Articles | Volume 19, issue 9
https://doi.org/10.5194/acp-19-5959-2019
© 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-19-5959-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities
Department of Chemistry, University of California, Irvine, California, USA
Department of Chemistry, University of California, Irvine, California, USA
Related authors
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2023-1444, https://doi.org/10.5194/egusphere-2023-1444, 2023
Short summary
Short summary
Secondary organic aerosols (SOA) can exist in liquid, semi-solid or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in the northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
Short summary
Short summary
This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
Short summary
Short summary
We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
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.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
Short summary
Short summary
Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
Short summary
Short summary
Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
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.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
Short summary
Short summary
We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
Short summary
Short summary
The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
Y. Tang, J. An, F. Wang, Y. Li, Y. Qu, Y. Chen, and J. Lin
Atmos. Chem. Phys., 15, 9381–9398, https://doi.org/10.5194/acp-15-9381-2015, https://doi.org/10.5194/acp-15-9381-2015, 2015
Short summary
Short summary
High daytime HONO mixing ratios in experiments suggest that an unknown daytime HONO source (P unknown) could exist. P unknown≈19.60×NO2×J(NO2) was obtained using observed data from 13 field experiments across the globe, then coupled into the WRF-Chem model. Simulations indicated that elevated P unknown was found in the coastal regions of China; the additional HONO sources, especially the P unknown produced significant increases of radicals in the major cities, and accelerated the radical cycles.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2024-51, https://doi.org/10.5194/egusphere-2024-51, 2024
Short summary
Short summary
SOA derived from n-alkanes is a major component of anthropogenic particulate matter. We provide a comprehensive analysis of n-alkane SOA by explicit chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopt low viscous semisolid or liquid states. Our results indicate little kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Daniel Alexander Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2023-2314, https://doi.org/10.5194/egusphere-2023-2314, 2023
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen to carbon ratio of the desorbing chemical species. Its application to gas-particle interactions is discussed.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2023-1444, https://doi.org/10.5194/egusphere-2023-1444, 2023
Short summary
Short summary
Secondary organic aerosols (SOA) can exist in liquid, semi-solid or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in the northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
Short summary
Short summary
Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
Short summary
Short summary
This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
Short summary
Short summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
Short summary
Short summary
We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
Short summary
Short summary
This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
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.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
Short summary
Short summary
Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
Short summary
Short summary
Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
Short summary
Short summary
Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
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.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
Short summary
Short summary
We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
Short summary
Short summary
We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
Short summary
Short summary
The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
Short summary
Short summary
We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
Short summary
Short summary
In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
Short summary
Short summary
Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
Short summary
Short summary
Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
Short summary
Short summary
We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
Short summary
Short summary
Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
Short summary
Short summary
Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
Short summary
Short summary
We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
Y. Tang, J. An, F. Wang, Y. Li, Y. Qu, Y. Chen, and J. Lin
Atmos. Chem. Phys., 15, 9381–9398, https://doi.org/10.5194/acp-15-9381-2015, https://doi.org/10.5194/acp-15-9381-2015, 2015
Short summary
Short summary
High daytime HONO mixing ratios in experiments suggest that an unknown daytime HONO source (P unknown) could exist. P unknown≈19.60×NO2×J(NO2) was obtained using observed data from 13 field experiments across the globe, then coupled into the WRF-Chem model. Simulations indicated that elevated P unknown was found in the coastal regions of China; the additional HONO sources, especially the P unknown produced significant increases of radicals in the major cities, and accelerated the radical cycles.
