Articles | Volume 19, issue 8
https://doi.org/10.5194/acp-19-5571-2019
© Author(s) 2019. 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-19-5571-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Apr 2019
Research article |
| 29 Apr 2019
| 29 Apr 2019
Insights into the morphology of multicomponent organic and inorganic aerosols from molecular dynamics simulations
Katerina S. Karadima
Department of Chemical Engineering, University of Patras, Patras,
26504, Greece
Institute of Chemical Engineering Sciences (ICE–HT/FORTH), Patras,
26504, Greece
Vlasis G. Mavrantzas
Department of Chemical Engineering, University of Patras, Patras,
26504, Greece
Institute of Chemical Engineering Sciences (ICE–HT/FORTH), Patras,
26504, Greece
Department of Mechanical and Process Engineering, ETH Zürich,
8092 Zurich, Switzerland
Spyros N. Pandis
CORRESPONDING AUTHOR
Department of Chemical Engineering, University of Patras, Patras,
26504, Greece
Institute of Chemical Engineering Sciences (ICE–HT/FORTH), Patras,
26504, Greece
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, PA 15213, USA
Related authors
No articles found.
Anna Maria Neroladaki, Maria Tsagkaraki, Kyriaki Papoutsidaki, Kalliopi Tavernaraki, Filothei Boufidou, Pavlos Zarmpas, Irini Tsiodra, Eleni Liakakou, Aikaterini Bougiatioti, Giorgos Kouvarakis, Nikos Kalivitis, Christos Kaltsonoudis, Athanasios Karagioras, Dimitrios Balis, Konstantinos Mihailidis, Konstantinos Kourtidis, Stelios Myriokefalitakis, Nikos Hatzianastassiou, Spyros N. Pandis, Athanasios Nenes, Nikolaos Mihalopoulos, and Maria Kanakidou
EGUsphere, https://doi.org/10.5194/egusphere-2025-3223, https://doi.org/10.5194/egusphere-2025-3223, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aerosol acidity affects aerosol composition and properties, and therefore climate, human health and ecosystems. We use summer and winter fine aerosol observations at 6 sites across Greece, and a thermodynamic model to calculate the spatial and seasonal variability of aerosol acidity. Aerosols were acidic to moderately acidic and more acidic during summer than winter. The importance of organics for aerosol acidity was small. Depending on location different factors controlled aerosol acidity.
Susanne M. C. Scholz, Vlassis A. Karydis, Georgios I. Gkatzelis, Hendrik Fuchs, Spyros N. Pandis, and Alexandra P. Tsimpidi
EGUsphere, https://doi.org/10.5194/egusphere-2025-2510, https://doi.org/10.5194/egusphere-2025-2510, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
We studied how pollution from cars and trucks contributes to tiny airborne particles that affect air quality and climate. These particles, called secondary organic aerosols, were often underestimated in global models. By improving how certain overlooked emissions from fuel use are represented in our model, we found that their impact is much larger than previously thought. Our results suggest that road traffic plays a far greater role in global air pollution than earlier estimates showed.
Maria P. Georgopoulou, Kalliopi Florou, Angeliki Matrali, Georgia Starida, Christos Kaltsonoudis, Athanasios Nenes, and Spyros N. Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2025-2728, https://doi.org/10.5194/egusphere-2025-2728, 2025
Short summary
Short summary
Residential biomass burning is an important wintertime source of aerosols. This study examined the complex diurnal aging cycles on biomass burning aerosol composition and oxidative potential, a key toxicity metric. Additional organic aerosol (OA) mass was produced after the two (day/night and night/day) cycles, varying from 35 to 90 % of the initial OA. The aging of the emissions led to a final oxidative potential increase of 60 % for both cycles.
Georgia A. Argyropoulou, Kalliopi Florou, and Spyros N. Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2025-1147, https://doi.org/10.5194/egusphere-2025-1147, 2025
Short summary
Short summary
Ultrafine particles (diameter less than 100 nm) are suspected to cause significant health effects. Accurately measuring their chemical composition and physical properties in real-time is challenging due to their low mass and interference from larger particles. This study proposes a method for the continuous, automated measurement of their composition, tested in a pilot field study to explore their chemical characteristics, physical properties, and sources.
David Patoulias, Kalliopi Florou, and Spyros N. Pandis
Geosci. Model Dev., 18, 1103–1118, https://doi.org/10.5194/gmd-18-1103-2025, https://doi.org/10.5194/gmd-18-1103-2025, 2025
Short summary
Short summary
The effect of the assumed atmospheric nucleation mechanism on particle number concentrations and size distribution was investigated. Two quite different mechanisms involving sulfuric acid and ammonia or a biogenic organic vapor gave quite similar results which were consistent with measurements at 26 measurement stations across Europe. The number of larger particles that serve as cloud condensation nuclei showed little sensitivity to the assumed nucleation mechanism.
Andreas Aktypis, Dontavious J. Sippial, Christina N. Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 13769–13791, https://doi.org/10.5194/acp-24-13769-2024, https://doi.org/10.5194/acp-24-13769-2024, 2024
Short summary
Short summary
A dual-chamber system was deployed in two different environments (Po Valley, Italy, and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary organic aerosol (SOA). In the Po Valley, the system reacts rapidly, forming large amounts of SOA, while in Pertouli the SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Konstantinos Mataras, Evangelia Siouti, David Patoulias, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3357, https://doi.org/10.5194/egusphere-2024-3357, 2024
Short summary
Short summary
Predicted levels of ultrafine particle mass (PM0.1) vary substantially over Europe with higher values in the summer than in the winter. In summer, PM0.1 was mostly comprised of sulfate (38 %) and secondary organics (32 %). During winter the sulfate fraction increased to 47 % and primary organics contributed 23 %. Correlations between PM0.1 and the regulated PM2.5 were low. This suggests that there are significant differences between the dominant sources and processes of PM0.1 and PM2.5.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
Short summary
Short summary
Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allows for novel model constraints and remote sensing products.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
Short summary
Short summary
Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Olga Zografou, Christos Kaltsonoudis, Maria Gini, Angeliki Matrali, Elias Panagiotopoulos, Alexandros Lekkas, Dimitris Papanastasiou, Spyros N. Pandis, and Konstantinos Eleftheriadis
EGUsphere, https://doi.org/10.5194/egusphere-2024-2126, https://doi.org/10.5194/egusphere-2024-2126, 2024
Preprint archived
Short summary
Short summary
A novel charge transfer ionization orthogonal Time-of-Flight Mass Spectrometer (oToF-MS) was field evaluated for the first time during a field campaign at the suburban DEM station in Athens, Greece from May to August 2023 focusing on key ambient Volatile Organic Compounds (VOCs). The results demonstrate the strengths of the new instrument in performing online, real time measurements of ambient VOCs.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
Short summary
Short summary
This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
Short summary
Short summary
Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Andreas Aktypis, Christos Kaltsonoudis, David Patoulias, Panayiotis Kalkavouras, Angeliki Matrali, Christina N. Vasilakopoulou, Evangelia Kostenidou, Kalliopi Florou, Nikos Kalivitis, Aikaterini Bougiatioti, Konstantinos Eleftheriadis, Stergios Vratolis, Maria I. Gini, Athanasios Kouras, Constantini Samara, Mihalis Lazaridis, Sofia-Eirini Chatoutsidou, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 65–84, https://doi.org/10.5194/acp-24-65-2024, https://doi.org/10.5194/acp-24-65-2024, 2024
Short summary
Short summary
Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation. The frequency during summer varied from close to zero in southwestern Greece to more than 60 % in the northern, central, and eastern regions. The spatial variability can be explained by the proximity of the sites to coal-fired power plants and agricultural areas.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
Short summary
Short summary
Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
Short summary
Short summary
Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
Short summary
Short summary
In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Christina N. Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 2837–2850, https://doi.org/10.5194/amt-16-2837-2023, https://doi.org/10.5194/amt-16-2837-2023, 2023
Short summary
Short summary
The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol in areas and periods during which an aerosol mass spectrometer is not available. In this work, an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing the uncertainty of the corresponding source apportionment significantly.
Spiro D. Jorga, Kalliopi Florou, David Patoulias, and Spyros N. Pandis
Atmos. Chem. Phys., 23, 85–97, https://doi.org/10.5194/acp-23-85-2023, https://doi.org/10.5194/acp-23-85-2023, 2023
Short summary
Short summary
We take advantage of this unexpected low, new particle formation frequency in Greece and use a dual atmospheric simulation chamber system with starting point ambient air in an effort to gain insight about the chemical species that is limiting nucleation in this area. A potential nucleation precursor, ammonia, was added in one of the chambers while the other one was used as a reference. The addition of ammonia assisted new particle formation in almost 50 % of the experiments conducted.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
Short summary
Short summary
The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 15, 6419–6431, https://doi.org/10.5194/amt-15-6419-2022, https://doi.org/10.5194/amt-15-6419-2022, 2022
Short summary
Short summary
Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols when online AMS measurements are not available. In this study, we examine whether and how the low time resolution (usually 24 h) of the offline technique affects source apportionment results. We concluded that use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis.
Stella E. I. Manavi and Spyros N. Pandis
Geosci. Model Dev., 15, 7731–7749, https://doi.org/10.5194/gmd-15-7731-2022, https://doi.org/10.5194/gmd-15-7731-2022, 2022
Short summary
Short summary
The paper describes the first step towards the development of a simulation framework for the chemistry and secondary organic aerosol production of intermediate-volatility organic compounds (IVOCs). These compounds can be a significant source of organic particulate matter. Our approach treats IVOCs as lumped compounds that retain their chemical characteristics. Estimated IVOC emissions from road transport were a factor of 8 higher than emissions used in previous applications.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
Short summary
Short summary
The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
Short summary
Short summary
A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
Short summary
Short summary
The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys., 22, 1689–1706, https://doi.org/10.5194/acp-22-1689-2022, https://doi.org/10.5194/acp-22-1689-2022, 2022
Short summary
Short summary
Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low-volatility organic compounds have a smaller-than-expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate-volatility organic compounds leads to decreases in the ultrafine-particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
Short summary
Short summary
An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
Short summary
Short summary
Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
Short summary
Short summary
We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
Short summary
Short summary
Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
Short summary
Short summary
Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
Short summary
Short summary
Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
Short summary
Short summary
Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
Short summary
Short summary
The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Antonios Tasoglou, Evangelos Louvaris, Kalliopi Florou, Aikaterini Liangou, Eleni Karnezi, Christos Kaltsonoudis, Ningxin Wang, and Spyros N. Pandis
Atmos. Chem. Phys., 20, 11625–11637, https://doi.org/10.5194/acp-20-11625-2020, https://doi.org/10.5194/acp-20-11625-2020, 2020
Short summary
Short summary
A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption. The measured light absorption was two or more times higher than that of fresh black carbon. The absorption enhancement due to the coating of black carbon cores by other aerosol components could explain only part of this absorption enhancement. The rest was due to brown carbon, mostly in the form of extremely low volatility organic compounds.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
Short summary
Short summary
We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
Short summary
Short summary
We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Christos Kaltsonoudis, Spiro D. Jorga, Evangelos Louvaris, Kalliopi Florou, and Spyros N. Pandis
Atmos. Meas. Tech., 12, 2733–2743, https://doi.org/10.5194/amt-12-2733-2019, https://doi.org/10.5194/amt-12-2733-2019, 2019
Short summary
Short summary
A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers surrounded by UV lamps. The system has been designed to use ambient air as the starting point of the experiments. It can be easily disassembled and transported, enabling the study of various atmospheric environments and it can be used with natural sunlight. The results of test experiments using ambient air are discussed as examples of applications of this system.
