, Bettina Weber, Stefan Wolff, Paulo Artaxo, Ulrich Pöschl, and Meinrat O. Andreae
Atmos. Chem. Phys., 19, 8425–8470, https://doi.org/10.5194/acp-19-8425-2019, https://doi.org/10.5194/acp-19-8425-2019, 2019
Short summary
Short summary
The Amazon Tall Tower Observatory (ATTO) has been established to monitor the rain forest's biosphere–atmosphere exchange, which experiences the combined pressures from human-made deforestation and progressing climate change. This work is meant to be a reference study, which characterizes various geospatial properties of the ATTO footprint region and shows how the human-made transformation of Amazonia may impact future atmospheric observations at ATTO.
Philipp Porada, Alexandra Tamm, Jose Raggio, Yafang Cheng, Axel Kleidon, Ulrich Pöschl, and Bettina Weber
Biogeosciences, 16, 2003–2031, https://doi.org/10.5194/bg-16-2003-2019, https://doi.org/10.5194/bg-16-2003-2019, 2019
Short summary
Short summary
The trace gases NO and HONO are crucial for atmospheric chemistry. It has been suggested that biological soil crusts in drylands contribute substantially to global NO and HONO emissions, based on empirical upscaling of laboratory and field observations. Here we apply an alternative, process-based modeling approach to predict these emissions. We find that biological soil crusts emit globally significant amounts of NO and HONO, which also vary depending on the type of biological soil crust.
Ying Li and Manabu Shiraiwa
Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, https://doi.org/10.5194/acp-19-5959-2019, 2019
Short summary
Short summary
Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
Tobias Könemann, Nicole Savage, Thomas Klimach, David Walter, Janine Fröhlich-Nowoisky, Hang Su, Ulrich Pöschl, J. Alex Huffman, and Christopher Pöhlker
Atmos. Meas. Tech., 12, 1337–1363, https://doi.org/10.5194/amt-12-1337-2019, https://doi.org/10.5194/amt-12-1337-2019, 2019
Short summary
Short summary
This study presents a comprehensive assessment of the SIBS, an instrument for spectrally resolved fluorescence detection of single particles. Exemplary ambient data and fluorescence spectra obtained for 16 reference compounds (biofluorophores and PSLs) show that the SIBS has the ability to expand the scope of fluorescent bioaerosol quantification and classification. Detailed technical insights will be broadly beneficial for users of various WIBS generations and other LIF instruments.
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232, https://doi.org/10.5194/acp-19-2209-2019, https://doi.org/10.5194/acp-19-2209-2019, 2019
Short summary
Short summary
VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Xiaoxiang Wang, Chuchu Chen, Kurt Binder, Uwe Kuhn, Ulrich Pöschl, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 18, 17077–17086, https://doi.org/10.5194/acp-18-17077-2018, https://doi.org/10.5194/acp-18-17077-2018, 2018
Short summary
Short summary
The surface tension of aqueous NaCl (σ) is investigated by molecular dynamics simulations from dilute to highly supersaturated solutions. The linear approximation of concentration dependence of σ at molality scale can be extended to the supersaturated NaCl solution until the solute mass fraction (xNaCl) of ~0.39. After that, the σ remains almost unchanged until an xNaCl of ~0.47. Then the σ gradually regains the growing momentum with a tendency to approach the surface tension of molten NaCl.
Anna T. Kunert, Mark Lamneck, Frank Helleis, Ulrich Pöschl, Mira L. Pöhlker, and Janine Fröhlich-Nowoisky
Atmos. Meas. Tech., 11, 6327–6337, https://doi.org/10.5194/amt-11-6327-2018, https://doi.org/10.5194/amt-11-6327-2018, 2018
Short summary
Short summary
The new Twin-plate Ice Nucleation Assay with infrared detection for high-throughput droplet freezing experiments in microliter-sized droplets is introduced, which was tested and characterized with bacterial and fungal ice nuclei. It was applied to investigate the influence of chemical processing on the activity of biological ice nuclei, and aqueous extracts of atmospheric aerosols were studied for ice nuclei activity.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
Short summary
Short summary
Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Jorge Saturno, Bruna A. Holanda, Christopher Pöhlker, Florian Ditas, Qiaoqiao Wang, Daniel Moran-Zuloaga, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Jeannine Ditas, Thorsten Hoffmann, Isabella Hrabe de Angelis, Tobias Könemann, Jošt V. Lavrič, Nan Ma, Jing Ming, Hauke Paulsen, Mira L. Pöhlker, Luciana V. Rizzo, Patrick Schlag, Hang Su, David Walter, Stefan Wolff, Yuxuan Zhang, Paulo Artaxo, Ulrich Pöschl, and Meinrat O. Andreae
Atmos. Chem. Phys., 18, 12817–12843, https://doi.org/10.5194/acp-18-12817-2018, https://doi.org/10.5194/acp-18-12817-2018, 2018
Short summary
Short summary
Biomass burning emits light-absorbing aerosol particles that warm the atmosphere. One of them is the primarily emitted black carbon, which strongly absorbs radiation in the visible and UV spectral regions. Another one is the so-called brown carbon, a fraction of organic aerosol particles that are able to absorb radiation, especially in the UV spectral region. The contribution of both kinds of aerosol particles to light absorption over the Amazon rainforest is studied in this paper.
Céline Degrendele, Jake Wilson, Petr Kukučka, Jana Klánová, and Gerhard Lammel
Atmos. Chem. Phys., 18, 12877–12890, https://doi.org/10.5194/acp-18-12877-2018, https://doi.org/10.5194/acp-18-12877-2018, 2018
Short summary
Short summary
Polybrominated diphenyl ethers (PBDEs) are persistent organic pollutants present in the global environment. This study, reporting on their atmospheric behaviour in central Europe, has shown that none of the three investigated gas–particle partitioning models provided a satisfactory prediction, highlighting the need for a model that is universally applicable. Finally, this study tends to show that the debromination from high to low brominated congeners, enhanced by photolysis, is important.
Jorge Saturno, Florian Ditas, Marloes Penning de Vries, Bruna A. Holanda, Mira L. Pöhlker, Samara Carbone, David Walter, Nicole Bobrowski, Joel Brito, Xuguang Chi, Alexandra Gutmann, Isabella Hrabe de Angelis, Luiz A. T. Machado, Daniel Moran-Zuloaga, Julian Rüdiger, Johannes Schneider, Christiane Schulz, Qiaoqiao Wang, Manfred Wendisch, Paulo Artaxo, Thomas Wagner, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10391–10405, https://doi.org/10.5194/acp-18-10391-2018, https://doi.org/10.5194/acp-18-10391-2018, 2018
Short summary
Short summary
This study uses satellite observations to track volcanic emissions in eastern Congo and their subsequent transport across the Atlantic Ocean into the Amazon Basin. Aircraft and ground-based observations are used to characterize the influence of volcanogenic aerosol on the chemical and microphysical properties of Amazonian aerosols. Further, this work is an illustrative example of the conditions and dynamics driving the transatlantic transport of African emissions to South America.
Mira L. Pöhlker, Florian Ditas, Jorge Saturno, Thomas Klimach, Isabella Hrabě de Angelis, Alessandro C. Araùjo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Bruna A. Holanda, Konrad Kandler, Jürgen Kesselmeier, Tobias Könemann, Ovid O. Krüger, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Luciana V. Rizzo, Diana Rose, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10289–10331, https://doi.org/10.5194/acp-18-10289-2018, https://doi.org/10.5194/acp-18-10289-2018, 2018
Short summary
Short summary
This paper presents the aerosol and cloud condensation nuclei (CCN) variability for characteristic atmospheric states – such as biomass burning, long-range transport, and pristine rain forest conditions – in the vulnerable and climate-relevant Amazon Basin. It summarizes the key properties of aerosol and CCN and, thus, provides a basis for an in-depth analysis of aerosol–cloud interactions in the Amazon region.
Daniel Moran-Zuloaga, Florian Ditas, David Walter, Jorge Saturno, Joel Brito, Samara Carbone, Xuguang Chi, Isabella Hrabě de Angelis, Holger Baars, Ricardo H. M. Godoi, Birgit Heese, Bruna A. Holanda, Jošt V. Lavrič, Scot T. Martin, Jing Ming, Mira L. Pöhlker, Nina Ruckteschler, Hang Su, Yaqiang Wang, Qiaoqiao Wang, Zhibin Wang, Bettina Weber, Stefan Wolff, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10055–10088, https://doi.org/10.5194/acp-18-10055-2018, https://doi.org/10.5194/acp-18-10055-2018, 2018
Short summary
Short summary
This study presents multiple years of aerosol coarse mode observations at the remote ATTO site in the Amazon Basin. The results are discussed in light of the frequent and episodic long-range transport of Saharan dust plumes in the early wet season as well as the persistent background bioaerosol cycling in the rain forest ecosystem. This work provides a solid basis for future studies on the dynamic coarse mode aerosol cycling and its biogeochemical relevance in the Amazon.
Jörn Wehking, Daniel A. Pickersgill, Robert M. Bowers, David Teschner, Ulrich Pöschl, Janine Fröhlich-Nowoisky, and Viviane R. Després
Biogeosciences, 15, 4205–4214, https://doi.org/10.5194/bg-15-4205-2018, https://doi.org/10.5194/bg-15-4205-2018, 2018
Short summary
Short summary
Archaea as a third domain of life play an important role in soils and marine environments. Although archaea have been found in air as a part of the atmospheric bioaerosol, little is known about their atmospheric dynamics due to their low number and challenging analysis.
Here we present a DNA-based study of airborne archaea, show seasonal dynamics, and discuss anthropogenic influences on the diversity, composition, and abundances of airborne archaea.
Luiz A. T. Machado, Alan J. P. Calheiros, Thiago Biscaro, Scott Giangrande, Maria A. F. Silva Dias, Micael A. Cecchini, Rachel Albrecht, Meinrat O. Andreae, Wagner F. Araujo, Paulo Artaxo, Stephan Borrmann, Ramon Braga, Casey Burleyson, Cristiano W. Eichholz, Jiwen Fan, Zhe Feng, Gilberto F. Fisch, Michael P. Jensen, Scot T. Martin, Ulrich Pöschl, Christopher Pöhlker, Mira L. Pöhlker, Jean-François Ribaud, Daniel Rosenfeld, Jaci M. B. Saraiva, Courtney Schumacher, Ryan Thalman, David Walter, and Manfred Wendisch
Atmos. Chem. Phys., 18, 6461–6482, https://doi.org/10.5194/acp-18-6461-2018, https://doi.org/10.5194/acp-18-6461-2018, 2018
Short summary
Short summary
This overview discuss the main precipitation processes and their sensitivities to environmental conditions in the Central Amazon Basin. It presents a review of the knowledge acquired about cloud processes and rainfall formation in Amazonas. In addition, this study provides a characterization of the seasonal variation and rainfall sensitivities to topography, surface cover, and aerosol concentration. Airplane measurements were evaluated to characterize and contrast cloud microphysical properties.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
Short summary
Short summary
The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Trismono C. Krisna, Manfred Wendisch, André Ehrlich, Evelyn Jäkel, Frank Werner, Ralf Weigel, Stephan Borrmann, Christoph Mahnke, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Luiz A. T. Machado
Atmos. Chem. Phys., 18, 4439–4462, https://doi.org/10.5194/acp-18-4439-2018, https://doi.org/10.5194/acp-18-4439-2018, 2018
Short summary
Short summary
The optical thickness and particle effective radius of a cirrus above liquid water clouds and a DCC topped by an anvil cirrus are retrieved based on SMART and MODIS radiance measurements. For the cirrus, retrieved particle effective radius are validated with corresponding in situ data using a vertical weighting method. This approach allows to assess the measurements, retrieval algorithms, and derived cloud products.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
Short summary
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.