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
Short summary
Short summary
Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
Short summary
Short summary
Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Improved estimates of smoke exposure during Australia fire seasons: importance of quantifying plume injection heights
New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau
Investigation of observed dust trends over the Middle East region in NASA Goddard Earth Observing System (GEOS) model simulations
A new process-based and scale-aware desert dust emission scheme for global climate models – Part II: Evaluation in the Community Earth System Model version 2 (CESM2)
How well do Earth system models reproduce the observed aerosol response to rapid emission reductions? A COVID-19 case study
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
Impact of acidity and surface-modulated acid dissociation on cloud response to organic aerosol
The contribution of residential wood combustion to the PM2.5 concentrations in the Helsinki metropolitan area
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
Expanding the simulation of East Asian super dust storms: physical transport mechanisms impacting the western Pacific
Improving 3-day deterministic air pollution forecasts using machine learning algorithms
Opinion: The importance of historical and paleoclimate aerosol radiative effects
Assessing the assimilation of Himawari-8 observations on aerosol forecasts and radiative effects during pollution transport from South Asia to the Tibetan Plateau
Aerosol–meteorology feedback diminishes the transboundary transport of black carbon into the Tibetan Plateau
Associations of interannual variation in summer tropospheric ozone with the Western Pacific Subtropical High in China from 1999 to 2017
Climate intervention using marine cloud brightening (MCB) compared with stratospheric aerosol injection (SAI) in the UKESM1 climate model
Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: Strong surfactants
Increased importance of aerosol–cloud interactions for surface PM2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions
The role of temporal scales in extracting dominant meteorological drivers of major airborne pollutants
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Air pollution trapping in the Dresden Basin from gray-zone scale urban modeling
The effect of atmospherically relevant aminium salts on water uptake
Droplet collection efficiencies estimated from satellite retrievals constrain effective radiative forcing of aerosol-cloud interactions
The impact of aerosols on stratiform clouds over southern West Africa: a large-eddy-simulation study
Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate-aerosol model
Molecular-level study on the role of methanesulfonic acid in iodine oxoacids nucleation
Global aerosol typing classification using a new hybrid algorithm utilizing Aerosol Robotic Network data
Temporal and spatial variations in dust activity in Australia based on remote sensing and reanalysis data sets
The underappreciated role of transboundary pollution in future air quality and health improvements in China
The export of African mineral dust across the Atlantic and its impact over the Amazon Basin
Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC
Assimilation of POLDER observations to estimate aerosol emissions
Effect of radiation interaction and aerosol processes on ventilation and aerosol concentrations in a real urban neighbourhood in Helsinki
Atlantic Multidecadal Oscillation modulates the relationship between El Niño–Southern Oscillation and fire weather in Australia
Sharp increase of Saharan dust intrusions over the Western Mediterranean and Euro-Atlantic region in winters 2020–2022 and associated atmospheric circulation
Phase state and viscosity of secondary organic aerosols over China simulated by WRF-Chem
Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020
Fire-precipitation interactions amplify the quasi-biennial variability of fires over southern Mexico and Central America
Identifying climate model structural inconsistencies allows for tight constraint of aerosol radiative forcing
Sensitivity of global direct aerosol radiative forcing to uncertainties in aerosol optical properties
Impacts of reducing scattering and absorbing aerosols on the temporal extent and intensity of South Asian summer monsoon and East Asian summer monsoon
Superimposed effects of typical local circulations driven by mountainous topography and aerosol–radiation interaction on heavy haze in the Beijing–Tianjin–Hebei central and southern plains in winter
Multi-model ensemble projection of the global dust cycle by the end of 21st century using the Coupled Model Intercomparison Project version 6 data
A thermodynamic framework for bulk–surface partitioning in finite-volume mixed organic–inorganic aerosol particles and cloud droplets
Improved Simulations of Biomass Burning Aerosol Optical Properties and Lifetimes in the NASA GEOS Model during the ORACLES-I Campaign
Change from aerosol-driven to cloud-feedback-driven trend in short-wave radiative flux over the North Atlantic
A new process-based and scale-aware desert dust emission scheme for global climate models – Part I: Description and evaluation against inverse modeling emissions
Transported aerosols regulate the pre-monsoon rainfall over north-east India: a WRF-Chem modelling study
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
Short summary
Short summary
During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
Short summary
Short summary
By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Adriana Rocha-Lima, Peter R. Colarco, Anton S. Darmenov, Edward P. Nowottnick, Arlindo M. da Silva, and Luke D. Oman
Atmos. Chem. Phys., 24, 2443–2464, https://doi.org/10.5194/acp-24-2443-2024, https://doi.org/10.5194/acp-24-2443-2024, 2024
Short summary
Short summary
Observations show an increasing aerosol optical depth trend in the Middle East between 2003–2012. We evaluate the NASA Goddard Earth Observing System (GEOS) model's ability to capture these trends and examine the meteorological and surface parameters driving dust emissions. Our results highlight the importance of data assimilation for long-term trends of atmospheric aerosols and support the hypothesis that vegetation cover loss may have contributed to increasing dust emissions in the period.
Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
Short summary
Short summary
This study uses a premier Earth system model to evaluate a new desert dust emission scheme proposed in our companion paper. We show that our scheme accounts for more dust emission physics, hence matching better against observations than other existing dust emission schemes do. Our scheme's dust emissions also couple tightly with meteorology, hence likely improving the modeled dust sensitivity to climate change. We believe this work is vital for improving dust representation in climate models.
Ruth A. R. Digby, Nathan P. Gillett, Adam H. Monahan, Knut von Salzen, Antonis Gkikas, Qianqian Song, and Zhibo Zhang
Atmos. Chem. Phys., 24, 2077–2097, https://doi.org/10.5194/acp-24-2077-2024, https://doi.org/10.5194/acp-24-2077-2024, 2024
Short summary
Short summary
The COVID-19 lockdowns reduced aerosol emissions. We ask whether these reductions affected regional aerosol optical depth (AOD) and compare the observed changes to predictions from Earth system models. Only India has an observed AOD reduction outside of typical variability. Models overestimate the response in some regions, but when key biases have been addressed, the agreement is improved. Our results suggest that current models can realistically predict the effects of future emission changes.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
Short summary
Short summary
This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Gargi Sengupta, Minjie Zheng, and Nønne L. Prisle
Atmos. Chem. Phys., 24, 1467–1487, https://doi.org/10.5194/acp-24-1467-2024, https://doi.org/10.5194/acp-24-1467-2024, 2024
Short summary
Short summary
The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in an atmospheric model. Organic acid dissociation was considered using both bulk and surface-related properties. We found that organic acid dissociation leads to increased hydrogen ion concentrations and sulfate aerosol mass in aqueous aerosols, increasing cloud formation. This could be important in large-scale climate models as many organic aerosol components are both acidic and surface-active.
Leena Kangas, Jaakko Kukkonen, Mari Kauhaniemi, Kari Riikonen, Mikhail Sofiev, Anu Kousa, Jarkko V. Niemi, and Ari Karppinen
Atmos. Chem. Phys., 24, 1489–1507, https://doi.org/10.5194/acp-24-1489-2024, https://doi.org/10.5194/acp-24-1489-2024, 2024
Short summary
Short summary
Residential wood combustion is a major source of fine particulate matter. This study has evaluated the contribution of residential wood combustion to fine particle concentrations and its year-to-year and seasonal variation in te Helsinki metropolitan area. The average concentrations attributed to wood combustion in winter were up to 10- or 15-fold compared to summer. Wood combustion caused 12 % to 14 % of annual fine particle concentrations. In winter, the contribution ranged from 16 % to 21 %.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
Atmos. Chem. Phys., 24, 1315–1328, https://doi.org/10.5194/acp-24-1315-2024, https://doi.org/10.5194/acp-24-1315-2024, 2024
Short summary
Short summary
Particle growth at the Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low-volatility organic compounds (LVOCs). Also, sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building knowledge of early growth of atmospheric particles.
Steven Soon-Kai Kong, Saginela Ravindra Babu, Sheng-Hsiang Wang, Stephen M. Griffith, Jackson Hian-Wui Chang, Ming-Tung Chuang, Guey-Rong Sheu, and Neng-Huei Lin
Atmos. Chem. Phys., 24, 1041–1058, https://doi.org/10.5194/acp-24-1041-2024, https://doi.org/10.5194/acp-24-1041-2024, 2024
Short summary
Short summary
In this study, we combined ground observations from 7-SEAS Dongsha Experiment, MERRA-2 reanalysis, and MODIS satellite images for evaluation and improvement of the CMAQ dust model for cases of East Asian Dust reaching the Taiwan region, including Dongsha in the western Pacific. We proposed a better CMAQ dust treatment over East Asia and for the first time revealed the impact of typhoons on dust transport.
Zhiguo Zhang, Christer Johansson, Magnuz Engardt, Massimo Stafoggia, and Xiaoliang Ma
Atmos. Chem. Phys., 24, 807–851, https://doi.org/10.5194/acp-24-807-2024, https://doi.org/10.5194/acp-24-807-2024, 2024
Short summary
Short summary
Up-to-date information on present and near-future air quality help people avoid exposure to high levels of air pollution. We apply different machine learning models to significantly improve traditional forecasts of PM10, NOx, and O3 in Stockholm, Sweden. It is shown that forecasts of all air pollutants are improved by the input of lagged measurements and taking calendar information into account. The final modelled errors are substantially smaller than uncertainties in the measurements.