Georgia N. Theodoritsi and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5403–5415, https://doi.org/10.5194/acp-19-5403-2019, https://doi.org/10.5194/acp-19-5403-2019, 2019
Short summary
Short summary
The chemical transport model PMCAMx was extended to investigate the effects of partitioning and photochemical aging of biomass burning emissions on organic aerosol (OA) concentrations and was applied in Europe. During the summer, the contribution of biomass burning to total OA levels over continental Europe was 16 % and during winter 47 %. Intermediate volatility organic compounds are predicted to be important precursors of secondary OA from biomass burning.
Anthoula D. Drosatou, Ksakousti Skyllakou, Georgia N. Theodoritsi, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 973–986, https://doi.org/10.5194/acp-19-973-2019, https://doi.org/10.5194/acp-19-973-2019, 2019
Short summary
Short summary
The ability of positive matrix factorization (PMF) factor analysis to identify and quantify the organic aerosol (OA) sources accurately is tested in this modeling study. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources is less than 40 %, when these sources contribute more than 20 % to the OA. Τhe first oxygenated OA factor includes mainly highly aged OA, while the second oxygenated OA factor contains fresher secondary OA.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
Short summary
Short summary
The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
Short summary
Short summary
PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
Short summary
Short summary
A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
Short summary
Short summary
Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
Short summary
Short summary
The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
Short summary
Short summary
This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
Kerrigan P. Cain and Spyros N. Pandis
Atmos. Meas. Tech., 10, 4865–4876, https://doi.org/10.5194/amt-10-4865-2017, https://doi.org/10.5194/amt-10-4865-2017, 2017
Short summary
Short summary
Hygroscopicity, oxidation level, and volatility of organic pollutants are three crucial properties that determine their fate in the atmosphere. This study assesses the feasibility of a novel measurement and analysis technique to determine these properties of organic aerosol
components at the same time and to establish their relationship.
Evangelos E. Louvaris, Eleni Karnezi, Evangelia Kostenidou, Christos Kaltsonoudis, and Spyros N. Pandis
Atmos. Meas. Tech., 10, 3909–3918, https://doi.org/10.5194/amt-10-3909-2017, https://doi.org/10.5194/amt-10-3909-2017, 2017
Short summary
Short summary
A method for the determination of the organic aerosol volatility distribution combining thermodenuder and isothermal dilution measurements is developed. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol produced during meat charbroiling. Addition of the dilution measurements to the thermodenuder data results in a lower uncertainty of the estimated vaporization enthalpy as well as the semivolatile content of the aerosol.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
Short summary
Short summary
We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Christos Kaltsonoudis, Evangelia Kostenidou, Evangelos Louvaris, Magda Psichoudaki, Epameinondas Tsiligiannis, Kalliopi Florou, Aikaterini Liangou, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 7143–7155, https://doi.org/10.5194/acp-17-7143-2017, https://doi.org/10.5194/acp-17-7143-2017, 2017
Short summary
Short summary
Cooking emissions can be a significant source of particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. More than 99% of the aerosol emitted was composed of organic compounds. The fresh particles were similar to the cooking organic aerosol over Greek cities during the winter, while the reacted particles were similar to those found in the atmosphere during the summer.
Kalliopi Florou, Dimitrios K. Papanastasiou, Michael Pikridas, Christos Kaltsonoudis, Evangelos Louvaris, Georgios I. Gkatzelis, David Patoulias, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 3145–3163, https://doi.org/10.5194/acp-17-3145-2017, https://doi.org/10.5194/acp-17-3145-2017, 2017
Short summary
Short summary
The composition of fine particulate matter (PM) in two major Greek cities (Athens and Patras) was measured during two wintertime campaigns in 2012 and 2013. Residential wood burning has dramatically increased due to the Greek financial crisis, contributing around 50 % of the fine PM on average and more than 80 % during nighttime. Cooking is also an important source during both midday and evening, while transportation dominates only during the morning rush hour.
Christos Kaltsonoudis, Evangelia Kostenidou, Kalliopi Florou, Magda Psichoudaki, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 14825–14842, https://doi.org/10.5194/acp-16-14825-2016, https://doi.org/10.5194/acp-16-14825-2016, 2016
Short summary
Short summary
Volatile organic compounds (VOCs) were monitored in urban backgrounds sites, in Athens and Patras in Greece. In summer most of the measured VOCs were due to biogenic and traffic emissions. Winter measurements in Athens revealed that biomass burning used for residential heating was the dominant VOC source. The biomass burning VOC emission ratios and emission factors were estimated.
Antigoni Panagiotopoulou, Panagiotis Charalampidis, Christos Fountoukis, Christodoulos Pilinis, and Spyros N. Pandis
Geosci. Model Dev., 9, 4257–4272, https://doi.org/10.5194/gmd-9-4257-2016, https://doi.org/10.5194/gmd-9-4257-2016, 2016
Short summary
Short summary
The ability of chemical transport model PMCAMx to reproduce ground and satellite aerosol optical depth (AOD) measurements over Europe is evaluated. PMCAMx reproduces AOD values over Spain, the UK, central Europe, and Russia with a fractional bias of less than 15 % and a fractional error of less than 30 %. The model overestimates the AOD over northern Europe probably due to an overestimation of organic aerosol and sulfates, and underestimates over the Balkans due to an underestimation of sulfates.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
Short summary
Short summary
The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
Short summary
Short summary
In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Christos Fountoukis, Athanasios G. Megaritis, Ksakousti Skyllakou, Panagiotis E. Charalampidis, Hugo A. C. Denier van der Gon, Monica Crippa, André S. H. Prévôt, Friederike Fachinger, Alfred Wiedensohler, Christodoulos Pilinis, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 3727–3741, https://doi.org/10.5194/acp-16-3727-2016, https://doi.org/10.5194/acp-16-3727-2016, 2016
Short summary
Short summary
We use PMCAMx with high grid resolution over Paris to simulate carbonaceous aerosol during the summer and winter MEGAPOLI campaigns. PMCAMx reproduces BC observations well. Addition of cooking organic aerosol emissions of 80 mg per day per capita is needed to reproduce the corresponding observations. While the oxygenated organic aerosol predictions during the summer are encouraging a major wintertime source appears to be missing.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
Short summary
Short summary
We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
G. I. Gkatzelis, D. K. Papanastasiou, K. Florou, C. Kaltsonoudis, E. Louvaris, and S. N. Pandis
Atmos. Meas. Tech., 9, 103–114, https://doi.org/10.5194/amt-9-103-2016, https://doi.org/10.5194/amt-9-103-2016, 2016
Short summary
Short summary
A method for the measurement of the nonvolatile atmospheric particle size distribution is developed and tested. The tests include laboratory experiments with biogenic and anthropogenic secondary organic aerosol as well as nucleation experiments with ambient air. The method is then further tested during an ambient campaign.
E. Kostenidou, K. Florou, C. Kaltsonoudis, M. Tsiflikiotou, S. Vratolis, K. Eleftheriadis, and S. N. Pandis
Atmos. Chem. Phys., 15, 11355–11371, https://doi.org/10.5194/acp-15-11355-2015, https://doi.org/10.5194/acp-15-11355-2015, 2015
Short summary
Short summary
The concentration and chemical composition of fine particulate matter were measured during the summer of 2012 in two Greek cities, Patras and Athens. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources. Analysis of the Aerosol Mass Spectrometer data suggested that the contribution of the primary sources to organic aerosol was important (22% in Patras and 35% in Athens) but not dominant.
M. Pikridas, J. Sciare, F. Freutel, S. Crumeyrolle, S.-L. von der Weiden-Reinmüller, A. Borbon, A. Schwarzenboeck, M. Merkel, M. Crippa, E. Kostenidou, M. Psichoudaki, L. Hildebrandt, G. J. Engelhart, T. Petäjä, A. S. H. Prévôt, F. Drewnick, U. Baltensperger, A. Wiedensohler, M. Kulmala, M. Beekmann, and S. N. Pandis
Atmos. Chem. Phys., 15, 10219–10237, https://doi.org/10.5194/acp-15-10219-2015, https://doi.org/10.5194/acp-15-10219-2015, 2015
Short summary
Short summary
Aerosol size distribution measurements from three ground sites, two mobile laboratories, and one airplane are combined to investigate the spatial and temporal variability of ultrafine particles in and around Paris during the summer and winter MEGAPOLI campaigns. The role of nucleation as a particle source and the influence of Paris emissions on their surroundings are examined.
M. Beekmann, A. S. H. Prévôt, F. Drewnick, J. Sciare, S. N. Pandis, H. A. C. Denier van der Gon, M. Crippa, F. Freutel, L. Poulain, V. Ghersi, E. Rodriguez, S. Beirle, P. Zotter, S.-L. von der Weiden-Reinmüller, M. Bressi, C. Fountoukis, H. Petetin, S. Szidat, J. Schneider, A. Rosso, I. El Haddad, A. Megaritis, Q. J. Zhang, V. Michoud, J. G. Slowik, S. Moukhtar, P. Kolmonen, A. Stohl, S. Eckhardt, A. Borbon, V. Gros, N. Marchand, J. L. Jaffrezo, A. Schwarzenboeck, A. Colomb, A. Wiedensohler, S. Borrmann, M. Lawrence, A. Baklanov, and U. Baltensperger
Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, https://doi.org/10.5194/acp-15-9577-2015, 2015
Short summary
Short summary
A detailed characterization of air quality in the Paris (France) agglomeration, a megacity, during two summer and winter intensive campaigns and from additional 1-year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported into the megacity from upwind regions. Unexpectedly, a major part of organic PM is of modern origin (woodburning and cooking activities, secondary formation from biogenic VOC).