Guo Li, Hang Su, Uwe Kuhn, Hannah Meusel, Markus Ammann, Min Shao, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 18, 2669–2686, https://doi.org/10.5194/acp-18-2669-2018, https://doi.org/10.5194/acp-18-2669-2018, 2018
Short summary
Short summary
Coated-wall flow tube reactors are frequently used to investigate gas uptake and heterogeneous or multiphase reaction kinetics under laminar flow conditions. In previous applications, the effects of coating surface roughness on flow conditions were not well quantified. In this study, a criterion is proposed to eliminate/minimize the potential effects of coating surface roughness on laminar flow in coated-wall flow tube experiments and validate the applications of diffusion correction methods.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
Short summary
Short summary
We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
Short summary
Short summary
We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
Short summary
Short summary
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.
Micael A. Cecchini, Luiz A. T. Machado, Manfred Wendisch, Anja Costa, Martina Krämer, Meinrat O. Andreae, Armin Afchine, Rachel I. Albrecht, Paulo Artaxo, Stephan Borrmann, Daniel Fütterer, Thomas Klimach, Christoph Mahnke, Scot T. Martin, Andreas Minikin, Sergej Molleker, Lianet H. Pardo, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, and Bernadett Weinzierl
Atmos. Chem. Phys., 17, 14727–14746, https://doi.org/10.5194/acp-17-14727-2017, https://doi.org/10.5194/acp-17-14727-2017, 2017
Short summary
Short summary
This study introduces and explores the concept of gamma phase space. This space is able to represent all possible variations in the cloud droplet size distributions (DSDs). The methodology was applied to recent in situ aircraft measurements over the Amazon. It is shown that the phase space is able to represent several processes occurring in the clouds in a simple manner. The consequences for cloud studies, modeling, and the representation of the transition from warm to mixed phase are discussed.
Ramon Campos Braga, Daniel Rosenfeld, Ralf Weigel, Tina Jurkat, Meinrat O. Andreae, Manfred Wendisch, Ulrich Pöschl, Christiane Voigt, Christoph Mahnke, Stephan Borrmann, Rachel I. Albrecht, Sergej Molleker, Daniel A. Vila, Luiz A. T. Machado, and Lucas Grulich
Atmos. Chem. Phys., 17, 14433–14456, https://doi.org/10.5194/acp-17-14433-2017, https://doi.org/10.5194/acp-17-14433-2017, 2017
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
Short summary
Short summary
In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Eugene F. Mikhailov, Svetlana Mironova, Gregory Mironov, Sergey Vlasenko, Alexey Panov, Xuguang Chi, David Walter, Samara Carbone, Paulo Artaxo, Martin Heimann, Jost Lavric, Ulrich Pöschl, and Meinrat O. Andreae
Atmos. Chem. Phys., 17, 14365–14392, https://doi.org/10.5194/acp-17-14365-2017, https://doi.org/10.5194/acp-17-14365-2017, 2017
Daniel A. Pickersgill, Jörn Wehking, Hauke Paulsen, Eckhard Thines, Ulrich Pöschl, Janine Fröhlich-Nowoisky, and Viviane R. Després
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-452, https://doi.org/10.5194/bg-2017-452, 2017
Manuscript not accepted for further review
Short summary
Short summary
To investigate lifestyle dependent sporulation strategies of wind-dispersed fungi, species and genera identified in environmental air samples were grouped according to their lifestyles or ecological niches. Findings revealed unrecognized characteristic patterns in the seasonal occurrence and size distribution of fungal spores for different types of pathogenic and saprophytic fungi growing on herbaceous and woody plants.
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, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
Short summary
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.
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
Short summary
Short summary
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.
Ryan Thalman, Suzane S. de Sá, Brett B. Palm, Henrique M. J. Barbosa, Mira L. Pöhlker, M. Lizabeth Alexander, Joel Brito, Samara Carbone, Paulo Castillo, Douglas A. Day, Chongai Kuang, Antonio Manzi, Nga Lee Ng, Arthur J. Sedlacek III, Rodrigo Souza, Stephen Springston, Thomas Watson, Christopher Pöhlker, Ulrich Pöschl, Meinrat O. Andreae, Paulo Artaxo, Jose L. Jimenez, Scot T. Martin, and Jian Wang
Atmos. Chem. Phys., 17, 11779–11801, https://doi.org/10.5194/acp-17-11779-2017, https://doi.org/10.5194/acp-17-11779-2017, 2017
Short summary
Short summary
Particle hygroscopicity, mixing state, and the hygroscopicity of organic components were characterized in central Amazonia for 1 year; their seasonal and diel variations were driven by a combination of primary emissions, photochemical oxidation, and boundary layer development. The relationship between the hygroscopicity of organic components and their oxidation level was examined, and the results help to reconcile the differences among the relationships observed in previous studies.
Paul J. DeMott, Thomas C. J. Hill, Markus D. Petters, Allan K. Bertram, Yutaka Tobo, Ryan H. Mason, Kaitlyn J. Suski, Christina S. McCluskey, Ezra J. T. Levin, Gregory P. Schill, Yvonne Boose, Anne Marie Rauker, Anna J. Miller, Jake Zaragoza, Katherine Rocci, Nicholas E. Rothfuss, Hans P. Taylor, John D. Hader, Cedric Chou, J. Alex Huffman, Ulrich Pöschl, Anthony J. Prenni, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 17, 11227–11245, https://doi.org/10.5194/acp-17-11227-2017, https://doi.org/10.5194/acp-17-11227-2017, 2017
Short summary
Short summary
The consistency and complementarity of different methods for measuring the numbers of particles capable of forming ice in clouds are examined in the atmosphere. Four methods for collecting particles for later (offline) freezing studies are compared to a common instantaneous method. Results support very good agreement in many cases but also biases that require further research. Present capabilities and uncertainties for obtaining global data on these climate-relevant aerosols are thus defined.
Micael A. Cecchini, Luiz A. T. Machado, Meinrat O. Andreae, Scot T. Martin, Rachel I. Albrecht, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Daniel Fütterer, Tina Jurkat, Christoph Mahnke, Andreas Minikin, Sergej Molleker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Bernadett Weinzierl, and Manfred Wendisch
Atmos. Chem. Phys., 17, 10037–10050, https://doi.org/10.5194/acp-17-10037-2017, https://doi.org/10.5194/acp-17-10037-2017, 2017
Short summary
Short summary
We study the effects of aerosol particles and updraft speed on the warm phase of Amazonian clouds. We expand the sensitivity analysis usually found in the literature by concomitantly considering cloud evolution and the effects on droplet size distribution (DSD) shape. The quantitative results show that particle concentration is the primary driver for the vertical profiles of effective diameter and droplet concentration in the warm phase of Amazonian convective clouds.
Evelyn Jäkel, Manfred Wendisch, Trismono C. Krisna, Florian Ewald, Tobias Kölling, Tina Jurkat, Christiane Voigt, Micael A. Cecchini, Luiz A. T. Machado, Armin Afchine, Anja Costa, Martina Krämer, Meinrat O. Andreae, Ulrich Pöschl, Daniel Rosenfeld, and Tianle Yuan
Atmos. Chem. Phys., 17, 9049–9066, https://doi.org/10.5194/acp-17-9049-2017, https://doi.org/10.5194/acp-17-9049-2017, 2017
Short summary
Short summary
Vertical profiles of the cloud particle phase state in tropical deep convective clouds (DCCs) were investigated using airborne imaging spectrometer measurements during the ACRIDICON-CHUVA campaign, which was conducted over the Brazilian rainforest in September 2014. A phase discrimination retrieval was applied to observations of clouds formed in different aerosol conditions. The profiles were compared to in situ and satellite measurements.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
Short summary
Short summary
Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Ramon Campos Braga, Daniel Rosenfeld, Ralf Weigel, Tina Jurkat, Meinrat O. Andreae, Manfred Wendisch, Mira L. Pöhlker, Thomas Klimach, Ulrich Pöschl, Christopher Pöhlker, Christiane Voigt, Christoph Mahnke, Stephan Borrmann, Rachel I. Albrecht, Sergej Molleker, Daniel A. Vila, Luiz A. T. Machado, and Paulo Artaxo
Atmos. Chem. Phys., 17, 7365–7386, https://doi.org/10.5194/acp-17-7365-2017, https://doi.org/10.5194/acp-17-7365-2017, 2017
Sergey S. Vlasenko, Hang Su, Ulrich Pöschl, Meinrat O. Andreae, and Eugene F. Mikhailov
Atmos. Meas. Tech., 10, 1269–1280, https://doi.org/10.5194/amt-10-1269-2017, https://doi.org/10.5194/amt-10-1269-2017, 2017
Short summary
Short summary
The paper describes a new technique for measuring the hygroscopic properties of laboratory and ambient aerosols. The direct measurements of humidified particle mass allow avoiding complications that occur in the commonly used technique due to poorly defined particle morphology and density. Both test results and field measurements have shown that the system can be applied for aerosol size-resolved mass growth factor measurements in hydration and dehydration modes up to 95 % RH.
Philipp Porada, Ulrich Pöschl, Axel Kleidon, Christian Beer, and Bettina Weber
Biogeosciences, 14, 1593–1602, https://doi.org/10.5194/bg-14-1593-2017, https://doi.org/10.5194/bg-14-1593-2017, 2017
Short summary
Short summary
Lichens and bryophytes have been shown to release nitrous oxide, which is a strong greenhouse gas and atmospheric ozone-depleting agent. Here we apply a process-based computer model of lichens and bryophytes at the global scale, to estimate growth and respiration of the organisms. By relating respiration to nitrous oxide release, we simulate global nitrous oxide emissions of 0.27 (0.19–0.35) Tg yr−1. Moreover, we quantify different sources of uncertainty in nitrous oxide emission rates.
Zhibin Wang, Yafang Cheng, Nan Ma, Eugene Mikhailov, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-253, https://doi.org/10.5194/acp-2017-253, 2017
Revised manuscript has not been submitted
Mira L. Pöhlker, Christopher Pöhlker, Florian Ditas, Thomas Klimach, Isabella Hrabe de Angelis, Alessandro Araújo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Jürgen Kesselmeier, Tobias Könemann, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Diana Rose, Jorge Saturno, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, and Ulrich Pöschl
Atmos. Chem. Phys., 16, 15709–15740, https://doi.org/10.5194/acp-16-15709-2016, https://doi.org/10.5194/acp-16-15709-2016, 2016
Short summary
Short summary
The paper presents a systematic characterization of cloud condensation nuclei (CCN) concentration in the central Amazonian atmosphere. Our results show that the CCN population in this globally important ecosystem follows a pollution-related seasonal cycle, in which it mainly depends on changes in total aerosol size distribution and to a minor extent in the aerosol chemical composition. Our results allow an efficient modeling and prediction of the CCN population based on a novel approach.