Natalie M. Mahowald, Longlei Li, Samuel Albani, Douglas S. Hamilton, and Jasper F. Kok
Atmos. Chem. Phys., 24, 533–551, https://doi.org/10.5194/acp-24-533-2024, https://doi.org/10.5194/acp-24-533-2024, 2024
Short summary
Short summary
Estimating past aerosol radiative effects and their uncertainties is an important topic in climate science. Aerosol radiative effects propagate into large uncertainties in estimates of how present and future climate evolves with changing greenhouse gas emissions. A deeper understanding of how aerosols interacted with the atmospheric energy budget under past climates is hindered in part by a lack of relevant paleo-observations and in part because less attention has been paid to the problem.
Min Zhao, Tie Dai, Daisuke Goto, Hao Wang, and Guangyu Shi
Atmos. Chem. Phys., 24, 235–258, https://doi.org/10.5194/acp-24-235-2024, https://doi.org/10.5194/acp-24-235-2024, 2024
Short summary
Short summary
During a springtime pollution input from South Asia to the Tibetan Plateau, we combined atmospheric chemistry modeling and data assimilation methods to assimilate and forecast aerosols from South Asia and the Tibetan Plateau. Assimilation of observations over a whole time window leads to a more reasonable distribution of daily variations in the aerosol forecast field. We also find that aerosol assimilation can improve the surface solar energy forecast in the Tibetan Plateau region.
Yuling Hu, Haipeng Yu, Shichang Kang, Junhua Yang, Mukesh Rai, Xiufeng Yin, Xintong Chen, and Pengfei Chen
Atmos. Chem. Phys., 24, 85–107, https://doi.org/10.5194/acp-24-85-2024, https://doi.org/10.5194/acp-24-85-2024, 2024
Short summary
Short summary
The Tibetan Plateau (TP) saw a record-breaking aerosol pollution event from April 20 to May 10, 2016. We studied the impact of aerosol–meteorology feedback on the transboundary transport flux of black carbon (BC) during this severe pollution event. It was found that the aerosol–meteorology feedback decreases the transboundary transport flux of BC from the central and western Himalayas towards the TP. This study is of great significance for the protection of the ecological environment of the TP.
Xiaodong Zhang, Ruiyu Zhugu, Xiaohu Jian, Xinrui Liu, Kaijie Chen, Shu Tao, Junfeng Liu, Hong Gao, Tao Huang, and Jianmin Ma
Atmos. Chem. Phys., 23, 15629–15642, https://doi.org/10.5194/acp-23-15629-2023, https://doi.org/10.5194/acp-23-15629-2023, 2023
Short summary
Short summary
WRF-Chem modeling was conducted to assess impacts of Western Pacific Subtropical High Pressure (WPSH) on interannual fluctuations of O3 pollution in China. We find that, while precursor emissions dominated the long-term trend and magnitude of O3 from 1999 to 2017, WPSH determined interannual variation of summer O3. The response of O3 pollution to WPSH in major urban clusters depended on the proximity of these urban areas to WPSH. The results could help long-term O3 pollution mitigation planning.
Jim M. Haywood, Andy Jones, Anthony C. Jones, Paul Halloran, and Philip J. Rasch
Atmos. Chem. Phys., 23, 15305–15324, https://doi.org/10.5194/acp-23-15305-2023, https://doi.org/10.5194/acp-23-15305-2023, 2023
Short summary
Short summary
The difficulties in ameliorating global warming and the associated climate change via conventional mitigation are well documented, with all climate model scenarios exceeding 1.5 °C above the preindustrial level in the near future. There is therefore a growing interest in geoengineering to reflect a greater proportion of sunlight back to space and offset some of the global warming. We use a state-of-the-art Earth-system model to investigate two of the most prominent geoengineering strategies.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, https://doi.org/10.5194/acp-23-15149-2023, 2023
Short summary
Short summary
Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six models to surface activity of strongly surface active aerosol and find significant differences between the models, especially with large fractions of surfactant in the dry particles.