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
Short summary
Short summary
Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
Short summary
Short summary
Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
D. Patoulias, C. Fountoukis, I. Riipinen, and S. N. Pandis
Atmos. Chem. Phys., 15, 6337–6350, https://doi.org/10.5194/acp-15-6337-2015, https://doi.org/10.5194/acp-15-6337-2015, 2015
Short summary
Short summary
A new aerosol dynamics model (DMANx) describing the organic vapor condensation on nanoparticles based on the volatility basis set framework is used to simulate typical nucleation events in two contrasting environments in Hyytiälä (Finland) and Finokalia (Greece). The role of semivolatile, low, and extremely low volatility organics and the corresponding surface energies is investigated.
I. Riipinen, N. Rastak, and S. N. Pandis
Atmos. Chem. Phys., 15, 6305–6322, https://doi.org/10.5194/acp-15-6305-2015, https://doi.org/10.5194/acp-15-6305-2015, 2015
Short summary
Short summary
Atmospheric organic aerosol is complex and thus a challenge to model. We introduce a theoretical framework (solubility distributions) to represent the solubility of multicomponent mixtures. Using the framework, we evaluate the commonly made assumptions about the cloud condensation nucleus (CCN) activity of organic mixtures. We find that material with water solubilities larger than 0.1-100 g/L can usually be treated as completely soluble, which simplifies the treatment of organic CCN.
A. Tasoglou and S. N. Pandis
Atmos. Chem. Phys., 15, 6035–6046, https://doi.org/10.5194/acp-15-6035-2015, https://doi.org/10.5194/acp-15-6035-2015, 2015
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
Short summary
Short summary
A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
A. G. Megaritis, C. Fountoukis, P. E. Charalampidis, H. A. C. Denier van der Gon, C. Pilinis, and S. N. Pandis
Atmos. Chem. Phys., 14, 10283–10298, https://doi.org/10.5194/acp-14-10283-2014, https://doi.org/10.5194/acp-14-10283-2014, 2014
E. Karnezi, I. Riipinen, and S. N. Pandis
Atmos. Meas. Tech., 7, 2953–2965, https://doi.org/10.5194/amt-7-2953-2014, https://doi.org/10.5194/amt-7-2953-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
B. N. Murphy, N. M. Donahue, A. L. Robinson, and S. N. Pandis
Atmos. Chem. Phys., 14, 5825–5839, https://doi.org/10.5194/acp-14-5825-2014, https://doi.org/10.5194/acp-14-5825-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
K. Skyllakou, B. N. Murphy, A. G. Megaritis, C. Fountoukis, and S. N. Pandis
Atmos. Chem. Phys., 14, 2343–2352, https://doi.org/10.5194/acp-14-2343-2014, https://doi.org/10.5194/acp-14-2343-2014, 2014
L. Ahlm, J. Julin, C. Fountoukis, S. N. Pandis, and I. Riipinen
Atmos. Chem. Phys., 13, 10271–10283, https://doi.org/10.5194/acp-13-10271-2013, https://doi.org/10.5194/acp-13-10271-2013, 2013
E. Kostenidou, C. Kaltsonoudis, M. Tsiflikiotou, E. Louvaris, L. M. Russell, and S. N. Pandis
Atmos. Chem. Phys., 13, 8797–8811, https://doi.org/10.5194/acp-13-8797-2013, https://doi.org/10.5194/acp-13-8797-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
E. Athanasopoulou, H. Vogel, B. Vogel, A. P. Tsimpidi, S. N. Pandis, C. Knote, and C. Fountoukis
Atmos. Chem. Phys., 13, 625–645, https://doi.org/10.5194/acp-13-625-2013, https://doi.org/10.5194/acp-13-625-2013, 2013
V.-M. Kerminen, M. Paramonov, T. Anttila, I. Riipinen, C. Fountoukis, H. Korhonen, E. Asmi, L. Laakso, H. Lihavainen, E. Swietlicki, B. Svenningsson, A. Asmi, S. N. Pandis, M. Kulmala, and T. Petäjä
Atmos. Chem. Phys., 12, 12037–12059, https://doi.org/10.5194/acp-12-12037-2012, https://doi.org/10.5194/acp-12-12037-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Regional variability of aerosol impacts on clouds and radiation in global kilometer-scale simulations
A novel method to quantify the uncertainty contribution of aerosol–radiation interaction factors
Exploring the aerosol activation properties in coastal shallow convection using cloud- and particle-resolving models
Machine-learning-assisted inference of the particle charge fraction and the ion-induced nucleation rates during new particle formation events
Modeling CMAQ dry deposition treatment over the western Pacific: a distinct characteristic of mineral dust and anthropogenic aerosols
Impact of post-monsoon crop residue burning on PM2.5 over northern India: optimizing emissions using a high-density in situ surface observation network
Modeling simulation of aerosol light absorption over the Beijing–Tianjin–Hebei region: the impact of mixing state and aging processes
An investigation of the impact of Canadian wildfires on US air quality using model, satellite, and ground measurements
How to trace the origins of short-lived atmospheric species: an Arctic example
Dust-producing weather patterns of the North American Great Plains
High-resolution air quality maps for Bucharest using a mixed-effects modeling framework
Interdecadal shift in the impact of winter land-sea thermal contrasts on following spring transcontinental dust transport pathways in North Africa
Anthropogenic and Natural Causes for the Interannual Variation of PM2.5 in East Asia During Summer Monsoon Periods From 2008 to 2018
Construction and application of a pollen emissions model based on phenology and random forests
An uncertain future for the climate and health impacts of anthropogenic aerosols in Africa
The impact of uncertainty in black carbon's refractive index on simulated optical depth and radiative forcing
Gas-phase collision rate enhancement factors for acid-base clusters up to 2 nm in diameter from atomistic simulation and the interacting hard sphere model
How well are aerosol–cloud interactions represented in climate models? – Part 2: Isolating the aerosol impact on clouds following the 2014–15 Holuhraun eruption
Characterization of brown carbon absorption in different European environments through source contribution analysis
Accounting for the black carbon aging process in a two-way coupled meteorology–air quality model
The effectiveness of solar radiation management using fine sea spray across multiple climatic regions
A global dust emission dataset for estimating dust radiative forcings in climate models
Tropospheric aerosols over the western North Atlantic Ocean during the winter and summer deployments of ACTIVATE 2020: life cycle, transport, and distribution
Spatial and temporal evolution of future atmospheric reactive nitrogen deposition in China under different climate change mitigation strategies
Steady-state mixing state of black carbon aerosols from a particle-resolved model
Direct radiative forcing of light-absorbing carbonaceous aerosol and the influencing factors over China
Distinctive dust weather intensities in North China resulted from two types of atmospheric circulation anomalies
Biomass burning emission analysis based on MODIS aerosol optical depth and AeroCom multi-model simulations: implications for model constraints and emission inventories
The effect of organic nucleation on the indirect radiative forcing with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)
Quasi-weekly oscillation of regional PM2.5 transport over China driven by the synoptic-scale disturbance of the East Asian winter monsoon circulation
Solar radiation estimation in West Africa: impact of dust conditions during the 2021 dry season
Modeling urban pollutant transport at multi-resolutions: Impacts of turbulent mixing
Homogeneous ice nucleation in adsorbed water films: A theoretical approach
Gaps in our understanding of ice-nucleating particle sources exposed by global simulation of the UK Earth System Model
The role of interfacial tension in the size-dependent phase separation of atmospheric aerosol particles
Saharan dust linked to European hail events
Impact of Topographic Wind Conditions on Dust Particle Size Distribution: Insights from a Regional Dust Reanalysis Dataset
Uncovering the Impact of Urban Functional Zones on Air Quality in China
Seasonal differences in observed versus modeled new particle formation over boreal regions
Warming effects of reduced sulfur emissions from shipping
The key role of atmospheric absorption in the Asian summer monsoon response to dust emissions in CMIP6 models
Multi-model effective radiative forcing of the 2020 sulfur cap for shipping
Representation of iron aerosol size distributions of anthropogenic emissions is critical in evaluating atmospheric soluble iron input to the ocean
Radiative and climate effects of aerosol scattering in long-wave radiation based on global climate modeling
Revealing dominant patterns of aerosol regimes in the lower troposphere and their evolution from preindustrial times to the future in global climate model simulations
Improving estimation of a record-breaking east Asian dust storm emission with lagged aerosol Ångström exponent observations
Impact of biomass burning aerosols (BBA) on the tropical African climate in an ocean–atmosphere–aerosol coupled climate model
Retrieval of refractive index and water content for the coating materials of aged black carbon aerosol based on optical properties: a theoretical analysis
Strong inter-model differences and biases in CMIP6 simulations of PM2.5, aerosol optical depth, and precipitation over Africa
Predicting hygroscopic growth of organosulfur aerosol particles using COSMOtherm
Ross J. Herbert, Andrew I. L. Williams, Philipp Weiss, Duncan Watson-Parris, Elisabeth Dingley, Daniel Klocke, and Philip Stier
Atmos. Chem. Phys., 25, 7789–7814, https://doi.org/10.5194/acp-25-7789-2025, https://doi.org/10.5194/acp-25-7789-2025, 2025
Short summary
Short summary
Clouds exist at scales that climate models struggle to represent, limiting our knowledge of how climate change may impact clouds. Here we use a new kilometer-scale global model representing an important step towards the necessary scale. We focus on how aerosol particles modify clouds, radiation, and precipitation. We find the magnitude and manner of responses tend to vary from region to region, highlighting the potential of global kilometer-scale simulations and a need to represent aerosols in climate models.
Bishuo He and Chunsheng Zhao
Atmos. Chem. Phys., 25, 7765–7776, https://doi.org/10.5194/acp-25-7765-2025, https://doi.org/10.5194/acp-25-7765-2025, 2025
Short summary
Short summary
Factor uncertainty analysis helps us understand the impacts of factors on complex systems. Traditional methods have many limitations. This study introduces a new method to measure how each factor contributes to uncertainty. It gains insights into the role of each variable and works for all multi-factor systems. As an application, we analyzed how aerosols affect solar radiation and identified the key factors. These analyses can improve our understanding of the role of aerosols in climate change.