Marie Ila Gosselin, Chathurika M. Rathnayake, Ian Crawford, Christopher Pöhlker, Janine Fröhlich-Nowoisky, Beatrice Schmer, Viviane R. Després, Guenter Engling, Martin Gallagher, Elizabeth Stone, Ulrich Pöschl, and J. Alex Huffman
Atmos. Chem. Phys., 16, 15165–15184, https://doi.org/10.5194/acp-16-15165-2016, https://doi.org/10.5194/acp-16-15165-2016, 2016
Short summary
Short summary
We present an analysis of bioaerosol measurements using two real-time fluorescence instruments in combination with molecular tracer techniques for quantifying airborne fungal spores in a semi-arid forest. Both techniques provide fungal spore concentrations of the order of 104 m−3 and up to 30 % of particle mass. Rainy periods exhibited higher concentrations and stronger correlations between fluorescent bioparticle and molecular tracer measurements. Fungal culture results are also presented.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
Short summary
Short summary
We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Hang Su, Yafang Cheng, Nan Ma, Zhibin Wang, Xiaoxiang Wang, Mira L. Pöhlker, Björn Nillius, Alfred Wiedensohler, and Ulrich Pöschl
Atmos. Meas. Tech., 9, 5183–5192, https://doi.org/10.5194/amt-9-5183-2016, https://doi.org/10.5194/amt-9-5183-2016, 2016
Short summary
Short summary
In cloud condensation nuclei (CCN) measurements, the supersaturation scan is often time-consuming and limits the temporal resolution of CCN measurements. Here we present a new concept, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, resulting in fast measurements of CCN activity.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
Short summary
Short summary
Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
Short summary
Short summary
Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
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, https://doi.org/10.5194/acp-16-12081-2016, https://doi.org/10.5194/acp-16-12081-2016, 2016
Short summary
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.
Xiawei Yu, Zhibin Wang, Minghui Zhang, Uwe Kuhn, Zhouqing Xie, Yafang Cheng, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 16, 11337–11348, https://doi.org/10.5194/acp-16-11337-2016, https://doi.org/10.5194/acp-16-11337-2016, 2016
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311, https://doi.org/10.5194/acp-16-10299-2016, https://doi.org/10.5194/acp-16-10299-2016, 2016
Short summary
Short summary
Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
A. E. Valsan, R. Ravikrishna, C. V. Biju, C. Pöhlker, V. R. Després, J. A. Huffman, U. Pöschl, and S. S. Gunthe
Atmos. Chem. Phys., 16, 9805–9830, https://doi.org/10.5194/acp-16-9805-2016, https://doi.org/10.5194/acp-16-9805-2016, 2016
S. T. Martin, P. Artaxo, L. A. T. Machado, A. O. Manzi, R. A. F. Souza, C. Schumacher, J. Wang, M. O. Andreae, H. M. J. Barbosa, J. Fan, G. Fisch, A. H. Goldstein, A. Guenther, J. L. Jimenez, U. Pöschl, M. A. Silva Dias, J. N. Smith, and M. Wendisch
Atmos. Chem. Phys., 16, 4785–4797, https://doi.org/10.5194/acp-16-4785-2016, https://doi.org/10.5194/acp-16-4785-2016, 2016
Short summary
Short summary
The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment took place in central Amazonia throughout 2014 and 2015. The experiment focused on the complex links among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other, especially when altered by urban pollution. This article serves as an introduction to the special issue of publications presenting findings of this experiment.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
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, https://doi.org/10.5194/acp-16-1823-2016, https://doi.org/10.5194/acp-16-1823-2016, 2016
Short summary
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.
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
Short summary
Short summary
We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
G. Gržinić, T. Bartels-Rausch, T. Berkemeier, A. Türler, and M. Ammann
Atmos. Chem. Phys., 15, 13615–13625, https://doi.org/10.5194/acp-15-13615-2015, https://doi.org/10.5194/acp-15-13615-2015, 2015
Short summary
Short summary
The heterogeneous loss of dinitrogen pentoxide (N2O5) to citric acid aerosol, a proxy for highly oxygenated secondary organic aerosol, is shown to be substantially lower than to other aqueous organic aerosol proxies investigated previously. This is attributed to the widely changing viscosity within the atmospherically relevant humidity range. It may explain some of the unexpectedly low loss rates of N2O5 to aerosol particles derived from field studies.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
Short summary
Short summary
The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
M. O. Andreae, O. C. Acevedo, A. Araùjo, P. Artaxo, C. G. G. Barbosa, H. M. J. Barbosa, J. Brito, S. Carbone, X. Chi, B. B. L. Cintra, N. F. da Silva, N. L. Dias, C. Q. Dias-Júnior, F. Ditas, R. Ditz, A. F. L. Godoi, R. H. M. Godoi, M. Heimann, T. Hoffmann, J. Kesselmeier, T. Könemann, M. L. Krüger, J. V. Lavric, A. O. Manzi, A. P. Lopes, D. L. Martins, E. F. Mikhailov, D. Moran-Zuloaga, B. W. Nelson, A. C. Nölscher, D. Santos Nogueira, M. T. F. Piedade, C. Pöhlker, U. Pöschl, C. A. Quesada, L. V. Rizzo, C.-U. Ro, N. Ruckteschler, L. D. A. Sá, M. de Oliveira Sá, C. B. Sales, R. M. N. dos Santos, J. Saturno, J. Schöngart, M. Sörgel, C. M. de Souza, R. A. F. de Souza, H. Su, N. Targhetta, J. Tóta, I. Trebs, S. Trumbore, A. van Eijck, D. Walter, Z. Wang, B. Weber, J. Williams, J. Winderlich, F. Wittmann, S. Wolff, and A. M. Yáñez-Serrano
Atmos. Chem. Phys., 15, 10723–10776, https://doi.org/10.5194/acp-15-10723-2015, https://doi.org/10.5194/acp-15-10723-2015, 2015
Short summary
Short summary
This paper describes the Amazon Tall Tower Observatory (ATTO), a new atmosphere-biosphere observatory located in the remote Amazon Basin. It presents results from ecosystem ecology, meteorology, trace gas, and aerosol measurements collected at the ATTO site during the first 3 years of operation.
D. Chang, Y. Cheng, P. Reutter, J. Trentmann, S. M. Burrows, P. Spichtinger, S. Nordmann, M. O. Andreae, U. Pöschl, and H. Su
Atmos. Chem. Phys., 15, 10325–10348, https://doi.org/10.5194/acp-15-10325-2015, https://doi.org/10.5194/acp-15-10325-2015, 2015
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
Short summary
Short summary
Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
M. Hummel, C. Hoose, M. Gallagher, D. A. Healy, J. A. Huffman, D. O'Connor, U. Pöschl, C. Pöhlker, N. H. Robinson, M. Schnaiter, J. R. Sodeau, M. Stengel, E. Toprak, and H. Vogel
Atmos. Chem. Phys., 15, 6127–6146, https://doi.org/10.5194/acp-15-6127-2015, https://doi.org/10.5194/acp-15-6127-2015, 2015
Z. Wang, H. Su, X. Wang, N. Ma, A. Wiedensohler, U. Pöschl, and Y. Cheng
Atmos. Meas. Tech., 8, 2161–2172, https://doi.org/10.5194/amt-8-2161-2015, https://doi.org/10.5194/amt-8-2161-2015, 2015
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
B. G. Pummer, C. Budke, S. Augustin-Bauditz, D. Niedermeier, L. Felgitsch, C. J. Kampf, R. G. Huber, K. R. Liedl, T. Loerting, T. Moschen, M. Schauperl, M. Tollinger, C. E. Morris, H. Wex, H. Grothe, U. Pöschl, T. Koop, and J. Fröhlich-Nowoisky
Atmos. Chem. Phys., 15, 4077–4091, https://doi.org/10.5194/acp-15-4077-2015, https://doi.org/10.5194/acp-15-4077-2015, 2015
G. J. Zheng, F. K. Duan, H. Su, Y. L. Ma, Y. Cheng, B. Zheng, Q. Zhang, T. Huang, T. Kimoto, D. Chang, U. Pöschl, Y. F. Cheng, and K. B. He
Atmos. Chem. Phys., 15, 2969–2983, https://doi.org/10.5194/acp-15-2969-2015, https://doi.org/10.5194/acp-15-2969-2015, 2015
J. Fröhlich-Nowoisky, T. C. J. Hill, B. G. Pummer, P. Yordanova, G. D. Franc, and U. Pöschl
Biogeosciences, 12, 1057–1071, https://doi.org/10.5194/bg-12-1057-2015, https://doi.org/10.5194/bg-12-1057-2015, 2015
S. Nordmann, Y. F. Cheng, G. R. Carmichael, M. Yu, H. A. C. Denier van der Gon, Q. Zhang, P. E. Saide, U. Pöschl, H. Su, W. Birmili, and A. Wiedensohler
Atmos. Chem. Phys., 14, 12683–12699, https://doi.org/10.5194/acp-14-12683-2014, https://doi.org/10.5194/acp-14-12683-2014, 2014
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
Short summary
Short summary
Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
J. Fröhlich-Nowoisky, C. Ruzene Nespoli, D. A. Pickersgill, P. E. Galand, I. Müller-Germann, T. Nunes, J. Gomes Cardoso, S. M. Almeida, C. Pio, M. O. Andreae, R. Conrad, U. Pöschl, and V. R. Després
Biogeosciences, 11, 6067–6079, https://doi.org/10.5194/bg-11-6067-2014, https://doi.org/10.5194/bg-11-6067-2014, 2014
Short summary
Short summary
We have investigated the presence of archaea as well as their amoA gene diversity in aerosol particles collected over 1 year in central Europe and found that, within the 16S and amoA gene, Thaumarchaeota prevail and experience a diversity peak in fall, while only few Euryarchaeota were detected primarily in spring. We also compared the results with airborne archaea from Cape Verde and observe that the proportions of Euryarchaeota seem to be enhanced in coastal air compared to continental air.