Da Gao, Bin Zhao, Shuxiao Wang, Yuan Wang, Brian Gaudet, Yun Zhu, Xiaochun Wang, Jiewen Shen, Shengyue Li, Yicong He, Dejia Yin, and Zhaoxin Dong
Atmos. Chem. Phys., 23, 14359–14373, https://doi.org/10.5194/acp-23-14359-2023, https://doi.org/10.5194/acp-23-14359-2023, 2023
Short summary
Short summary
Surface PM2.5 concentrations can be enhanced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). In this study, we found PM2.5 enhancement induced by ACIs shows a significantly smaller decrease ratio than that induced by ARIs in China with anthropogenic emission reduction from 2013 to 2021, making ACIs more important for enhancing PM2.5 concentrations. ACI-induced PM2.5 enhancement needs to be emphatically considered to meet the national PM2.5 air quality standard.
Miaoqing Xu, Jing Yang, Manchun Li, Xiao Chen, Qiancheng Lv, Qi Yao, Bingbo Gao, and Ziyue Chen
Atmos. Chem. Phys., 23, 14065–14076, https://doi.org/10.5194/acp-23-14065-2023, https://doi.org/10.5194/acp-23-14065-2023, 2023
Short summary
Short summary
Although the temporal-scale effects on PM2.5–meteorology associations have been discussed, no quantitative evidence has proved this before. Based on rare 3 h meteorology data, we revealed that the dominant meteorological factor for PM2.5 concentrations across China extracted at the 3 h and 24 h scales presented large variations. This research suggests that data sources of different temporal scales should be comprehensively considered for better attribution and prevention of airborne pollution.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
Short summary
Short summary
To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Michael Weger and Bernd Heinold
Atmos. Chem. Phys., 23, 13769–13790, https://doi.org/10.5194/acp-23-13769-2023, https://doi.org/10.5194/acp-23-13769-2023, 2023
Short summary
Short summary
This study investigates the effects of complex terrain on air pollution trapping using a numerical model which simulates the dispersion of emissions under real meteorological conditions. The additionally simulated aerosol age allows us to distinguish areas that accumulate aerosol over time from areas that are more influenced by fresh emissions. The Dresden Basin, a widened section of the Elbe Valley in eastern Germany, is selected as the target area in a case study to demonstrate the concept.
Noora Hyttinen
Atmos. Chem. Phys., 23, 13809–13817, https://doi.org/10.5194/acp-23-13809-2023, https://doi.org/10.5194/acp-23-13809-2023, 2023
Short summary
Short summary
Water activity in aerosol particles describes how particles respond to variations in relative humidity. Here, water activities were calculated for a set of 80 salts that may be present in aerosol particles using a state-of-the-art quantum-chemistry-based method. The effect of the dissociated salt on water activity varies with both the cation and anion. Most of the studied salts increase water uptake compared to pure water-soluble organic particles.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
EGUsphere, https://doi.org/10.5194/egusphere-2023-2161, https://doi.org/10.5194/egusphere-2023-2161, 2023
Short summary
Short summary
Single-layer warm liquid clouds cover nearly one-third of the earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth Systems Model estimates of the radiative forcing due to the interactions of aerosols with clouds due to warm rain processes.
Lambert Delbeke, Chien Wang, Pierre Tulet, Cyrielle Denjean, Maurin Zouzoua, Nicolas Maury, and Adrien Deroubaix
Atmos. Chem. Phys., 23, 13329–13354, https://doi.org/10.5194/acp-23-13329-2023, https://doi.org/10.5194/acp-23-13329-2023, 2023
Short summary
Short summary
Low-level stratiform clouds (LLSCs) appear frequently over southern West Africa during the West African monsoon. Local and remote aerosol sources (biomass burning aerosols from central Africa) play a significant role in the LLSC life cycle. Based on measurements by the DACCIWA campaign, large-eddy simulation (LES) was conducted using different aerosol scenarios. The results show that both indirect and semi-direct effects can act individually or jointly to influence the life cycles of LLSCs.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
Short summary
Short summary
Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
EGUsphere, https://doi.org/10.5194/egusphere-2023-2070, https://doi.org/10.5194/egusphere-2023-2070, 2023
Short summary
Short summary
We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the Southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass-burning plumes.