Ge Yu, Yueya Wang, Zhe Wang, and Xiaoming Shi
Atmos. Chem. Phys., 25, 7527–7542, https://doi.org/10.5194/acp-25-7527-2025, https://doi.org/10.5194/acp-25-7527-2025, 2025
Short summary
Short summary
Studying the cloud-forming capacity of aerosols is crucial in climate research. The PartMC model can provide detailed particle information and help these studies. This model is integrated with the ideal meteorological Cloud Model 1 (CM1) to simulate the aerosols at cloud-forming locations. Significant changes are revealed in the hygroscopicity distribution of aerosols within ascending air parcels. Additionally, different ascent times also affect aerosol aging processes.
Pan Wang, Yue Zhao, Jiandong Wang, Veli-Matti Kerminen, Jingkun Jiang, and Chenxi Li
Atmos. Chem. Phys., 25, 7431–7446, https://doi.org/10.5194/acp-25-7431-2025, https://doi.org/10.5194/acp-25-7431-2025, 2025
Short summary
Short summary
We developed a numerical model to investigate the evolution of the charge state of newly formed atmospheric particles. Based on the simulation results, we successfully employed neural networks to predict particle charge states and estimate ion-induced nucleation rates. This study provides new insights into the dynamics of particle charging and introduces advanced methods for evaluating ion-induced nucleation in atmospheric research.
Steven Soon-Kai Kong, Joshua S. Fu, Neng-Huei Lin, Guey-Rong Sheu, and Wei-Syun Huang
Atmos. Chem. Phys., 25, 7245–7268, https://doi.org/10.5194/acp-25-7245-2025, https://doi.org/10.5194/acp-25-7245-2025, 2025
Short summary
Short summary
The accuracy of the chemical transport model, a key focus of our research, is strongly dependent on the dry deposition parameterization. Our findings show that the refined CMAQ dust model correlated well with ground-based and high-altitude in situ measurements by implementing the suggested dry deposition schemes. Furthermore, we reveal the mixing state of two types of aerosols at the upper level, a finding supported by both the optimized model and measurements.
Mizuo Kajino, Kentaro Ishijima, Joseph Ching, Kazuyo Yamaji, Rio Ishikawa, Tomoki Kajikawa, Tanbir Singh, Tomoki Nakayama, Yutaka Matsumi, Koyo Kojima, Taisei Machida, Takashi Maki, Prabir K. Patra, and Sachiko Hayashida
Atmos. Chem. Phys., 25, 7137–7160, https://doi.org/10.5194/acp-25-7137-2025, https://doi.org/10.5194/acp-25-7137-2025, 2025
Short summary
Short summary
Air pollution in Delhi during the post-monsoon period is severe, and association with intensive crop residue burning (CRB) over Punjab state has attracted attention. However, the relationship has been unclear as the CRB emissions conventionally derived from satellites were underestimated due to clouds or thick smoke/haze over the region. We evaluated the impact of CRB on PM2.5 to be about 50 %, based on a combination of numerical modeling and an observation network using low-cost sensors we installed.
Huiyun Du, Jie Li, Xueshun Chen, Gabriele Curci, Fangqun Yu, Yele Sun, Xu Dao, Song Guo, Zhe Wang, Wenyi Yang, Lianfang Wei, and Zifa Wang
Atmos. Chem. Phys., 25, 5665–5681, https://doi.org/10.5194/acp-25-5665-2025, https://doi.org/10.5194/acp-25-5665-2025, 2025
Short summary
Short summary
Inadequate consideration of mixing states and coatings on black carbon (BC) hinders aerosol radiation forcing quantification. Core–shell mixing aligns well with observations, but partial internal mixing is a more realistic representation. We used a microphysics module to determine the fraction of embedded BC and coating aerosols, constraining the mixing state. This reduced absorption enhancement by 30 %–43 % in northern China, offering insights into BC's radiative effects.
Zhixin Xue, Nair Udaysankar, and Sundar A. Christopher
Atmos. Chem. Phys., 25, 5497–5517, https://doi.org/10.5194/acp-25-5497-2025, https://doi.org/10.5194/acp-25-5497-2025, 2025
Short summary
Short summary
Canadian wildfires in August 2018 significantly increased surface air pollution across the United States (US) – by up to 69 % in some areas. Using model, satellite, and ground measurements, the study highlights how weather patterns and long-range smoke transport drive pollution. The northwestern US was most affected by Canadian wildfire smoke, while the northeastern US experienced the least impact. These findings indicate the growing concern that wildfire smoke poses to air quality across the US.
Anderson Da Silva, Louis Marelle, Jean-Christophe Raut, Yvette Gramlich, Karolina Siegel, Sophie L. Haslett, Claudia Mohr, and Jennie L. Thomas
Atmos. Chem. Phys., 25, 5331–5354, https://doi.org/10.5194/acp-25-5331-2025, https://doi.org/10.5194/acp-25-5331-2025, 2025
Short summary
Short summary
Particle sources in polar climates are unclear, affecting climate representation in models. This study introduces an evaluated method for tracking particles with backward modeling. Tests on simulated particles allowed us to show that traditional detection methods often misidentify sources. An improved method that accurately traces the origins of aerosol particles in the Arctic is presented. The study recommends using this enhanced method for better source identification of atmospheric species.
Stuart Evans
Atmos. Chem. Phys., 25, 4833–4845, https://doi.org/10.5194/acp-25-4833-2025, https://doi.org/10.5194/acp-25-4833-2025, 2025
Short summary
Short summary
This study of the North American Great Plains identifies the various weather patterns responsible for blowing dust in all parts of the region using a weather pattern classification. In the southwestern plains passing cold fronts are the primary cause of dust; in the understudied northern plains, summertime patterns and southerly pre-frontal winds are most important in the west and east, respectively. These results are valuable to understanding and forecasting dust in this complex source region.
Camelia Talianu, Jeni Vasilescu, Doina Nicolae, Alexandru Ilie, Andrei Dandocsi, Anca Nemuc, and Livio Belegante
Atmos. Chem. Phys., 25, 4639–4654, https://doi.org/10.5194/acp-25-4639-2025, https://doi.org/10.5194/acp-25-4639-2025, 2025
Short summary
Short summary
For Bucharest, Romania's capital, mobile measurements during two intensive campaigns and mixed-effect LUR (land-use regression) models to derive seasonal maps of near-surface PM10, NO2 and UFPs (ultrafine particles) have successfully been used. The model's performance was evaluated, demonstrating its potential for high-resolution mapping in other cities with well-characterized urban structures and diverse in situ monitoring stations.
Qi Wen, Yan Li, Mengying Du, Wenjun Song, Linbo Wei, Zhilan Wang, and Xu Li
EGUsphere, https://doi.org/10.5194/egusphere-2025-826, https://doi.org/10.5194/egusphere-2025-826, 2025
Short summary
Short summary
We find that, through an interdecadal phase-locking effect of sea-land thermal forcing-North Atlantic Oscillation-Westerly Jet coupling, springtime dust from North Africa is more likely to be transported eastwards (extending into North America) after the late 1990s, whereas before that time westward transport paths for dust were more frequent. Subject to thermal forcing, wind speed and drought contribute to dust emissions in the two periods, respectively.
Danyang Ma, Min Xie, Huan He, Tijian Wang, Mengzhu Xi, Lingyun Feng, Shuxian Zhang, and Shitong Chen
EGUsphere, https://doi.org/10.5194/egusphere-2025-10, https://doi.org/10.5194/egusphere-2025-10, 2025
Short summary
Short summary
The PM2.5 concentration in China underwent significant changes in 2013. We examined the underlying causes from three perspectives: anthropogenic pollutant emissions, meteorological conditions, and CO2 concentration variations. Our study highlighted the importance of considering the role of CO2 on vegetation when predicting PM2.5 concentrations and developing corresponding control strategies.
Jiangtao Li, Xingqin An, Zhaobin Sun, Caihua Ye, Qing Hou, Yuxin Zhao, and Zhe Liu
Atmos. Chem. Phys., 25, 3583–3602, https://doi.org/10.5194/acp-25-3583-2025, https://doi.org/10.5194/acp-25-3583-2025, 2025
Short summary
Short summary
Climate change and pollution have intensified pollen allergies. We developed a pollen emissions model using phenology and random forests. Key factors affecting annual pollen emissions include temperature, relative humidity and sunshine hours. Pollen dispersal starts around 10 August, peaks around 30 August and ends by 25 September, lasting about 45 d. Over time, annual pollen emissions exhibit significant fluctuations and a downward trend.
Joe Adabouk Amooli, Marianne T. Lund, Sourangsu Chowdhury, Gunnar Myhre, Ane N. Johansen, Bjørn H. Samset, and Daniel M. Westervelt
EGUsphere, https://doi.org/10.5194/egusphere-2025-948, https://doi.org/10.5194/egusphere-2025-948, 2025
Short summary
Short summary
We analyze various projections of African aerosol emissions and their potential impacts on climate and public health. We find that future emissions vary widely across emission projections, with differences in sectoral emission distributions. Using the Oslo chemical transport model, we show that air pollution exposure in some regions of Africa could increase significantly by 2050, increasing pollution-related deaths, with most scenarios projecting aerosol-induced warming over sub-Saharan Africa.
Ruth A. R. Digby, Knut von Salzen, Adam H. Monahan, Nathan P. Gillett, and Jiangnan Li
Atmos. Chem. Phys., 25, 3109–3130, https://doi.org/10.5194/acp-25-3109-2025, https://doi.org/10.5194/acp-25-3109-2025, 2025
Short summary
Short summary
The refractive index of black carbon (BCRI), which determines how much energy black carbon absorbs and scatters, is difficult to measure, and different climate models use different values. We show that varying the BCRI across commonly used values can increase absorbing aerosol optical depth by 42 % and the warming effect from interactions between black carbon and radiation by 47 %, an appreciable fraction of the overall spread between models reported in recent literature assessments.
Valtteri Tikkanen, Huan Yang, Hanna Vehkamäki, and Bernhard Reischl
EGUsphere, https://doi.org/10.5194/egusphere-2025-507, https://doi.org/10.5194/egusphere-2025-507, 2025
Short summary
Short summary
Collisions of neutral molecules and clusters is the prevalent pathway in atmospheric new particle formation. In heavily polluted urban areas, where clusters are formed rapidly and in large number, cluster-cluster collisions also become relevant. We calculate cluster-cluster collision rates from atomistic molecular dynamics simulations and an interacting hard sphere model. Not accounting for long-range attractive interactions underestimates collision and particle formation rates significantly.