D. I. Haga, S. M. Burrows, R. Iannone, M. J. Wheeler, R. H. Mason, J. Chen, E. A. Polishchuk, U. Pöschl, and A. K. Bertram
Atmos. Chem. Phys., 14, 8611–8630, https://doi.org/10.5194/acp-14-8611-2014, https://doi.org/10.5194/acp-14-8611-2014, 2014
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
M. L. Krüger, S. Mertes, T. Klimach, Y. F. Cheng, H. Su, J. Schneider, M. O. Andreae, U. Pöschl, and D. Rose
Atmos. Meas. Tech., 7, 2615–2629, https://doi.org/10.5194/amt-7-2615-2014, https://doi.org/10.5194/amt-7-2615-2014, 2014
D. A. Healy, J. A. Huffman, D. J. O'Connor, C. Pöhlker, U. Pöschl, and J. R. Sodeau
Atmos. Chem. Phys., 14, 8055–8069, https://doi.org/10.5194/acp-14-8055-2014, https://doi.org/10.5194/acp-14-8055-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
C. J. Schumacher, C. Pöhlker, P. Aalto, V. Hiltunen, T. Petäjä, M. Kulmala, U. Pöschl, and J. A. Huffman
Atmos. Chem. Phys., 13, 11987–12001, https://doi.org/10.5194/acp-13-11987-2013, https://doi.org/10.5194/acp-13-11987-2013, 2013
D. Rose, S. S. Gunthe, Z. Jurányi, M. Gysel, G. P. Frank, J. Schneider, J. Curtius, and U. Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-32575-2013, https://doi.org/10.5194/acpd-13-32575-2013, 2013
Revised manuscript has not been submitted
C. Pöhlker, J. A. Huffman, J.-D. Förster, and U. Pöschl
Atmos. Meas. Tech., 6, 3369–3392, https://doi.org/10.5194/amt-6-3369-2013, https://doi.org/10.5194/amt-6-3369-2013, 2013
P. Porada, B. Weber, W. Elbert, U. Pöschl, and A. Kleidon
Biogeosciences, 10, 6989–7033, https://doi.org/10.5194/bg-10-6989-2013, https://doi.org/10.5194/bg-10-6989-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
J. A. Huffman, A. J. Prenni, P. J. DeMott, C. Pöhlker, R. H. Mason, N. H. Robinson, J. Fröhlich-Nowoisky, Y. Tobo, V. R. Després, E. Garcia, D. J. Gochis, E. Harris, I. Müller-Germann, C. Ruzene, B. Schmer, B. Sinha, D. A. Day, M. O. Andreae, J. L. Jimenez, M. Gallagher, S. M. Kreidenweis, A. K. Bertram, and U. Pöschl
Atmos. Chem. Phys., 13, 6151–6164, https://doi.org/10.5194/acp-13-6151-2013, https://doi.org/10.5194/acp-13-6151-2013, 2013
A.-P. Hyvärinen, V. Vakkari, L. Laakso, R. K. Hooda, V. P. Sharma, T. S. Panwar, J. P. Beukes, P. G. van Zyl, M. Josipovic, R. M. Garland, M. O. Andreae, U. Pöschl, and A. Petzold
Atmos. Meas. Tech., 6, 81–90, https://doi.org/10.5194/amt-6-81-2013, https://doi.org/10.5194/amt-6-81-2013, 2013
J. A. Huffman, B. Sinha, R. M. Garland, A. Snee-Pollmann, S. S. Gunthe, P. Artaxo, S. T. Martin, M. O. Andreae, and U. Pöschl
Atmos. Chem. Phys., 12, 11997–12019, https://doi.org/10.5194/acp-12-11997-2012, https://doi.org/10.5194/acp-12-11997-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Modeling impacts of dust mineralogy on fast climate response
Uncertainties in laboratory-measured shortwave refractive indices of mineral dust aerosols and derived optical properties: a theoretical assessment
Diagnosing uncertainties in global biomass burning emission inventories and their impact on modeled air pollutants
Role of atmospheric aerosols in severe winter fog over the Indo-Gangetic Plain of India: a case study
Long-term variability in black carbon emissions constrained by gap-filled absorption aerosol optical depth and associated premature mortality in China
Intercomparison of aerosol optical depths from four reanalyses and their multi-reanalysis consensus
Global aviation contrail climate effects from 2019 to 2021
Rapid iodine oxoacid nucleation enhanced by dimethylamine in broad marine regions
Simulations of the impact of cloud condensation nuclei and ice-nucleating particles perturbations on the microphysics and radar reflectivity factor of stratiform mixed-phase clouds
Aerosols in the central Arctic cryosphere: satellite and model integrated insights during Arctic spring and summer
Observationally constrained regional variations of shortwave absorption by iron oxides emphasize the cooling effect of dust
Droplet collection efficiencies inferred from satellite retrievals constrain effective radiative forcing of aerosol–cloud interactions
Global aerosol-type classification using a new hybrid algorithm and Aerosol Robotic Network data
Simulated phase state and viscosity of secondary organic aerosols over China
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign
Sharp increase in Saharan dust intrusions over the western Euro-Mediterranean in February–March 2020–2022 and associated atmospheric circulation
Temporal and spatial variations in dust activity in Australia based on remote sensing and reanalysis datasets
Sensitivity of global direct aerosol shortwave radiative forcing to uncertainties in aerosol optical properties
Molecular-level study on the role of methanesulfonic acid in iodine oxoacid nucleation
Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020
Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC
Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate aerosol model
Fire–precipitation interactions amplify the quasi-biennial variability in fires over southern Mexico and Central America
Improved estimates of smoke exposure during Australia fire seasons: importance of quantifying plume injection heights
New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau
Investigation of observed dust trends over the Middle East region in NASA Goddard Earth Observing System (GEOS) model simulations
A new process-based and scale-aware desert dust emission scheme for global climate models – Part II: Evaluation in the Community Earth System Model version 2 (CESM2)
How well do Earth system models reproduce the observed aerosol response to rapid emission reductions? A COVID-19 case study
In-plume and out-of-plume analysis of aerosol-cloud interactions derived from the 2014–15 Holuhraun volcanic eruption
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
Impact of acidity and surface-modulated acid dissociation on cloud response to organic aerosol
The contribution of residential wood combustion to the PM2.5 concentrations in the Helsinki metropolitan area
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
Investigating the sign of stratocumulus adjustments to aerosols in the global storm-resolving model ICON
Expanding the simulation of East Asian super dust storms: physical transport mechanisms impacting the western Pacific
Insights into the sources of ultrafine particle numbers at six European urban sites obtained by investigating COVID–19 lockdowns
Improving 3-day deterministic air pollution forecasts using machine learning algorithms
Opinion: The importance of historical and paleoclimate aerosol radiative effects
Assessing the assimilation of Himawari-8 observations on aerosol forecasts and radiative effects during pollution transport from South Asia to the Tibetan Plateau
Aerosol–meteorology feedback diminishes the transboundary transport of black carbon into the Tibetan Plateau
Associations of interannual variation in summer tropospheric ozone with the Western Pacific Subtropical High in China from 1999 to 2017
Climate intervention using marine cloud brightening (MCB) compared with stratospheric aerosol injection (SAI) in the UKESM1 climate model
Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: Strong surfactants
A model study on investigating the sensitivity of aerosol forcing on the volatilities of semi-volatile organic compounds
Decomposing the Effective Radiative Forcing of anthropogenic aerosols based on CMIP6 Earth System Models
Increased importance of aerosol–cloud interactions for surface PM2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions
The role of temporal scales in extracting dominant meteorological drivers of major airborne pollutants
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Air pollution trapping in the Dresden Basin from gray-zone scale urban modeling
Qianqian Song, Paul Ginoux, María Gonçalves Ageitos, Ron L. Miller, Vincenzo Obiso, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7421–7446, https://doi.org/10.5194/acp-24-7421-2024, https://doi.org/10.5194/acp-24-7421-2024, 2024
Short summary
Short summary
We implement and simulate the distribution of eight dust minerals in the GFDL AM4.0 model. We found that resolving the eight minerals reduces dust absorption compared to the homogeneous dust used in the standard GFDL AM4.0 model that assumes a globally uniform hematite content of 2.7 % by volume. Resolving dust mineralogy results in significant impacts on radiation, land surface temperature, surface winds, and precipitation over North Africa in summer.
Senyi Kong, Zheng Wang, and Lei Bi
Atmos. Chem. Phys., 24, 6911–6935, https://doi.org/10.5194/acp-24-6911-2024, https://doi.org/10.5194/acp-24-6911-2024, 2024
Short summary
Short summary
The retrieval of refractive indices of dust aerosols from laboratory optical measurements is commonly done assuming spherical particles. This paper aims to investigate the uncertainties in the shortwave refractive indices and corresponding optical properties by considering non-spherical and inhomogeneous models for dust samples. The study emphasizes the significance of using non-spherical models for simulating dust aerosols.
Wenxuan Hua, Sijia Lou, Xin Huang, Lian Xue, Ke Ding, Zilin Wang, and Aijun Ding
Atmos. Chem. Phys., 24, 6787–6807, https://doi.org/10.5194/acp-24-6787-2024, https://doi.org/10.5194/acp-24-6787-2024, 2024
Short summary
Short summary
In this study, we diagnose uncertainties in carbon monoxide and organic carbon emissions from four inventories for seven major wildfire-prone regions. Uncertainties in vegetation classification methods, fire detection products, and cloud obscuration effects lead to bias in these biomass burning (BB) emission inventories. By comparing simulations with measurements, we provide certain inventory recommendations. Our study has implications for reducing uncertainties in emissions in further studies.
Chandrakala Bharali, Mary Barth, Rajesh Kumar, Sachin D. Ghude, Vinayak Sinha, and Baerbel Sinha
Atmos. Chem. Phys., 24, 6635–6662, https://doi.org/10.5194/acp-24-6635-2024, https://doi.org/10.5194/acp-24-6635-2024, 2024
Short summary
Short summary
This study examines the role of atmospheric aerosols in winter fog over the Indo-Gangetic Plains of India using WRF-Chem. The increase in RH with aerosol–radiation feedback (ARF) is found to be important for fog formation as it promotes the growth of aerosols in the polluted environment. Aqueous-phase chemistry in the fog increases PM2.5 concentration, further affecting ARF. ARF and aqueous-phase chemistry affect the fog intensity and the timing of fog formation by ~1–2 h.
Wenxin Zhao, Yu Zhao, Yu Zheng, Dong Chen, Jinyuan Xin, Kaitao Li, Huizheng Che, Zhengqiang Li, Mingrui Ma, and Yun Hang
Atmos. Chem. Phys., 24, 6593–6612, https://doi.org/10.5194/acp-24-6593-2024, https://doi.org/10.5194/acp-24-6593-2024, 2024
Short summary
Short summary
We evaluate the long-term (2000–2020) variabilities of aerosol absorption optical depth, black carbon emissions, and associated health risks in China with an integrated framework that combines multiple observations and modeling techniques. We demonstrate the remarkable emission abatement resulting from the implementation of national pollution controls and show how human activities affected the emissions with a spatiotemporal heterogeneity, thus supporting differentiated policy-making by region.
Peng Xian, Jeffrey S. Reid, Melanie Ades, Angela Benedetti, Peter R. Colarco, Arlindo da Silva, Tom F. Eck, Johannes Flemming, Edward J. Hyer, Zak Kipling, Samuel Rémy, Tsuyoshi Thomas Sekiyama, Taichu Tanaka, Keiya Yumimoto, and Jianglong Zhang
Atmos. Chem. Phys., 24, 6385–6411, https://doi.org/10.5194/acp-24-6385-2024, https://doi.org/10.5194/acp-24-6385-2024, 2024
Short summary
Short summary
The study compares and evaluates monthly AOD of four reanalyses (RA) and their consensus (i.e., ensemble mean). The basic verification characteristics of these RA versus both AERONET and MODIS retrievals are presented. The study discusses the strength of each RA and identifies regions where divergence and challenges are prominent. The RA consensus usually performs very well on a global scale in terms of how well it matches the observational data, making it a good choice for various applications.