Jiawei Li, Zhiwei Han, Pingqing Fu, and Xiaohong Yao
EGUsphere, https://doi.org/10.5194/egusphere-2023-1916, https://doi.org/10.5194/egusphere-2023-1916, 2023
Short summary
Short summary
Organic aerosols of marine origin are important to aerosol climatic effect, but are poorly understood at present. For the first time, an on-line coupled regional chemistry-climate model is applied to explore the characteristics of emission, distribution, direct and indirect radiative effects of marine organic aerosols for the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Jing Li, Nan Wu, An Ning, and Xiuhui Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2084, https://doi.org/10.5194/egusphere-2023-2084, 2023
Short summary
Short summary
Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas, however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3-HIO2-based nucleation is unclear. Our study provides molecular-level evidence that MSA can efficiently promote the formation of HIO3-HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help to deeply understand marine NPF events with burst of iodine particles.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
EGUsphere, https://doi.org/10.5194/egusphere-2023-1754, https://doi.org/10.5194/egusphere-2023-1754, 2023
Short summary
Short summary
A new aerosol-type classification algorithm was proposed. It includes an optical database building by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated using the new algorithm to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Yahui Che, Bofu Yu, and Katherine Bracco
EGUsphere, https://doi.org/10.5194/egusphere-2023-1710, https://doi.org/10.5194/egusphere-2023-1710, 2023
Short summary
Short summary
Dust events over Australia concentrated in the north and southeast in spring, and can occur anywhere to the east in summer, with the dust season finishing in autumn using a combined DAOD. Near-surface dust concentrations were the highest over the cente, and weakened radially away the center, decreasing along two main pathways. Total dust emission was about 40 Mt (mega-tonnes) per year from1980–2020, of which nearly 50 % was deposited on land; the rest as net export from the Australian continent.
Jun-Wei Xu, Jintai Lin, Dan Tong, and Lulu Chen
Atmos. Chem. Phys., 23, 10075–10089, https://doi.org/10.5194/acp-23-10075-2023, https://doi.org/10.5194/acp-23-10075-2023, 2023
Short summary
Short summary
This study highlights the necessity of a low-carbon pathway in foreign countries for China to achieve air quality goals and to protect public health. We find that adopting the low-carbon instead of the fossil-fuel-intensive pathway in foreign countries would prevent 63 000–270 000 transboundary PM2.5-associated mortalities in China in 2060. Our study provides direct evidence of the necessity of inter-regional cooperation for air quality improvement.
Xurong Wang, Qiaoqiao Wang, Maria Prass, Christopher Pöhlker, Daniel Moran-Zuloaga, Paulo Artaxo, Jianwei Gu, Ning Yang, Xiajie Yang, Jiangchuan Tao, Juan Hong, Nan Ma, Yafang Cheng, Hang Su, and Meinrat O. Andreae
Atmos. Chem. Phys., 23, 9993–10014, https://doi.org/10.5194/acp-23-9993-2023, https://doi.org/10.5194/acp-23-9993-2023, 2023
Short summary
Short summary
In this work, with an optimized particle mass size distribution, we captured observed aerosol optical depth (AOD) and coarse aerosol concentrations over source and/or receptor regions well, demonstrating good performance in simulating export of African dust toward the Amazon Basin. In addition to factors controlling the transatlantic transport of African dust, the study investigated the impact of African dust over the Amazon Basin, including the nutrient inputs associated with dust deposition.
Christof Gerhard Beer, Johannes Hendricks, and Mattia Righi
EGUsphere, https://doi.org/10.5194/egusphere-2023-1983, https://doi.org/10.5194/egusphere-2023-1983, 2023
Short summary
Short summary
Ice-nucleating aerosol particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol-climate model to analyse INP-induced cirrus changes and the resulting climate impact. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP-cirrus effect.
Athanasios Tsikerdekis, Otto P. Hasekamp, Nick A. J. Schutgens, and Qirui Zhong
Atmos. Chem. Phys., 23, 9495–9524, https://doi.org/10.5194/acp-23-9495-2023, https://doi.org/10.5194/acp-23-9495-2023, 2023
Short summary
Short summary
Aerosols are tiny particles of different substances (species) that can be emitted into the atmosphere by natural processes or by anthropogenic activities. However, the actual aerosol emission amount per species is highly uncertain. Thus in this work we correct the aerosol emissions used to drive a global aerosol–climate model using satellite observations through a process called data assimilation. These more accurate aerosol emissions can lead to a more accurate weather and climate prediction.