George Jordan, Florent Malavelle, Jim Haywood, Ying Chen, Ben Johnson, Daniel Partridge, Amy Peace, Eliza Duncan, Duncan Watson-Parris, David Neubauer, Anton Laakso, Martine Michou, and Pierre Nabat
EGUsphere, https://doi.org/10.5194/egusphere-2025-835, https://doi.org/10.5194/egusphere-2025-835, 2025
Short summary
Short summary
The 2014–15 Holuhraun eruption created a vast aerosol plume that acted as a natural experiment to assess how well climate models capture changes in cloud properties due to increased aerosol. We find that the models accurately represent the observed shift to smaller, more numerous cloud droplets. However, the models diverge in their aerosol induced changes to large-scale cloud properties, particularly cloud liquid water content. Our study shows that Holuhraun had a cooling effect on the Earth.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
Short summary
Short summary
Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Yuzhi Jin, Jiandong Wang, Chao Liu, David C. Wong, Golam Sarwar, Kathleen M. Fahey, Shang Wu, Jiaping Wang, Jing Cai, Zeyuan Tian, Zhouyang Zhang, Jia Xing, Aijun Ding, and Shuxiao Wang
Atmos. Chem. Phys., 25, 2613–2630, https://doi.org/10.5194/acp-25-2613-2025, https://doi.org/10.5194/acp-25-2613-2025, 2025
Short summary
Short summary
Black carbon (BC) affects climate and the environment, and its aging process alters its properties. Current models, like WRF-CMAQ, lack full accounting for it. We developed the WRF-CMAQ-BCG model to better represent BC aging by introducing bare and coated BC species and their conversion. The WRF-CMAQ-BCG model introduces the capability to simulate BC mixing states and bare and coated BC wet deposition, and it improves the accuracy of BC mass concentration and aerosol optics.
Zhe Song, Shaocai Yu, Pengfei Li, Ningning Yao, Lang Chen, Yuhai Sun, Boqiong Jiang, and Daniel Rosenfeld
Atmos. Chem. Phys., 25, 2473–2494, https://doi.org/10.5194/acp-25-2473-2025, https://doi.org/10.5194/acp-25-2473-2025, 2025
Short summary
Short summary
Our results with injected sea salt aerosols for five open oceans show that sea salt aerosols with low injection amounts dominate shortwave radiation, mainly through indirect effects. As indirect aerosol effects saturate with increasing injection rates, direct effects exceed indirect effects. This implies that marine cloud brightening is best implemented in areas with extensive cloud cover, while aerosol direct scattering effects remain dominant when clouds are scarce.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
Atmos. Chem. Phys., 25, 2311–2331, https://doi.org/10.5194/acp-25-2311-2025, https://doi.org/10.5194/acp-25-2311-2025, 2025
Short summary
Short summary
This study derives a gridded dust emission dataset for 1841–2000 by employing a combination of observed dust from core records and reanalyzed global dust cycle constraints. We evaluate the ability of global models to replicate the observed historical dust variability by using the emission dataset to force a historical simulation in an Earth system model. We show that prescribing our emissions forces the model to better match observations than other mechanistic models.
Hongyu Liu, Bo Zhang, Richard H. Moore, Luke D. Ziemba, Richard A. Ferrare, Hyundeok Choi, Armin Sorooshian, David Painemal, Hailong Wang, Michael A. Shook, Amy Jo Scarino, Johnathan W. Hair, Ewan C. Crosbie, Marta A. Fenn, Taylor J. Shingler, Chris A. Hostetler, Gao Chen, Mary M. Kleb, Gan Luo, Fangqun Yu, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
Atmos. Chem. Phys., 25, 2087–2121, https://doi.org/10.5194/acp-25-2087-2025, https://doi.org/10.5194/acp-25-2087-2025, 2025
Short summary
Short summary
We use the GEOS-Chem model to simulate aerosol distributions and properties over the western North Atlantic Ocean (WNAO) during the winter and summer deployments in 2020 of the NASA ACTIVATE mission. Model results are evaluated against aircraft, ground-based, and satellite observations. The improved understanding of life cycle, composition, transport pathways, and distribution of aerosols has important implications for characterizing aerosol–cloud–meteorology interactions over WNAO.
Mingrui Ma, Jiachen Cao, Dan Tong, Bo Zheng, and Yu Zhao
Atmos. Chem. Phys., 25, 2147–2166, https://doi.org/10.5194/acp-25-2147-2025, https://doi.org/10.5194/acp-25-2147-2025, 2025
Short summary
Short summary
We combined two global climate change pathways and three national emission control scenarios to analyze the future evolution of reactive nitrogen (Nr) deposition till the 2060s in China with air quality modeling. We show China’s clean air and carbon neutrality policies would overcome the adverse effects of climate change and efficiently reduce Nr deposition. The outflow of Nr fluxes from mainland China to the west Pacific would also be clearly reduced from continuous stringent emission controls.
Zhouyang Zhang, Jiandong Wang, Jiaping Wang, Nicole Riemer, Chao Liu, Yuzhi Jin, Zeyuan Tian, Jing Cai, Yueyue Cheng, Ganzhen Chen, Bin Wang, Shuxiao Wang, and Aijun Ding
Atmos. Chem. Phys., 25, 1869–1881, https://doi.org/10.5194/acp-25-1869-2025, https://doi.org/10.5194/acp-25-1869-2025, 2025
Short summary
Short summary
Black carbon (BC) exerts notable warming effects. We use a particle-resolved model to investigate the long-term behavior of the BC mixing state, revealing its compositions, coating thickness distribution, and optical properties all stabilize with a characteristic time of less than 1 d. This study can effectively simplify the description of the BC mixing state, which facilitates the precise assessment of the optical properties of BC aerosols in global and chemical transport models.
Shuangqin Yang, Yusi Liu, Li Chen, Nan Cao, Jing Wang, and Shuang Gao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3705, https://doi.org/10.5194/egusphere-2024-3705, 2025
Short summary
Short summary
Black carbon, primary brown carbon, and secondary brown carbon are the leading light-absorbing carbonaceous aerosols (LACs) that contribute significantly to climate change. We modified the GEOS-Chem model to simulate the climate change by LACs based on local emission inventory, and explored the impacts of LACs properties and atmospheric variables on the corresponding DRFs in seven regions of China. The study confirms the warming effect of LACs and deepens our knowledge of their climatic effects.
Qianyi Huo, Zhicong Yin, Xiaoqing Ma, and Huijun Wang
Atmos. Chem. Phys., 25, 1711–1724, https://doi.org/10.5194/acp-25-1711-2025, https://doi.org/10.5194/acp-25-1711-2025, 2025
Short summary
Short summary
Dust days during the spring seasons of 2015–2023 in North China were classified into Mongolian cyclone and cold high types depending on the presence of the Mongolian cyclone. The Mongolian cyclone type led to more frequent and severe dust weather, indicated by PM10 concentrations. To comprehensively forecast the two types of dust weather, a common predictor was established based on 500 hPa anomalous circulation systems, offering insights for dust weather forecasting and climate prediction.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes W. Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
Atmos. Chem. Phys., 25, 1545–1567, https://doi.org/10.5194/acp-25-1545-2025, https://doi.org/10.5194/acp-25-1545-2025, 2025
Short summary
Short summary
We compared smoke plume simulations from 11 global models to each other and to satellite smoke amount observations aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss rate assumptions vary enormously among models, causing uncertainties that require systematic in situ measurements to resolve.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Stephen R. Arnold, Leighton A. Regayre, Duseong S. Jo, Wenxiang Shen, Hao Wang, Man Yue, Jingyi Wang, Wenxin Zhang, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-4135, https://doi.org/10.5194/egusphere-2024-4135, 2025
Short summary
Short summary
This study uses a global chemistry-climate model to investigate how new particle formation (NPF) from highly oxygenated organic molecules (HOMs) contributes to cloud condensation nuclei (CCN) in both preindustrial (PI) and present-day (PD) environments, and its impact on aerosol indirect radiative forcing. The findings highlight the crucial role of biogenic emissions in climate change, providing new insights for carbon-neutral scenarios and enhancing understanding of aerosol-cloud interactions.
Yongqing Bai, Tianliang Zhao, Kai Meng, Yue Zhou, Jie Xiong, Xiaoyun Sun, Lijuan Shen, Yanyu Yue, Yan Zhu, Weiyang Hu, and Jingyan Yao
Atmos. Chem. Phys., 25, 1273–1287, https://doi.org/10.5194/acp-25-1273-2025, https://doi.org/10.5194/acp-25-1273-2025, 2025
Short summary
Short summary
We proposed a composite statistical method to identify the quasi-weekly oscillation (QWO) of regional PM2.5 transport over China in winter from 2015 to 2019. The QWO of regional PM2.5 transport is constrained by synoptic-scale disturbances of the East Asian winter monsoon circulation with the periodic activities of the Siberian high, providing a new insight into the understanding of regional pollutant transport with meteorological drivers in atmospheric environment changes.
Léo Clauzel, Sandrine Anquetin, Christophe Lavaysse, Gilles Bergametti, Christel Bouet, Guillaume Siour, Rémy Lapere, Béatrice Marticorena, and Jennie Thomas
Atmos. Chem. Phys., 25, 997–1021, https://doi.org/10.5194/acp-25-997-2025, https://doi.org/10.5194/acp-25-997-2025, 2025
Short summary
Short summary
Solar energy production in West Africa is set to rise and needs accurate solar radiation estimates which are affected by desert dust. This work analyses a March 2021 dust event using a modelling strategy incorporating desert dust. Results show that considering desert dust cuts errors in solar radiation estimates by 75 % and reduces surface solar radiation by 18 %. This highlights the importance of incorporating dust aerosols into solar forecasting for better accuracy.
Zining Yang, Qiuyan Du, Qike Yang, Chun Zhao, Gudongze Li, Zihan Xia, Mingyue Xu, Renmin Yuan, Yubin Li, Kaihui Xia, Jun Gu, and Jiawang Feng
EGUsphere, https://doi.org/10.5194/egusphere-2024-3890, https://doi.org/10.5194/egusphere-2024-3890, 2025
Short summary
Short summary
This study investigates the impact of turbulent mixing on black carbon (BC) concentrations in urban areas using WRF-Chem at 25, 5, and 1 km resolutions. Significant variations in BC and turbulent mixing occur mainly at night. Higher resolutions reduce BC overestimation due to enhanced PBL mixing coefficients and vertical wind fluxes. Small-scale eddies at higher resolutions increase BC lifetime and column concentrations. Land use and terrain variations across multi-resolutions affect PBL mixing.