Roger Teoh, Zebediah Engberg, Ulrich Schumann, Christiane Voigt, Marc Shapiro, Susanne Rohs, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 6071–6093, https://doi.org/10.5194/acp-24-6071-2024, https://doi.org/10.5194/acp-24-6071-2024, 2024
Short summary
Short summary
The radiative forcing (RF) due to aviation contrails is comparable to that caused by CO2. We estimate that global contrail net RF in 2019 was 62.1 mW m−2. This is ~1/2 the previous best estimate for 2018. Contrail RF varies regionally due to differences in conditions required for persistent contrails. COVID-19 reduced contrail RF by 54% in 2020 relative to 2019. Globally, 2 % of all flights account for 80 % of the annual contrail energy forcing, suggesting a opportunity to mitigate contrail RF.
Haotian Zu, Biwu Chu, Yiqun Lu, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 5823–5835, https://doi.org/10.5194/acp-24-5823-2024, https://doi.org/10.5194/acp-24-5823-2024, 2024
Short summary
Short summary
The nucleation of iodic acid (HIO3) and iodous acid (HIO2) was proven to be critical in marine areas. However, HIO3–HIO2 nucleation cannot effectively derive the rapid nucleation in some polluted coasts. We find a significant enhancement of dimethylamine (DMA) on the HIO3–HIO2 nucleation in marine and polar regions with abundant DMA sources, which may establish reasonable connections between the HIO3–HIO2 nucleation and the rapid formation of new particles in polluted marine and polar regions.
Junghwa Lee, Patric Seifert, Tempei Hashino, Maximilian Maahn, Fabian Senf, and Oswald Knoth
Atmos. Chem. Phys., 24, 5737–5756, https://doi.org/10.5194/acp-24-5737-2024, https://doi.org/10.5194/acp-24-5737-2024, 2024
Short summary
Short summary
Spectral bin model simulations of an idealized supercooled stratiform cloud were performed with the AMPS model for variable CCN and INP concentrations. We performed radar forward simulations with PAMTRA to transfer the simulations into radar observational space. The derived radar reflectivity factors were compared to observational studies of stratiform mixed-phase clouds. These studies report a similar response of the radar reflectivity factor to aerosol perturbations as we found in our study.
Basudev Swain, Marco Vountas, Aishwarya Singh, Nidhi L. Anchan, Adrien Deroubaix, Luca Lelli, Yanick Ziegler, Sachin S. Gunthe, Hartmut Bösch, and John P. Burrows
Atmos. Chem. Phys., 24, 5671–5693, https://doi.org/10.5194/acp-24-5671-2024, https://doi.org/10.5194/acp-24-5671-2024, 2024
Short summary
Short summary
Arctic amplification (AA) accelerates the warming of the central Arctic cryosphere and affects aerosol dynamics. Limited observations hinder a comprehensive analysis. This study uses AEROSNOW aerosol optical density (AOD) data and GEOS-Chem simulations to assess AOD variability. Discrepancies highlight the need for improved observational integration into models to refine our understanding of aerosol effects on cloud microphysics, ice nucleation, and radiative forcing under evolving AA.
Vincenzo Obiso, María Gonçalves Ageitos, Carlos Pérez García-Pando, Jan P. Perlwitz, Gregory L. Schuster, Susanne E. Bauer, Claudia Di Biagio, Paola Formenti, Kostas Tsigaridis, and Ron L. Miller
Atmos. Chem. Phys., 24, 5337–5367, https://doi.org/10.5194/acp-24-5337-2024, https://doi.org/10.5194/acp-24-5337-2024, 2024
Short summary
Short summary
We calculate the dust direct radiative effect (DRE) in an Earth system model accounting for regionally varying soil mineralogy through a new observationally constrained method. Linking dust absorption at solar wavelengths to the varying amount of specific minerals (i.e., iron oxides) improves the modeled range of dust single scattering albedo compared to observations and increases the global cooling by dust. Our results may contribute to improved estimates of the dust DRE and its climate impact.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
Atmos. Chem. Phys., 24, 5287–5302, https://doi.org/10.5194/acp-24-5287-2024, https://doi.org/10.5194/acp-24-5287-2024, 2024
Short summary
Short summary
Single-layer warm liquid clouds cover nearly one-third of the Earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth system model estimates of the radiative forcing from the interactions of aerosols with clouds due to warm rain processes.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
Atmos. Chem. Phys., 24, 5025–5045, https://doi.org/10.5194/acp-24-5025-2024, https://doi.org/10.5194/acp-24-5025-2024, 2024
Short summary
Short summary
A new aerosol-type classification algorithm has been proposed. It includes an optical database built by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
Short summary
Short summary
Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
Atmos. Chem. Phys., 24, 4591–4610, https://doi.org/10.5194/acp-24-4591-2024, https://doi.org/10.5194/acp-24-4591-2024, 2024
Short summary
Short summary
We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass burning plumes.
Sampa Das, Peter R. Colarco, Huisheng Bian, and Santiago Gassó
Atmos. Chem. Phys., 24, 4421–4449, https://doi.org/10.5194/acp-24-4421-2024, https://doi.org/10.5194/acp-24-4421-2024, 2024
Short summary
Short summary
The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
Atmos. Chem. Phys., 24, 4083–4104, https://doi.org/10.5194/acp-24-4083-2024, https://doi.org/10.5194/acp-24-4083-2024, 2024
Short summary
Short summary
During February–March (FM) 2020–2022, unusually intense dust storms from northern Africa hit the western Euro-Mediterranean (WEM). Using dust products from satellites and atmospheric reanalysis for 2003–2022, results show that cut-off lows and European blocking are key drivers of FM dust intrusions over the WEM. A higher frequency of cut-off lows associated with subtropical ridges is observed in the late 2020–2022 period.
Yahui Che, Bofu Yu, and Katherine Bracco
Atmos. Chem. Phys., 24, 4105–4128, https://doi.org/10.5194/acp-24-4105-2024, https://doi.org/10.5194/acp-24-4105-2024, 2024
Short summary
Short summary
Dust events occur more frequently during the Austral spring and summer in dust regions, including central Australia, the southwest of Western Australia, and the northern and southern regions of eastern Australia using remote sensing and reanalysis datasets. High-concentration dust is distributed around central Australia and in the downwind northern and southern Australia. Typically, around 50 % of the dust lifted settles on Australian land, with the remaining half being deposited in the ocean.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
Atmos. Chem. Phys., 24, 4065–4081, https://doi.org/10.5194/acp-24-4065-2024, https://doi.org/10.5194/acp-24-4065-2024, 2024
Short summary
Short summary
Aerosols influence the Earth's energy balance. The uncertainty in this radiative forcing is large depending partly on uncertainty in measurements of aerosol optical properties. We have developed a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty, but non-aerosol uncertainties must also be considered.
Jing Li, Nan Wu, Biwu Chu, An Ning, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 3989–4000, https://doi.org/10.5194/acp-24-3989-2024, https://doi.org/10.5194/acp-24-3989-2024, 2024
Short summary
Short summary
Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
Short summary
Short summary
We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 24, 3217–3240, https://doi.org/10.5194/acp-24-3217-2024, https://doi.org/10.5194/acp-24-3217-2024, 2024
Short summary
Short summary
Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol–climate model to analyse INP-induced cirrus changes and the resulting climate impacts. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP–cirrus effect.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
Short summary
Short summary
Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
Short summary
Short summary
Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
Short summary
Short summary
During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
Short summary
Short summary
By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Adriana Rocha-Lima, Peter R. Colarco, Anton S. Darmenov, Edward P. Nowottnick, Arlindo M. da Silva, and Luke D. Oman
Atmos. Chem. Phys., 24, 2443–2464, https://doi.org/10.5194/acp-24-2443-2024, https://doi.org/10.5194/acp-24-2443-2024, 2024
Short summary
Short summary
Observations show an increasing aerosol optical depth trend in the Middle East between 2003–2012. We evaluate the NASA Goddard Earth Observing System (GEOS) model's ability to capture these trends and examine the meteorological and surface parameters driving dust emissions. Our results highlight the importance of data assimilation for long-term trends of atmospheric aerosols and support the hypothesis that vegetation cover loss may have contributed to increasing dust emissions in the period.
Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
Short summary
Short summary
This study uses a premier Earth system model to evaluate a new desert dust emission scheme proposed in our companion paper. We show that our scheme accounts for more dust emission physics, hence matching better against observations than other existing dust emission schemes do. Our scheme's dust emissions also couple tightly with meteorology, hence likely improving the modeled dust sensitivity to climate change. We believe this work is vital for improving dust representation in climate models.
Ruth A. R. Digby, Nathan P. Gillett, Adam H. Monahan, Knut von Salzen, Antonis Gkikas, Qianqian Song, and Zhibo Zhang
Atmos. Chem. Phys., 24, 2077–2097, https://doi.org/10.5194/acp-24-2077-2024, https://doi.org/10.5194/acp-24-2077-2024, 2024
Short summary
Short summary
The COVID-19 lockdowns reduced aerosol emissions. We ask whether these reductions affected regional aerosol optical depth (AOD) and compare the observed changes to predictions from Earth system models. Only India has an observed AOD reduction outside of typical variability. Models overestimate the response in some regions, but when key biases have been addressed, the agreement is improved. Our results suggest that current models can realistically predict the effects of future emission changes.
Amy H. Peace, Ying Chen, George Jordan, Daniel G. Partridge, Florent Malavelle, Eliza Duncan, and Jim M. Haywood
EGUsphere, https://doi.org/10.5194/egusphere-2024-360, https://doi.org/10.5194/egusphere-2024-360, 2024
Short summary
Short summary
Natural aerosols from volcanic eruptions can help us understand how anthropogenic aerosols modify climate. We use observations and model simulations of the 2014–15 Holuhraun eruption plume to examine aerosol-cloud interactions in September 2014. We find a shift to clouds with smaller, more numerous cloud droplets in the first two weeks of the eruption. In the third week, the background meteorology and previous conditions experienced by airmasses modulate the aerosol perturbation to clouds.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
Short summary
Short summary
This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Gargi Sengupta, Minjie Zheng, and Nønne L. Prisle
Atmos. Chem. Phys., 24, 1467–1487, https://doi.org/10.5194/acp-24-1467-2024, https://doi.org/10.5194/acp-24-1467-2024, 2024
Short summary
Short summary
The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in an atmospheric model. Organic acid dissociation was considered using both bulk and surface-related properties. We found that organic acid dissociation leads to increased hydrogen ion concentrations and sulfate aerosol mass in aqueous aerosols, increasing cloud formation. This could be important in large-scale climate models as many organic aerosol components are both acidic and surface-active.