Ari Laaksonen, Golnaz Roudsari, Ana A. Piedehierro, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-4095, https://doi.org/10.5194/egusphere-2024-4095, 2025
Short summary
Short summary
The mechanisms of ice nucleation at temperatures below 235 K have remained unclear for the past century. We suggest that ice nucleation is caused by the freezing of water adsorbed on aerosol surfaces. To test this hypothesis, we derived theoretical equations to predict the exact atmospheric conditions under which ice nucleation occurs. Our predictions agree well with experiments. The new theory thus provides a basis for an improved description of ice nucleation in the atmosphere.
Ross J. Herbert, Alberto Sanchez-Marroquin, Daniel P. Grosvenor, Kirsty J. Pringle, Stephen R. Arnold, Benjamin J. Murray, and Kenneth S. Carslaw
Atmos. Chem. Phys., 25, 291–325, https://doi.org/10.5194/acp-25-291-2025, https://doi.org/10.5194/acp-25-291-2025, 2025
Short summary
Short summary
Aerosol particles that help form ice in clouds vary in number and type around the world and with time. However, in many weather and climate models cloud ice is not linked to aerosols that are known to nucleate ice. Here we report the first steps towards representing ice-nucleating particles within the UK Earth System Model. We conclude that in addition to ice nucleation by sea spray and mineral components of soil dust, we also need to represent ice nucleation by the organic components of soils.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 25, 327–346, https://doi.org/10.5194/acp-25-327-2025, https://doi.org/10.5194/acp-25-327-2025, 2025
Short summary
Short summary
Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Killian P. Brennan and Lena Wilhelm
EGUsphere, https://doi.org/10.5194/egusphere-2024-3924, https://doi.org/10.5194/egusphere-2024-3924, 2024
Short summary
Short summary
In this study, we discovered that natural dust carried into Europe significantly increases the likelihood of hailstorms. By analyzing dust data, weather records, and hail reports, we found that moderate dust levels lead to more frequent hail, while very high or low dust amounts reduce it. Adding dust information into statistical models improved forecasting skills. We aimed to understand how dust affects hailstorms.
Xinyue Huang, Wenyu Gao, and Hosein Foroutan
EGUsphere, https://doi.org/10.5194/egusphere-2024-3076, https://doi.org/10.5194/egusphere-2024-3076, 2024
Short summary
Short summary
This study investigates the relationship between wind-blown dust aerosols size distribution and wind conditions over topography at a regional scale, utilizing 10 years of dust reanalysis data. Linear regression models suggest that higher wind speeds and steeper land slopes, particularly under uphill winds, are associated with increased fractions of coarser dust particles. Moreover, these positive correlations weaken during summer and afternoon events, likely related to the haboob storms.
Lulu Yuan, Wenchao Han, Jiachen Meng, Yang Wang, Haojie Yu, and Wenze Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3350, https://doi.org/10.5194/egusphere-2024-3350, 2024
Short summary
Short summary
This study utilizes multi-source data to reveal the impact of various urban functional zones in China on the spatial distribution of pollutants. The findings indicate that the residential and commercial zones see notable air quality gains, but the improvement of air quality in the transportation zone is the least considerable. Moreover, the industrial zone has the most seasonal air quality variation. Therefore, air pollution prevention policies should consider differences in functional zones.
Carl Svenhag, Pontus Roldin, Tinja Olenius, Robin Wollesen de Jonge, Sara Blichner, Daniel Yazgi, and Moa Sporre
EGUsphere, https://doi.org/10.5194/egusphere-2024-3626, https://doi.org/10.5194/egusphere-2024-3626, 2024
Short summary
Short summary
This study investigates the model representation of how particles are formed and grow in the atmosphere. Using modeled and observed data from two boreal forest stations in 2018, we identify key factors for NPF to improve particle-climate predictions in the global EC-Earth3 model. Comparisons with the detailed ADCHEM model show that adding ammonia improves particle growth predictions, though EC-Earth3 still highly underestimates the number of particles during warmer months.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 13681–13692, https://doi.org/10.5194/acp-24-13681-2024, https://doi.org/10.5194/acp-24-13681-2024, 2024
Short summary
Short summary
A 2020 regulation has reduced sulfur emissions from shipping by about 80 %, leading to a decrease in atmospheric aerosols that have a cooling effect primarily by affecting cloud properties and amounts. Our climate model simulations predict a global temperature increase of 0.04 K over the next 3 decades as a result, which could contribute to surpassing the Paris Agreement's 1.5 °C target. Reduced aerosols may have also contributed to the recent temperature spikes.
Alcide Zhao, Laura J. Wilcox, and Claire L. Ryder
Atmos. Chem. Phys., 24, 13385–13402, https://doi.org/10.5194/acp-24-13385-2024, https://doi.org/10.5194/acp-24-13385-2024, 2024
Short summary
Short summary
Climate models include desert dust aerosols, which cause atmospheric heating and can change circulation patterns. We assess the effect of dust on the Indian and east Asian summer monsoons through multi-model experiments isolating the effect of dust in current climate models for the first time. Dust atmospheric heating results in a southward shift of western Pacific equatorial rainfall and an enhanced Indian summer monsoon. This shows the importance of accurate dust representation in models.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
Atmos. Chem. Phys., 24, 13361–13370, https://doi.org/10.5194/acp-24-13361-2024, https://doi.org/10.5194/acp-24-13361-2024, 2024
Short summary
Short summary
In 2020, new regulations by the International Maritime Organization regarding sulfur emissions came into force, reducing emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate how much the Earth energy balance changed due to the emission reduction or the so-called effective radiative forcing. The calculated effective radiative forcing is weak, comparable to the effect of the increase in CO2 over the last 2 to 3 years.
Mingxu Liu, Hitoshi Matsui, Douglas S. Hamilton, Sagar D. Rathod, Kara D. Lamb, and Natalie M. Mahowald
Atmos. Chem. Phys., 24, 13115–13127, https://doi.org/10.5194/acp-24-13115-2024, https://doi.org/10.5194/acp-24-13115-2024, 2024
Short summary
Short summary
Atmospheric aerosol deposition provides bioavailable iron to promote marine primary production, yet the estimates of its fluxes remain highly uncertain. This study, by performing global aerosol simulations, demonstrates that iron-containing particle size upon emission is a critical factor in regulating soluble iron input to open oceans. Further observational constraints on this are needed to reduce modeling uncertainties.
Thomas Drugé, Pierre Nabat, Martine Michou, and Marc Mallet
EGUsphere, https://doi.org/10.5194/egusphere-2024-3659, https://doi.org/10.5194/egusphere-2024-3659, 2024
Short summary
Short summary
Aerosol scattering in long-wave radiation is often neglected in climate models. In this study, we analyze its impact through a physical modeling of this process in the CNRM ARPEGE-Climat model. It mainly leads to surface LW radiation increases across Sahara, Sahel and Arabian Peninsula, resulting in daily minimum near-surface temperature rises. Other changes in atmospheric fields are also simulated.
Jingmin Li, Mattia Righi, Johannes Hendricks, Christof G. Beer, Ulrike Burkhardt, and Anja Schmidt
Atmos. Chem. Phys., 24, 12727–12747, https://doi.org/10.5194/acp-24-12727-2024, https://doi.org/10.5194/acp-24-12727-2024, 2024
Short summary
Short summary
Aiming to understand underlying patterns and trends in aerosols, we characterize the spatial patterns and long-term evolution of lower tropospheric aerosols by clustering multiple aerosol properties from preindustrial times to the year 2050 under three Shared
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Yueming Cheng, Tie Dai, Junji Cao, Daisuke Goto, Jianbing Jin, Teruyuki Nakajima, and Guangyu Shi
Atmos. Chem. Phys., 24, 12643–12659, https://doi.org/10.5194/acp-24-12643-2024, https://doi.org/10.5194/acp-24-12643-2024, 2024
Short summary
Short summary
In March 2021, east Asia experienced an outbreak of severe dust storms after an absence of 1.5 decades. Here, we innovatively used the time-lagged ground-based aerosol size information with the fixed-lag ensemble Kalman smoother to optimize dust emission and reproduce the dust storm. This work is valuable for not only the quantification of health damage, aviation risks, and profound impacts on the Earth's system but also revealing the climatic driving force and the process of desertification.
Marc Mallet, Aurore Voldoire, Fabien Solmon, Pierre Nabat, Thomas Drugé, and Romain Roehrig
Atmos. Chem. Phys., 24, 12509–12535, https://doi.org/10.5194/acp-24-12509-2024, https://doi.org/10.5194/acp-24-12509-2024, 2024
Short summary
Short summary
This study investigates the interactions between smoke aerosols and climate in tropical Africa using a coupled ocean–atmosphere–aerosol climate model. The work shows that smoke plumes have a significant impact by increasing the low-cloud fraction, decreasing the ocean and continental surface temperature and reducing the precipitation of coastal western Africa. It also highlights the role of the ocean temperature response and its feedbacks for the September–November season.
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
Short summary
Short summary
The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Catherine Anne Toolan, Joe Adabouk Amooli, Laura J. Wilcox, Bjørn H. Samset, Andrew G. Turner, and Daniel M. Westervelt
EGUsphere, https://doi.org/10.5194/egusphere-2024-3057, https://doi.org/10.5194/egusphere-2024-3057, 2024
Short summary
Short summary
Our research explores how well air pollution and rainfall patterns in Africa are represented in current climate models, by comparing model data to observations from 1981 to 2023. While most models capture seasonal air quality changes well, they struggle to replicate the distribution of non-dust pollutants and certain rainfall patterns, especially over east Africa. Improving these models is crucial for better climate predictions and preparing for future risks.
Zijun Li, Angela Buchholz, and Noora Hyttinen
Atmos. Chem. Phys., 24, 11717–11725, https://doi.org/10.5194/acp-24-11717-2024, https://doi.org/10.5194/acp-24-11717-2024, 2024
Short summary
Short summary
Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Cited articles
Allen, M. P. and Tildesley, D. J.: Computer Simulation of Liquids, Oxford
University Press, New York, 1991.
Altaf, M. B. and Freedman, M. A.: Effect of Drying Rate on Aerosol Particle
Morphology, J. Phys. Chem. Lett., 8, 3613–3618, 2017.