Leena Kangas, Jaakko Kukkonen, Mari Kauhaniemi, Kari Riikonen, Mikhail Sofiev, Anu Kousa, Jarkko V. Niemi, and Ari Karppinen
Atmos. Chem. Phys., 24, 1489–1507, https://doi.org/10.5194/acp-24-1489-2024, https://doi.org/10.5194/acp-24-1489-2024, 2024
Short summary
Short summary
Residential wood combustion is a major source of fine particulate matter. This study has evaluated the contribution of residential wood combustion to fine particle concentrations and its year-to-year and seasonal variation in te Helsinki metropolitan area. The average concentrations attributed to wood combustion in winter were up to 10- or 15-fold compared to summer. Wood combustion caused 12 % to 14 % of annual fine particle concentrations. In winter, the contribution ranged from 16 % to 21 %.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
Atmos. Chem. Phys., 24, 1315–1328, https://doi.org/10.5194/acp-24-1315-2024, https://doi.org/10.5194/acp-24-1315-2024, 2024
Short summary
Short summary
Particle growth at the Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low-volatility organic compounds (LVOCs). Also, sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building knowledge of early growth of atmospheric particles.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-195, https://doi.org/10.5194/egusphere-2024-195, 2024
Short summary
Short summary
Aerosols can modify the liquid water path (LWP) of stratocumulus (Sc), and thus their radiative effect. This study compares model outputs and satellite data that disagree on the sign of Sc LWP adjustments: positive and negative, respectively. We use causality to diagnose this discrepancy and find that strong precipitation and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, while entrainment enhancement prevails in observations.
Steven Soon-Kai Kong, Saginela Ravindra Babu, Sheng-Hsiang Wang, Stephen M. Griffith, Jackson Hian-Wui Chang, Ming-Tung Chuang, Guey-Rong Sheu, and Neng-Huei Lin
Atmos. Chem. Phys., 24, 1041–1058, https://doi.org/10.5194/acp-24-1041-2024, https://doi.org/10.5194/acp-24-1041-2024, 2024
Short summary
Short summary
In this study, we combined ground observations from 7-SEAS Dongsha Experiment, MERRA-2 reanalysis, and MODIS satellite images for evaluation and improvement of the CMAQ dust model for cases of East Asian Dust reaching the Taiwan region, including Dongsha in the western Pacific. We proposed a better CMAQ dust treatment over East Asia and for the first time revealed the impact of typhoons on dust transport.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Tuukka Petäjä, Máté Vörösmarty, Imre Salma, Jarkko V. Niemi, Hanna E. Manninen, Dominik van Pinxteren, Roy M. Harrison, Thomas Tuch, and Kay Weinhold
EGUsphere, https://doi.org/10.5194/egusphere-2023-3053, https://doi.org/10.5194/egusphere-2023-3053, 2024
Short summary
Short summary
Different sources of airborne particles in the atmospheres of four European cities were distinguished by recognising their particle size distributions using a statistical procedure, Positive Matrix Factorization. The various sources responded differently to the changes in emissions associated with Covid lockdowns, and the reasons are investigated. While traffic emissions generally decreased, particles formed from reactions of atmospheric gases decreased in some cities, but increased in others.
Zhiguo Zhang, Christer Johansson, Magnuz Engardt, Massimo Stafoggia, and Xiaoliang Ma
Atmos. Chem. Phys., 24, 807–851, https://doi.org/10.5194/acp-24-807-2024, https://doi.org/10.5194/acp-24-807-2024, 2024
Short summary
Short summary
Up-to-date information on present and near-future air quality help people avoid exposure to high levels of air pollution. We apply different machine learning models to significantly improve traditional forecasts of PM10, NOx, and O3 in Stockholm, Sweden. It is shown that forecasts of all air pollutants are improved by the input of lagged measurements and taking calendar information into account. The final modelled errors are substantially smaller than uncertainties in the measurements.
Natalie M. Mahowald, Longlei Li, Samuel Albani, Douglas S. Hamilton, and Jasper F. Kok
Atmos. Chem. Phys., 24, 533–551, https://doi.org/10.5194/acp-24-533-2024, https://doi.org/10.5194/acp-24-533-2024, 2024
Short summary
Short summary
Estimating past aerosol radiative effects and their uncertainties is an important topic in climate science. Aerosol radiative effects propagate into large uncertainties in estimates of how present and future climate evolves with changing greenhouse gas emissions. A deeper understanding of how aerosols interacted with the atmospheric energy budget under past climates is hindered in part by a lack of relevant paleo-observations and in part because less attention has been paid to the problem.
Min Zhao, Tie Dai, Daisuke Goto, Hao Wang, and Guangyu Shi
Atmos. Chem. Phys., 24, 235–258, https://doi.org/10.5194/acp-24-235-2024, https://doi.org/10.5194/acp-24-235-2024, 2024
Short summary
Short summary
During a springtime pollution input from South Asia to the Tibetan Plateau, we combined atmospheric chemistry modeling and data assimilation methods to assimilate and forecast aerosols from South Asia and the Tibetan Plateau. Assimilation of observations over a whole time window leads to a more reasonable distribution of daily variations in the aerosol forecast field. We also find that aerosol assimilation can improve the surface solar energy forecast in the Tibetan Plateau region.
Yuling Hu, Haipeng Yu, Shichang Kang, Junhua Yang, Mukesh Rai, Xiufeng Yin, Xintong Chen, and Pengfei Chen
Atmos. Chem. Phys., 24, 85–107, https://doi.org/10.5194/acp-24-85-2024, https://doi.org/10.5194/acp-24-85-2024, 2024
Short summary
Short summary
The Tibetan Plateau (TP) saw a record-breaking aerosol pollution event from April 20 to May 10, 2016. We studied the impact of aerosol–meteorology feedback on the transboundary transport flux of black carbon (BC) during this severe pollution event. It was found that the aerosol–meteorology feedback decreases the transboundary transport flux of BC from the central and western Himalayas towards the TP. This study is of great significance for the protection of the ecological environment of the TP.
Xiaodong Zhang, Ruiyu Zhugu, Xiaohu Jian, Xinrui Liu, Kaijie Chen, Shu Tao, Junfeng Liu, Hong Gao, Tao Huang, and Jianmin Ma
Atmos. Chem. Phys., 23, 15629–15642, https://doi.org/10.5194/acp-23-15629-2023, https://doi.org/10.5194/acp-23-15629-2023, 2023
Short summary
Short summary
WRF-Chem modeling was conducted to assess impacts of Western Pacific Subtropical High Pressure (WPSH) on interannual fluctuations of O3 pollution in China. We find that, while precursor emissions dominated the long-term trend and magnitude of O3 from 1999 to 2017, WPSH determined interannual variation of summer O3. The response of O3 pollution to WPSH in major urban clusters depended on the proximity of these urban areas to WPSH. The results could help long-term O3 pollution mitigation planning.
Jim M. Haywood, Andy Jones, Anthony C. Jones, Paul Halloran, and Philip J. Rasch
Atmos. Chem. Phys., 23, 15305–15324, https://doi.org/10.5194/acp-23-15305-2023, https://doi.org/10.5194/acp-23-15305-2023, 2023
Short summary
Short summary
The difficulties in ameliorating global warming and the associated climate change via conventional mitigation are well documented, with all climate model scenarios exceeding 1.5 °C above the preindustrial level in the near future. There is therefore a growing interest in geoengineering to reflect a greater proportion of sunlight back to space and offset some of the global warming. We use a state-of-the-art Earth-system model to investigate two of the most prominent geoengineering strategies.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, https://doi.org/10.5194/acp-23-15149-2023, 2023
Short summary
Short summary
Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six models to surface activity of strongly surface active aerosol and find significant differences between the models, especially with large fractions of surfactant in the dry particles.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
EGUsphere, https://doi.org/10.5194/egusphere-2023-2768, https://doi.org/10.5194/egusphere-2023-2768, 2023
Short summary
Short summary
The study underscores the influence of semi-volatile organic compounds on the formation of secondary organic aerosol (SOA). Our findings demonstrate their considerable impact on climate, emphasizing the necessity to improve their representation in large-scale climate models. This research provides a nuanced perspective on the challenges in modelling, emphasizing the significance of semi-volatile compounds and their volatility distribution in predicting global climate patterns.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
EGUsphere, https://doi.org/10.5194/egusphere-2023-2571, https://doi.org/10.5194/egusphere-2023-2571, 2023
Short summary
Short summary
Effective Radiative Forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF and we estimate the contribution of individual processes to the total ERF using simulations from Earth System Models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol-cloud interactions drive ERF variability during the last 150 years.
Da Gao, Bin Zhao, Shuxiao Wang, Yuan Wang, Brian Gaudet, Yun Zhu, Xiaochun Wang, Jiewen Shen, Shengyue Li, Yicong He, Dejia Yin, and Zhaoxin Dong
Atmos. Chem. Phys., 23, 14359–14373, https://doi.org/10.5194/acp-23-14359-2023, https://doi.org/10.5194/acp-23-14359-2023, 2023
Short summary
Short summary
Surface PM2.5 concentrations can be enhanced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). In this study, we found PM2.5 enhancement induced by ACIs shows a significantly smaller decrease ratio than that induced by ARIs in China with anthropogenic emission reduction from 2013 to 2021, making ACIs more important for enhancing PM2.5 concentrations. ACI-induced PM2.5 enhancement needs to be emphatically considered to meet the national PM2.5 air quality standard.
Miaoqing Xu, Jing Yang, Manchun Li, Xiao Chen, Qiancheng Lv, Qi Yao, Bingbo Gao, and Ziyue Chen
Atmos. Chem. Phys., 23, 14065–14076, https://doi.org/10.5194/acp-23-14065-2023, https://doi.org/10.5194/acp-23-14065-2023, 2023
Short summary
Short summary
Although the temporal-scale effects on PM2.5–meteorology associations have been discussed, no quantitative evidence has proved this before. Based on rare 3 h meteorology data, we revealed that the dominant meteorological factor for PM2.5 concentrations across China extracted at the 3 h and 24 h scales presented large variations. This research suggests that data sources of different temporal scales should be comprehensively considered for better attribution and prevention of airborne pollution.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
Short summary
Short summary
To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Michael Weger and Bernd Heinold
Atmos. Chem. Phys., 23, 13769–13790, https://doi.org/10.5194/acp-23-13769-2023, https://doi.org/10.5194/acp-23-13769-2023, 2023
Short summary
Short summary
This study investigates the effects of complex terrain on air pollution trapping using a numerical model which simulates the dispersion of emissions under real meteorological conditions. The additionally simulated aerosol age allows us to distinguish areas that accumulate aerosol over time from areas that are more influenced by fresh emissions. The Dresden Basin, a widened section of the Elbe Valley in eastern Germany, is selected as the target area in a case study to demonstrate the concept.
Cited articles
Akyüz, M. and Çabuk, H.: Gas–particle partitioning and seasonal variation of polycyclic aromatic hydrocarbons in the atmosphere of Zonguldak, Turkey, Sci. Total Environ., 408, 5550–5558, https://doi.org/10.1016/j.scitotenv.2010.07.063, 2010. a
Arp, H. P. H., Schwarzenbach, R. P., and Goss, K.-U.: Ambient gas/particle partitioning. 2: The influence of particle source and temperature on sorption to dry terrestrial aerosols, Environ. Sci. Technol., 42, 5951–5957, https://doi.org/10.1021/es703096p, 2008. a
Berkemeier, T., Takeuchi, M., Eris, G., and Ng, N. L.: Kinetic modeling of formation and evaporation of secondary organic aerosol from NO3 oxidation of pure and mixed monoterpenes, Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, 2020. a
Bernasconi, C. F.: Relaxation Kinetics, Chapter 1 – Basic Principles, Academic Press, New York, https://doi.org/10.1016/B978-0-12-092950-4.50005-8, 1976. a
Bertram, A. K., Ivanov, A. V., Hunter, M., Molina, L. T., and Molina, M. J.: The reaction probability of OH on organic surfaces of tropospheric interest, J. Phys. Chem. A, 105, 9415–9421, https://doi.org/10.1021/jp0114034, 2001. a
Billiard, S. M., Meyer, J. N., Wassenberg, D. M., Hodson, P. V., and Di Giulio, R. T.: Nonadditive effects of PAHs on Early Vertebrate Development: mechanisms and implications for risk assessment, Toxicol. Sci., 105, 5–23, https://doi.org/10.1093/toxsci/kfm303, 2008. a
Boström, C.-E., Gerde, P., Hanberg, A., Jernström, B., Johansson, C., Kyrklund, T., Rannug, A., Törnqvist, M., Victorin, K., and Westerholm, R.: Cancer risk assessment, indicators, and guidelines for polycyclic aromatic hydrocarbons in the ambient air., Environ. Health Persp., 110, 451–488, https://doi.org/10.1289/ehp.110-1241197, 2002. a
Brasseur, G. P. and Jacob, D. J.: Modeling of Atmospheric Chemistry, Cambridge University Press, Cambridge, United Kingdom, https://doi.org/10.1017/9781316544754, 2017. a
Brubaker, W. W. and Hites, R. A.: OH Reaction kinetics of polycyclic aromatic hydrocarbons and polychlorinated dibenzo-p-dioxins and dibenzofurans, J. Phys. Chem. A, 102, 915–921, 1998. a
Callén, M. S., de la Cruz, M. T., López, J. M., Murillo, R., Navarro, M. V., and Mastral, A. M.: Some inferences on the mechanism of atmospheric gas/particle partitioning of polycyclic aromatic hydrocarbons (PAH) at Zaragoza (Spain), Chemosphere, 73, 1357–1365, https://doi.org/10.1016/j.chemosphere.2008.06.063, 2008. a
Cappa, C. D. and Wilson, K. R.: Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior, Atmos. Chem. Phys., 11, 1895–1911, https://doi.org/10.5194/acp-11-1895-2011, 2011. a
Chu, S. N., Sands, S., Tomasik, M. R., Lee, P. S., and McNeill, V. F.: Ozone oxidation of surface-adsorbed polycyclic aromatic hydrocarbons: Role of PAH–surface interaction, J. Am. Chem. Soc, 132, 15968–15975, https://doi.org/10.1021/ja1014772, 2010. a
Dachs, J. and Eisenreich, S. J.: Adsorption onto aerosol soot carbon dominates gas-particle partitioning of polycyclic aromatic hydrocarbons, Environ. Sci. Technol., 34, 3690–3697, https://doi.org/10.1021/es991201+, 2000. a
Ding, N., Chen, X., and Wu, C.-M. L.: Interactions between polybrominated diphenyl ethers and graphene surface: a DFT and MD investigation, Environ. Sci. Nano, 1, 55–63, https://doi.org/10.1039/C3EN00037K, 2014. a
Fasnacht, M. P. and Blough, N. V.: Aqueous photodegradation of polycyclic aromatic hydrocarbons, Environ. Sci. Technol., 36, 4364–4369, https://doi.org/10.1021/es025603k, 2002. a
Finizio, A., Mackay, D., Bidleman, T., and Harner, T.: Octanol-air partition coefficient as a predictor of partitioning of semi-volatile organic chemicals to aerosols, Atmos. Environ., 31, 2289–2296, https://doi.org/10.1016/S1352-2310(97)00013-7, 1997. a
Fraser, S. J.: The steady state and equilibrium approximations: A geometrical picture, J. Chem. Phys., 88, 4732–4738, https://doi.org/10.1063/1.454686, 1988. a
Friedman, C. L., Pierce, J. R., and Selin, N. E.: Assessing the influence of secondary organic versus primary carbonaceous aerosols on long-range atmospheric polycyclic aromatic hydrocarbon transport, Environ. Sci. Technol., 48, 3293–3302, https://doi.org/10.1021/es405219r, 2014. a
Galarneau, E., Makar, P. A., Zheng, Q., Narayan, J., Zhang, J., Moran, M. D., Bari, M. A., Pathela, S., Chen, A., and Chlumsky, R.: PAH concentrations simulated with the AURAMS-PAH chemical transport model over Canada and the USA, Atmos. Chem. Phys., 14, 4065–4077, https://doi.org/10.5194/acp-14-4065-2014, 2014. a, b
Geyer, A., Bächmann, K., Hofzumahaus, A., Holland, F., Konrad, S., Klüpfel, T., Pätz, H.-W., Perner, D., Mihelcic, D., Schäfer, H.-J., Volz-Thomas, A., and Platt, U.: Nighttime formation of peroxy and hydroxyl radicals during the BERLIOZ campaign: Observations and modeling studies, J. Geophys. Res.-Atmos., 108, 8249, https://doi.org/10.1029/2001JD000656, 2003. a
Gross, S. and Bertram, A. K.: Reactive uptake of NO3, N2O5, NO2, HNO3, and O3 on three types of polycyclic aromatic hydrocarbon surfaces, J. Phys. Chem. A, 112, 3104–3113, https://doi.org/10.1021/jp7107544, 2008. a
Guilloteau, A., Nguyen, M. L., Bedjanian, Y., and Le Bras, G.: Desorption of polycyclic aromatic hydrocarbons from soot surface: Pyrene and fluoranthene, J. Phys. Chem. A, 112, 10552–10559, https://doi.org/10.1021/jp803043s, 2008. a, b
Harner, T. and Bidleman, T. F.: Octanol–air partition coefficient for describing particle/gas partitioning of aromatic compounds in urban air, Environ. Sci. Technol., 32, 1494–1502, https://doi.org/10.1021/es970890r, 1998. a
Hobbs, P. V., Sinha, P., Yokelson, R. J., Christian, T. J., Blake, D. R., Gao, S., Kirchstetter, T. W., Novakov, T., and Pilewskie, P.: Evolution of gases and particles from a savanna fire in South Africa, J. Geophys. Res.-Atmos., 108, 8485, https://doi.org/10.1029/2002JD002352, 2003. a
Hofzumahaus, A., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C.-C., Fuchs, H., Holland, F., Kita, K., Kondo, Y., Li, X., Lou, S., Shao, M., Zeng, L., Wahner, A., and Zhang, Y.: Amplified trace gas removal in the troposphere, Science, 324, 1702–1704, https://doi.org/10.1126/science.1164566, 2009. a
Julin, J., Winkler, P. M., Donahue, N. M., Wagner, P. E., and Riipinen, I.: Near-unity mass accommodation coefficient of organic molecules of varying structure, Environ. Sci. Technol., 48, 12083–12089, https://doi.org/10.1021/es501816h, 2014. a, b, c
Junge, C.: Basic considerations about trace constituents in the atmosphere as related to the fate of global pollutants, in: Fate of pollutants in the air and water environments. Part I., edited by: Suffet, I. H., Wiley-Interscience, New York, 1977. a
Kamens, R., Odum, J., and Fan, Z.-H.: Some observations on times to equilibrium for semivolatile polycyclic aromatic hydrocarbons, Environ. Sci. Technol., 29, 43–50, https://doi.org/10.1021/es00001a005, 1995. a
Keyte, I. J., Harrison, R. M., and Lammel, G.: Chemical reactivity and long-range transport potential of polycyclic aromatic hydrocarbons – a review, Chem. Soc. Rev., 42, 9333–9391, https://doi.org/10.1039/C3CS60147A, 2013. a, b
Kiefer, J.: Sequential minimax search for a maximum, Proc. Am. Math. Soc., 4, 502–506, https://doi.org/10.1090/S0002-9939-1953-0055639-3, 1953. a
Kim, K.-H., Jahan, S. A., Kabir, E., and Brown, R. J. C.: A review of airborne polycyclic aromatic hydrocarbons (PAHs) and their human health effects, Environ. Int., 60, 71–80, https://doi.org/10.1016/j.envint.2013.07.019, 2013. a
Kubicki, J. D.: Molecular simulations of benzene and PAH interactions with soot, Environ. Sci. Technol., 40, 2298–2303, https://doi.org/10.1021/es051083s, 2006. a, b
Lammel, G., Sehili, A. M., Bond, T. C., Feichter, J., and Grassl, H.: Gas/particle partitioning and global distribution of polycyclic aromatic hydrocarbons – A modelling approach, Chemosphere, 76, 98–106, https://doi.org/10.1016/j.chemosphere.2009.02.017, 2009. a
Lammel, G., Klánová, J., Ilić, P., Kohoutek, J., Gasić, B., Kovacić, I., and Škrdlíková, L.: Polycyclic aromatic hydrocarbons in air on small spatial and temporal scales – II. Mass size distributions and gas-particle partitioning, Atmos. Environ., 44, 5022–5027, https://doi.org/10.1016/j.atmosenv.2010.08.001, 2010. a
Lammel, G., Kitanovski, Z., Kukučka, P., Novák, J., Arangio, A. M., Codling, G. P., Filippi, A., Hovorka, J., Kuta, J., Leoni, C., Příbylová, P., Prokeš, R., Sáňka, O., Shahpoury, P., Tong, H., and Wietzoreck, M.: Oxygenated and nitrated polycyclic aromatic hydrocarbons in ambient air–levels, phase partitioning, mass size distributions, and inhalation bioaccessibility, Environ. Sci. Technol., 54, 2615–2625, 2020. a
Lazar, P., Karlický, F., Jurečka, P., Kocman, M., Otyepková, E., Šafářová, K., and Otyepka, M.: Adsorption of small organic molecules on graphene, J. Am. Chem. Soc., 135, 6372–6377, https://doi.org/10.1021/ja403162r, 2013. a
Lechner, C. and Sax, A. F.: Adhesive forces between aromatic molecules and graphene, J. Phys. Chem. C, 118, 20970–20981, https://doi.org/10.1021/jp505894p, 2014. a
Li, Y. and Shiraiwa, M.: Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities, Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, 2019. a
Li, Y.-F., Ma, W.-L., and Yang, M.: Prediction of gas/particle partitioning of polybrominated diphenyl ethers (PBDEs) in global air: A theoretical study, Atmos. Chem. Phys., 15, 1669–1681, https://doi.org/10.5194/acp-15-1669-2015, 2015. a