Bahadur, R., Russell, L. M. and Prather, K.: Composition and morphology of
individual combustion, biomass burning, and secondary organic particle types
obtained using urban and coastal ATOFMS and STXM-NEXAFS measurements, Aerosol
Sci. Technol., 44, 551–562, 2010.
Berendsen, H. J. C., Grigera, J. R. and Straatsma, T. P.: The missing term in
effective pair potentials, J. Phys. Chem., 91, 6269–6271, 1987.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A.,
Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the
relative humidities of liquid-liquid phase separation, efflorescence, and
deliquescence of mixed particles of ammonium sulfate, organic material, and
water using the organic-to-sulfate mass ratio of the particle and the
oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem.
Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Brooks, B. R., Bruccoleri, R. E., Olafson, B. D., States, D. J., Swaminathan,
S., and Karplus, M.: CHARMM: A program for macromolecular energy,
minimization, and dynamics calculations, J. Comput. Chem., 4, 187–217, 1983.
Buseck, P. R. and Adachi, K.: Nanoparticles in the atmosphere, Elements, 4,
389–394, 2008.
Chakraborty, P. and Zachariah, M. R.: On the structure of organic-coated
water droplets: From “net water attractors” to “oily” drops, J. Geophys.
Res., 116, 1–8, 2011.
Cheng, Y., Brook, J. R., Li, S.-M., and Leithead, A.: Seasonal variation in
the biogenic secondary organic aerosol tracer cis-pinonic acid: Enhancement
due to emissions from regional and local biomass burning, Atmos. Environ.,
45, 7105–7112, 2011.
Clegg, S. L., Pitzer, K. S., and Brimblecombe, P.: Thermodynamics of
multicomponent, miscible, ionic solutions. Mixtures including unsymmetrical
electrolytes, J. Phys. Chem., 96, 9470–9479, 1992.
Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: Thermodynamic model of the
system H+-NH
Dassault Systèmes BIOVIA Discovery Visualizer Studios: Dassault
Systèmes BIOVIA, San Diego, available at:
http://accelrys.com/products/collaborative-science/biovia-discovery-studio/visualization.html,
last access: 18 February 2016.
Davies, J. F., Miles, R. E. H., Haddrell, A. E., and Reid, J. P.: Influence
of organic films on the evaporation and condensation of water in aerosol, P.
Natl. Acad. Sci. USA, 110, 8807–8812, 2013.
Dennis-Smither, B. J., Hanford, K. L., Kwamena, N. O. A., Miles, R. E. H.,
and Reid, J. P.: Phase, morphology, and hygroscopicity of mixed oleic
acid/sodium chloride/water aerosol particles before and after ozonolysis, J.
Phys. Chem. A, 116, 6159–6168, 2012.
Dette, H. P., Qi, M., Schröder, D. C., Godt, A., and Koop, T.:
Glass-forming properties of 3-methylbutane-1,2,3-tricarboxylic acid and its
mixtures with water and pinonic acid, J. Phys. Chem. A, 118, 7024–7033,
2014.
Eastwood, J. W., Hockney, R. W., and Lawrence, D. N.: P3M3DP – The
three-dimensional periodic particle-particle/particle-mesh program, Comput.
Phys. Commun., 19, 215–261, 1980.
Folkers, M., Mentel, T. F., and Wahner, A.: Influence of an organic coating
on the reactivity of aqueous aerosols probed by the heterogeneous hydrolysis
of N2O5, Geophys. Res. Lett., 30, 2–5, 2003.
Fuzzi, S., Baltensperger, U., Carslaw, K., Decesari, S., Denier van der Gon,
H., Facchini, M. C., Fowler, D., Koren, I., Langford, B., Lohmann, U.,
Nemitz, E., Pandis, S., Riipinen, I., Rudich, Y., Schaap, M., Slowik, J. G.,
Spracklen, D. V., Vignati, E., Wild, M., Williams, M., and Gilardoni, S.:
Particulate matter, air quality and climate: lessons learned and future
needs, Atmos. Chem. Phys., 15, 8217–8299,
https://doi.org/10.5194/acp-15-8217-2015, 2015.
Glasius, M. and Goldstein, A. H.: Recent discoveries and future challenges in
atmospheric organic chemistry, Environ. Sci. Technol., 50, 2754–2764, 2016.
Goldstein, H., Poole, C., and Safko, J.: Classical Mechanics, 3rd edn.,
Pearson, London, 2007.
Gopalakrishnan, S., Jungwirth, P., Tobias, D. J., and Allen, H. C.:
Air-liquid interfaces of aqueous solutions containing ammonium and sulfate:
Spectroscopic and molecular dynamics studies, J. Phys. Chem. B, 109,
8861–8872, 2005.
Hede, T., Li, X., Leck, C., Tu, Y., and Ågren, H.: Model HULIS compounds
in nanoaerosol clusters – investigations of surface tension and aggregate
formation using molecular dynamics simulations, Atmos. Chem. Phys., 11,
6549–6557, https://doi.org/10.5194/acp-11-6549-2011, 2011.
Hoover, W. G.: Canonical dynamics: Equilibrium phase-space distributions,
Phys. Rev. A, 31, 1695–1697, 1985.
Hoover, W. G.: Constant-pressure equations of motion, Phys. Rev. A, 34,
2499–2500, 1986.
Hudait, A. and Molinero, V.: Ice crystallization in ultrafine water-salt
aerosols: Nucleation, ice-solution equilibrium, and internal structure, J.
Am. Chem. Soc., 136, 8081–8093, 2014.
Hyvärinen, A. P., Lihavainen, H., Gaman, A., Vairila, L., Ojala, H.,
Kulmala, M., and Viisanen, Y.: Surface tensions and densities of oxalic,
malonic, succinic, maleic, malic, and cis-pinonic acids, J. Chem. Eng. Data,
51, 255–260, 2006.
IPCC: Climate Change 2013: The Physical Science Basis, Contribution of
Working Group I to the Fifth Assessment Report of the Intergovernmental Panel
on Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K.,
Tignor, M., Allen, S. K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and
Midgley, P. M., Cambridge University Press, Cambridge, UK, New York, 2013.
Jorgensen, W. L. and Tirado-Rives, J.: The OPLS Potential Functions for
Proteins. Energy Minimizations for Crystals of Cyclic Peptides and Crambin,
J. Am. Chem. Soc., 110, 1657–1666, 1988.
Jungwirth, P., Rosenfeld, D., and Buch, V.: A possible new molecular
mechanism of thundercloud electrification, Atmos. Res., 76, 190–205, 2005.
Karadima, K. S., Mavrantzas, V. G., and Pandis, S. N.: Molecular dynamics
simulation of the local concentration and structure in multicomponent aerosol
nanoparticles under atmospheric conditions, Phys. Chem. Chem. Phys., 19,
16681–16692, 2017.
Koo, B., Ansari, A. S., and Pandis, S. N.: Integrated approaches to modeling
the organic and inorganic atmospheric aerosol components, Atmos. Environ.,
37, 4757–4768, 2003.
Kotianová, P., Puxbaum, H., Bauer, H., Caseiro, A., Marr, I. L., and
Čík, G.: Temporal patterns of n-alkanes at traffic exposed and
suburban sites in Vienna, Atmos. Environ., 42, 2993–3005, 2008.
Kwamena, N.-O. A., Buajarern, J., and Reid, J. P.: Equilibrium morphology of
mixed organic/inorganic/aqueous aerosol droplets: Investigating the effect of
relative humidity and surfactants, J. Phys. Chem. A, 114, 5787–5795, 2010.
Li, X., Hede, T., Tu, Y., Leck, C., and Ågren, H.: Surface-active
cis-pinonic acid in atmospheric droplets: A molecular dynamics study, J.
Phys. Chem. Lett., 1, 769–773, 2010.
Liyana-Arachchi, T., Zhang, Z., Ehrenhauser, F. S., Avij, P., Valsaraj, K.
T., and Hung, F. R.: Bubble bursting as an aerosol generation mechanism
during an oil spill in the deep-sea environment: molecular dynamics
simulations of oil alkanes and dispersants in atmospheric air/salt water
interfaces, Environ. Sci. Process. Impacts, 16, 53–64, 2014.
Ma, X., Chakraborty, P., Henz, B. J., and Zachariah, M. R.: Molecular dynamic
simulation of dicarboxylic acid coated aqueous aerosol: structure and
processing of water vapor., Phys. Chem. Chem. Phys., 13, 9374–9384, 2011.
Marcolli, C. and Krieger, U. K.: Phase changes during hygroscopic cycles of
mixed organic/inorganic model systems of tropospheric aerosols, J. Phys.
Chem. A, 110, 1881–1893, 2006.
Mavrantza, I.-E., Prentzas, D., Mavrantzas, V. G., and Galiotis, C.: Detailed
atomistic molecular-dynamics simulation of the orthorhombic phase of
crystalline polyethylene and alkane crystals, J. Chem. Phys., 115,
3937–3950, 2001.
Miyamoto, S. and Kollman, P. A.: SETTLE: An analytical version of the SHAKE
and RATTLE algorithm for rigid water models, J. Comput. Chem., 13, 952–962,
1992.
Müller, L., Reinnig, M.-C., Naumann, K. H., Saathoff, H., Mentel, T. F.,
Donahue, N. M., and Hoffmann, T.: Formation of
3-methyl-1,2,3-butanetricarboxylic acid via gas phase oxidation of pinonic
acid – a mass spectrometric study of SOA aging, Atmos. Chem. Phys., 12,
1483–1496, https://doi.org/10.5194/acp-12-1483-2012, 2012.
Nosé, S.: A molecular dynamics method for simulations in the canonical
ensemble, Mol. Phys., 52, 255–268, 1984.
O'Brien, R. E., Wang, B., Kelly, S. T., Lundt, N., You, Y., Bertram, A. K.,
Leone, S. R., Laskin, A., and Gilles, M. K.: Liquid–liquid phase separation
in aerosol particles: Imaging at the nanometer scale, Environ. Sci. Technol.,
49, 4995–5002, 2015.
Ovadnevaite, J., Zuend, A., Laaksonen, A., Sanchez, K. J., Roberts, G.,
Ceburnis, D., Decesari, S., Rinaldi, M., Hodas, N., Facchini, M. C.,
Seinfeld, J. H., and O'Dowd, C.: Surface tension prevails over solute effect
in organic-influenced cloud droplet activation, Nature, 546, 637–641, 2017.
Plimpton, S.: Fast parallel algorithms for short-range molecular dynamics, J.
Comput. Phys., 117, 1–19, 1995.
Pun, B. K., Wu, S. Y., Seigneur, C., Seinfeld, J. H., Griffin, R. J., and
Pandis, S. N.: Uncertainties in modeling secondary organic aerosols:
Three-dimensional modeling studies in Nashville/Western Tennessee, Environ.
Sci. Technol., 37, 3647–3661, 2003.
Qiu, Y. and Molinero, V.: Morphology of liquid-liquid phase separated
serosols, J. Am. Chem. Soc., 137, 10642–10651, 2015.
Qiu, Y. and Molinero, V.: Strength of alkane–fluid attraction determines the
interfacial orientation of liquid alkanes and their crystallization through
heterogeneous or homogeneous mechanisms, Crystals, 7, 86, 2017.
Reid, J. P., Dennis-Smither, B. J., Kwamena, N.-O. A., Miles, R. E. H.,
Hanford, K. L., and Homer, C. J.: The morphology of aerosol particles
consisting of hydrophobic and hydrophilic phases: hydrocarbons, alcohols and
fatty acids as the hydrophobic component, Phys. Chem. Chem. Phys., 13,
15559–15572, 2011.
Renbaum-Wolff, L., Song, M., Marcolli, C., Zhang, Y., Liu, P. F., Grayson, J.
W., Geiger, F. M., Martin, S. T., and Bertram, A. K.: Observations and
implications of liquid–liquid phase separation at high relative humidities
in secondary organic material produced by α-pinene ozonolysis without
inorganic salts, Atmos. Chem. Phys., 16, 7969–7979,
https://doi.org/10.5194/acp-16-7969-2016, 2016.
Robinson, E. S., Saleh, R., and Donahue, N. M.: Probing the evaporation
dynamics of mixed SOA/squalane particles using size-resolved composition and
single-particle measurements, Environ. Sci. Technol., 49, 9724–9732, 2015.
Ruehl, C. R. and Wilson, K. R.: Surface organic monolayers control the
hygroscopic growth of submicrometer particles at high relative humidity, J.
Phys. Chem. A, 118, 3952–3966, 2014.
Sareen, N., Schwier, A. N., Lathem, T. L., Nenes, A., and McNeill, V. F.:
Surfactants from the gas phase may promote cloud droplet formation, P. Natl.
Acad. Sci. USA, 110, 2723–2728, 2013.
Scienomics SARL: MAPS, Paris, available at:
http://scienomics.com/products/molecular-modeling-platform, last
access: 16 July 2015.
Seidl, W.: Model for a surface film of fatty acids on rain water and aerosol
particles, Atmos. Environ., 34, 4917–4932, 2000.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: From
air pollution to climate change, 2nd edn., Johh Wiley & Sons, New Jersey,
2006.
Shiraiwa, M., Ammann, M., Koop, T., and Poschl, U.: Gas uptake and chemical
aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108,
11003–11008, 2011.
Shiraiwa, M., Zuend, A., Bertram, A. K. and Seinfeld, J. H.: Gas–particle
partitioning of atmospheric aerosols: interplay of physical state, non–ideal
mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, 2013.
Smolenskii, E. A., Ryzhov, A. N., Member, C. and Lapidus, R. A. S. A. L.:
Simulation of melting temperatures of normal alkanes, Dokl. Chem., 387,
297–301, 2002.
Song, C., Zaveri, R. A., Alexander, M. L., Thornton, J. A., Madronich, S.,
Ortega, J. V., Zelenyuk, A., Yu, X. Y., Laskin, A., and Maughan, D. A.:
Effect of hydrophobic primary organic aerosols on secondary organic aerosol
formation from ozonolysis of α-pinene, Geophys. Res. Lett., 34, 1–5,
2007.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid-liquid phase separation in aerosol particles: Dependence on O : C,
organic functionalities, and compositional complexity, Geophys. Res. Lett.,
39, 1–5, 2012.
Song, M., Marcolli, C., Krieger, U. K., Lienhard, D. M., and Peter, T.:
Morphologies of mixed organic/inorganic/aqueous aerosol droplets, Faraday
Discuss., 165, 289–316, 2013.
Szmigielski, R., Surratt, J. D., Gómez-González, Y., van der Veken,
P., Kourtchev, I., Vermeylen, R., Blockhuys, F., Jaoui, M., Kleindienst, T.
E., Lewandowski, M., Offenberg, J. H., Edney, E. O., Seinfeld, J. H.,
Maenhaut, W., and Claeys, M.: 3-methyl-1,2,3-butanetricarboxylic acid: An
atmospheric tracer for terpene secondary organic aerosol, Geophys. Res.
Lett., 34, 2–7, 2007.
Takahama, S., Liu, S., and Russell, L. M.: Coatings and clusters of
carboxylic acids in carbon-containing atmospheric particles from
spectromicroscopy and their implications for cloud-nucleating and optical
properties, J. Geophys. Res.-Atmos., 115, 1–21, 2010.
Theodorou, D. N. and Suter, U. W.: Shape of unperturbed linear polymers:
polypropylene, Macromolecules, 18, 1206–1214, 1985.
Tsolou, G. and Mavrantzas, V. G.: Atomistic simulation of the sorption of
small gas molecules in polyisobutylene, Macromolecules, 41, 6228–6238, 2008.
Veghte, D. P., Altaf, M. B., and Freedman, M. A.: Size dependence of the
structure of organic aerosol, J. Am. Chem. Soc., 135, 16046–16049, 2013.
Veghte, D. P., Bittner, D. R., and Freedman, M. A.: Cryo-transmission
electron microscopy imaging of the morphology of submicrometer aerosol
containing organic acids and ammonium sulfate, Anal. Chem., 86, 2436–2442,
2014.
Verlet, L.: Computer “experiments” on classical fluids. I. Thermodynamical
properties of Lennard-Jones molecules, Phys. Rev., 159, 98–103, 1967.
Verlet, L.: Computer “experiments” on classical fluids. II. Equilibrium
correlation functions, Phys. Rev., 165, 201–214, 1968.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P.,
Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U.,
Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of
biogenic secondary organic aerosol particles, Nature, 467, 824–7, 2010.
Wang, B.-B., Wang, X.-D., Chen, M., and Xu, J.-L.: Molecular dynamics
simulations on evaporation of droplets with dissolved salts, Entropy, 15,
1232–1246, 2013.
Wang, G., Kawamura, K., Xie, M., Hu, S., Gao, S., Cao, J., An, Z., and Wang,
Z.: Size-distributions of n-alkanes, PAHs and hopanes and their sources in
the urban, mountain and marine atmospheres over East Asia, Atmos. Chem.
Phys., 9, 8869–8882, https://doi.org/10.5194/acp-9-8869-2009, 2009.
Wang, Y. H., Liu, Z. R., Zhang, J. K., Hu, B., Ji, D. S., Yu, Y. C., and
Wang, Y. S.: Aerosol physicochemical properties and implications for
visibility during an intense haze episode during winter in Beijing, Atmos.
Chem. Phys., 15, 3205–3215, https://doi.org/10.5194/acp-15-3205-2015, 2015.
Werner, J., Dalirian, M., Walz, M. M., Ekholm, V., Wideqvist, U., Lowe, S.
J., Öhrwall, G., Persson, I., Riipinen, I., and Björneholm, O.:
Surface partitioning in organic-inorganic mixtures contributes to the
size-dependence of the phase-state of atmospheric nanoparticles, Environ.
Sci. Technol., 50, 7434–7442, 2016.
Wexler, A. S. and Clegg, S. L.: Atmospheric aerosol models for systems
including the ions H+, NH
World Health Organization: Ambient Air Pollution: A global assessment of
exposure and burden of disease, World Health Organ., 1–131, 2016.
You, Y. and Bertram, A. K.: Effects of molecular weight and temperature on
liquid–liquid phase separation in particles containing organic species and
inorganic salts, Atmos. Chem. Phys., 15, 1351–1365,
https://doi.org/10.5194/acp-15-1351-2015, 2015.
You, Y., Renbaum-Wolff, L., Carreras-Sospedra, M., Hanna, S. J., Hiranuma,
N., Kamal, S., Smith, M. L., Zhang, X., Weber, R. J., Shilling, J. E.,
Dabdub, D., Martin, S. T., and Bertram, A. K.: Images reveal that atmospheric
particles can undergo liquid-liquid phase separations, P. Natl. Acad. Sci.
USA, 109, 13188–13193, 2012.
You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.:
Liquid-liquid phase separation in atmospherically relevant particles
consisting of organic species and inorganic salts, Int. Rev. Phys. Chem., 33,
43–77, 2014.
Zhang, Q. and Thompson, J. E.: Effect of particle mixing morphology on
aerosol scattering and absorption: A discrete dipole modeling study, Geo.
Res. J., 3–4, 9–18, 2014.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., et al.: Ubiquity and dominance
of oxygenated species in organic aerosols in anthropogenically-influenced
Northern Hemisphere midlatitudes, Geophys. Res. Lett., 34, 1–6, 2007.
Zhang, X., McVay, R. C., Huang, D. D., Dalleska, N. F., Aumont, B., Flagan,
R. C., and Seinfeld, J. H.: Formation and evolution of molecular products in
α-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 112,
14168–14173, 2015.
Zhou, S., Lee, A. K. Y., Mcwhinney, R. D., and Abbatt, J. P. D.: Burial
effects of organic coatings on the heterogeneous reactivity of particle-borne
benzo[a]pyrene (BaP) toward ozone, Phys. Chem. A, 116, 7050–7056, 2012.
Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of
secondary organic aerosol: the importance of liquid-liquid phase separation,
Atmos. Chem. Phys., 12, 3857–3882, https://doi.org/10.5194/acp-12-3857-2012,
2012.
Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of
liquid-liquid equilibria and phase stabilities: implications for RH-dependent
gas/particle partitioning of organic-inorganic aerosols, Atmos. Chem. Phys.,
10, 7795–7820, https://doi.org/10.5194/acp-10-7795-2010, 2010.
Short summary
We explore the morphologies of multicomponent nanoparticles through atomistic molecular dynamics simulations under atmospherically relevant conditions. Phase separation is predicted for almost all simulated nanoparticles either between organics and inorganics or between hydrophobic and hydrophilic constituents. Three main particle types were identified: organic islands at the surface, inorganic core-organic shell morphologies and complex structures with hydrophobic and hydrophilic domains.
We explore the morphologies of multicomponent nanoparticles through atomistic molecular dynamics...
Altmetrics
Final-revised paper
Preprint