Liu, C., Zhang, Y., and Weschler, C. J.: Exposure to SVOCs from inhaled particles: Impact of desorption, Environ. Sci. Technol., 51, 2615–2625, 2017. a
Liu, Y., Ivanov, A., Zelenov, V., and Molina, M.: Temperature dependence of OH uptake by carbonaceous surfaces of atmospheric importance, Russ. J. Phys. Ch. B, 6, 327–332, 2012. a
Lohmann, R. and Lammel, G.: Adsorptive and absorptive contributions to the gas-particle partitioning of polycyclic aromatic hydrocarbons: State of knowledge and recommended parametrization for modeling, Environ. Sci. Technol., 38, 3793–3803, https://doi.org/10.1021/es035337q, 2004. a
Lohmann, R., Harner, T., Thomas, G. O., and Jones, K. C.: A comparative study of the gas-particle partitioning of PCDD/Fs, PCBs, and PAHs, Environ. Sci. Technol., 34, 4943–4951, https://doi.org/10.1021/es9913232, 2000. a
Mader, B. T. and Pankow, J. F.: Study of the effects of particle-phase carbon on the gas/particle partitioning of semivolatile organic compounds in the atmosphere using controlled field experiments, Environ. Sci. Technol., 36, 5218–5228, https://doi.org/10.1021/es011048v, 2002. a
Mandalakis, M., Tsapakis, M., Tsoga, A., and Stephanou, E. G.: Gas–particle concentrations and distribution of aliphatic hydrocarbons, PAHs, PCBs and PCDD/Fs in the atmosphere of Athens (Greece), Atmos. Environ., 36, 4023–4035, https://doi.org/10.1016/S1352-2310(02)00362-X, 2002. a
Massman, W. J.: A review of the molecular diffusivities of H2O, CO2, CH4, CO, O3, SO2, NH3, N2O, NO, and NO2 in air, O2 and N2 near STP, Atmos. Environ., 32, 1111–1127, https://doi.org/10.1016/S1352-2310(97)00391-9, 1998. a
McFiggans, G. B., Alfarra, M. R., Allan, J., Coe, H., Hamilton, J., Harrison, R., Jenkin, M. E., Lewis, A., Moller, S. J., and Williams, P. I.: A review of the state-of-the-science relating to secondary particulate matter of relevance to the composition of the UK atmosphere: Full technical report to Defra, project AQ0732, 131–165, http://eprints.whiterose.ac.uk/92381/ (last access: 12 April 2021), 2015. a
Meng, Z. and Seinfeld, J. H.: Time scales to achieve atmospheric gas-aerosol equilibrium for volatile species, Atmos. Environ., 30, 2889–2900, https://doi.org/10.1016/1352-2310(95)00493-9, 1996. a
Miguel, A. H., Kirchstetter, T. W., Harley, R. A., and Hering, S. V.: On-road emissions of particulate polycyclic aromatic hydrocarbons and black carbon from gasoline and diesel vehicles, Environ. Sci. Technol., 32, 450–455, https://doi.org/10.1021/es970566w, 1998. a
Mu, Q., Shiraiwa, M., Octaviani, M., Ma, N., Ding, A., Su, H., Lammel, G., Pöschl, U., and Cheng, Y.: Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs, Sci. Adv., 4, eaap7314, https://doi.org/10.1126/sciadv.aap7314, 2018. a
Odum, J. R., Yu, J., and Kamens, R. M.: Modeling the mass transfer of semivolatile organics in combustion aerosols, Environ. Sci. Technol., 28, 2278–2285, https://doi.org/10.1021/es00062a011, 1994. a
Pankow, J. F.: An absorption model of gas/particle partitioning of organic compounds in the atmosphere, Atmos. Environ., 28, 185–188, https://doi.org/10.1016/1352-2310(94)90093-0, 1994. a
Pankow, J. F. and Bidleman, T. F.: Interdependence of the slopes and intercepts from log-log correlations of measured gas-particle paritioning and vapor pressure–I. theory and analysis of available data, Atmos. Environ., 26, 1071–1080, https://doi.org/10.1016/0960-1686(92)90039-N, 1992. a
Pöschl, U.: Atmospheric aerosols: Composition, transformation, climate and health effects, Angew. Chem. Int. Ed., 44, 7520–7540, https://doi.org/10.1002/anie.200501122, 2005. a, b
Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for aerosol and cloud surface chemistry and gas–particle interactions – Part 1: General equations, parameters, and terminology, Atmos. Chem. Phys., 7, 5989–6023, https://doi.org/10.5194/acp-7-5989-2007, 2007. a, b
Ravindra, K., Sokhi, R., and Van Grieken, R.: Atmospheric polycyclic aromatic hydrocarbons: Source attribution, emission factors and regulation, Atmos. Environ., 42, 2895–2921, https://doi.org/10.1016/j.atmosenv.2007.12.010, 2008. a
Rounds, S. A. and Pankow, J. F.: Application of a radial diffusion model to describe gas/particle sorption kinetics, Environ. Sci. Technol., 24, 1378–1386, https://doi.org/10.1021/es00079a012, 1990. a
Saleh, R., Donahue, N. M., and Robinson, A. L.: Time scales for gas-particle partitioning equilibration of secondary organic aerosol formed from alpha-pinene ozonolysis, Environ. Sci. Technol., 47, 5588–5594, https://doi.org/10.1021/es400078d, 2013. a
Sehili, A. M. and Lammel, G.: Global fate and distribution of polycyclic aromatic hydrocarbons emitted from Europe and Russia, Atmos. Environ., 41, 8301–8315, https://doi.org/10.1016/j.atmosenv.2007.06.050, 2007. a
Shahpoury, P., Lammel, G., Albinet, A., Sofuoǧlu, A., Dumanoğlu, Y., Sofuoǧlu, S. C., Wagner, Z., and Zdimal, V.: Evaluation of a conceptual model for gas-particle partitioning of polycyclic aromatic hydrocarbons using polyparameter linear free energy relationships, Environ. Sci. Technol., 50, 12312–12319, https://doi.org/10.1021/acs.est.6b02158, 2016. a
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, https://doi.org/10.1029/2012GL054008, 2012. a, b
Shiraiwa, M., Garland, R. M., and Pöschl, U.: Kinetic double-layer model of aerosol surface chemistry and gas-particle interactions (K2-SURF): Degradation of polycyclic aromatic hydrocarbons exposed to O3, NO2, H2O, OH and NO3, Atmos. Chem. Phys., 9, 9571–9586, https://doi.org/10.5194/acp-9-9571-2009, 2009. a, b, c
Shiraiwa, M., Sosedova, Y., Rouvière, A., Yang, H., Zhang, Y., Abbatt, J. P. D., Ammann, M., and Pöschl, U.: The role of long-lived reactive oxygen intermediates in the reaction of ozone with aerosol particles, Nat. Chem, 3, 291–295, https://doi.org/10.1038/nchem.988, 2011. a
Shiraiwa, M., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend, A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA, 110, 11746–11750, https://doi.org/10.1073/pnas.1307501110, 2013. a
Shrivastava, M., Lou, S., Zelenyuk, A., Easter, R. C., Corley, R. A., Thrall, B. D., Rasch, P. J., Fast, J. D., Simonich, S. L. M., Shen, H., and Tao, S.: Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol, P. Natl. Acad. Sci. USA, 114, 1246–1251, https://doi.org/10.1073/pnas.1618475114, 2017. a
Siddiqi, M. A., Siddiqui, R. A., and Atakan, B.: Thermal stability, sublimation pressures, and diffusion coefficients of anthracene, pyrene, and some metal β-diketonates, J. Chem. Eng. Data, 54, 2795–2802, https://doi.org/10.1021/je9001653, 2009. a, b
Škrdlíková, L., Landlová, L., Klánová, J., and Lammel, G.: Wet deposition and scavenging efficiency of gaseous and particulate phase polycyclic aromatic compounds at a central European suburban site, Atmos. Environ., 45, 4305–4312, https://doi.org/10.1016/j.atmosenv.2011.04.072, 2011. a
Stone, D., Whalley, L. K., and Heard, D. E.: Tropospheric OH and HO2 radicals: field measurements and model comparisons, Chem. Soc. Rev., 41, 6348–6404, https://doi.org/10.1039/C2CS35140D, 2012. a
Tang, M. J., Cox, R. A., and Kalberer, M.: Compilation and evaluation of gas phase diffusion coefficients of reactive trace gases in the atmosphere: volume 1. Inorganic compounds, Atmos. Chem. Phys., 14, 9233–9247, https://doi.org/10.5194/acp-14-9233-2014, 2014. a
Terzi, E. and Samara, C.: Gas-particle partitioning of polycyclic aromatic hydrocarbons in urban, adjacent coastal, and continental background sites of Western Greece, Environ. Sci. Technol., 38, 4973–4978, https://doi.org/10.1021/es040042d, 2004. a
Vingarzan, R.: A review of surface ozone background levels and trends, Atmos. Environ., 38, 3431–3442, https://doi.org/10.1016/j.atmosenv.2004.03.030, 2004. a
Wang, T., Xue, L., Brimblecombe, P., Lam, Y. F., Li, L., and Zhang, L.: Ozone pollution in China: A review of concentrations, meteorological influences, chemical precursors, and effects, Sci. Total Environ., 575, 1582–1596, https://doi.org/10.1016/j.scitotenv.2016.10.081, 2017. a
Wei, C., Han, Y., Bandowe, B. A. M., Cao, J., Huang, R.-J., Ni, H., Tian, J., and Wilcke, W.: Occurrence, gas/particle partitioning and carcinogenic risk of polycyclic aromatic hydrocarbons and their oxygen and nitrogen containing derivatives in Xi'an, central China, Sci. Total Environ., 505, 814–822, https://doi.org/10.1016/j.scitotenv.2014.10.054, 2015. a
Wei, W., Ramalho, O., and Mandin, C.: Modeling the bioaccessibility of inhaled semivolatile organic compounds in the human respiratory tract, Int. J. Hyg. Environ. Health, 224, 113436, https://doi.org/10.1016/j.ijheh.2019.113436, 2020. a
Yamasaki, H., Kuwata, K., and Miyamoto, H.: Effects of ambient temperature on aspects of airborne polycyclic aromatic hydrocarbons, Environ. Sci. Technol., 16, 189–194, https://doi.org/10.1021/es00098a003, 1982.
a
Zhang, H., Worton, D. R., Shen, S., Nah, T., Isaacman-VanWertz, G., Wilson, K. R., and Goldstein, A. H.: Fundamental time scales governing organic aerosol multiphase partitioning and oxidative aging, Environ. Sci. Technol., 49, 9768–9777, https://doi.org/10.1021/acs.est.5b02115, 2015. a
Zhang, Q., Gao, R., Xu, F., Zhou, Q., Jiang, G., Wang, T., Chen, J., Hu, J., Jiang, W., and Wang, W.: Role of water molecule in the gas-phase formation process of nitrated polycyclic aromatic hydrocarbons in the atmosphere: A computational study, Environ. Sci. Technol., 48, 5051–5057, https://doi.org/10.1021/es500453g, 2014. a, b
Short summary
This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show...
Altmetrics
Final-revised paper
Preprint