Jani Strömberg, Xiaoyu Li, Mona Kurppa, Heino Kuuluvainen, Liisa Pirjola, and Leena Järvi
Atmos. Chem. Phys., 23, 9347–9364, https://doi.org/10.5194/acp-23-9347-2023, https://doi.org/10.5194/acp-23-9347-2023, 2023
Short summary
Short summary
We conclude that with low wind speeds, solar radiation has a larger decreasing effect (53 %) on pollutant concentrations than aerosol processes (18 %). Additionally, our results showed that with solar radiation included, pollutant concentrations were closer to observations (−13 %) than with only aerosol processes (+98 %). This has implications when planning simulations under calm conditions such as in our case and when deciding whether or not simulations need to include these processes.
Guanyu Liu, Jing Li, and Tong Ying
Atmos. Chem. Phys., 23, 9217–9228, https://doi.org/10.5194/acp-23-9217-2023, https://doi.org/10.5194/acp-23-9217-2023, 2023
Short summary
Short summary
Fires in Australia are positively correlated with the El Niño–Southern Oscillation (ENSO). However, the correlation between ENSO and the Australian Fire Weather Index (FWI) increases from 0.17 to 0.70 when the Atlantic Multidecadal Oscillation (AMO) shifts from a negative to positive phase. This is explained by the teleconnection effect through which the warmer AMO generates Rossby wave trains and results in high pressures and a weather condition conducive to wildfires.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
EGUsphere, https://doi.org/10.5194/egusphere-2023-1749, https://doi.org/10.5194/egusphere-2023-1749, 2023
Short summary
Short summary
In 2020–2022, several international agencies and media reported severe winter dust intrusions in Europe. Although winter dust intrusions are more common in the eastern Mediterranean, these events largely affected the western Mediterranean and Canary Islands. The present work provides a catalogue of dust events over the western Mediterranean region and describes their characteristics during the climatological (2003–2019) and recent anomalous (2020–2022) periods.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2023-1444, https://doi.org/10.5194/egusphere-2023-1444, 2023
Short summary
Short summary
Secondary organic aerosols (SOA) can exist in liquid, semi-solid or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in the northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
EGUsphere, https://doi.org/10.5194/egusphere-2023-1830, https://doi.org/10.5194/egusphere-2023-1830, 2023
Short summary
Short summary
We quantified different drivers of biogenic VOC (BVOC) emission trends over the past 20 years at global and regional scales. The results showed that global greening trends significantly boost BVOC emissions and the deforestation reduce BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia also significantly enhance BVOC emissions. The results can deepen our understanding of long-term BVOC emission trends in hotspots.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Yuhang Wang, Minghuai Wang, Hailong Wang, and Xiu-Qun Yang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1628, https://doi.org/10.5194/egusphere-2023-1628, 2023
Short summary
Short summary
Fire management has long been a challenge. Here we report the spring-peak fire activities over southern Mexico and Central America (SMCA) have a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by a quasi-biennial variability of precipitation and is further amplified by positive feedback of fire-precipitation interaction on short timescales. This work highlights the importance of fire-climate interactions in shaping fires on interannual scale.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
Short summary
Short summary
Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
EGUsphere, https://doi.org/10.5194/egusphere-2023-1096, https://doi.org/10.5194/egusphere-2023-1096, 2023
Short summary
Short summary
Aerosols influence the Earth’s Energy balance. The uncertainty in this radiative forcing is large, depending partly on uncertainty in measurements of aerosol optical properties. We develop a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty but that non-aerosol uncertainties must also be considered.
Chenwei Fang, Jim M. Haywood, Ju Liang, Ben T. Johnson, Ying Chen, and Bin Zhu
Atmos. Chem. Phys., 23, 8341–8368, https://doi.org/10.5194/acp-23-8341-2023, https://doi.org/10.5194/acp-23-8341-2023, 2023
Short summary
Short summary
The responses of Asian summer monsoon duration and intensity to air pollution mitigation are identified given the net-zero future. We show that reducing scattering aerosols makes the rainy season longer and stronger across South Asia and East Asia but that absorbing aerosol reduction has the opposite effect. Our results hint at distinct monsoon responses to emission controls that target different aerosols.
Yue Peng, Hong Wang, Xiaoye Zhang, Zhaodong Liu, Wenjie Zhang, Siting Li, Chen Han, and Huizheng Che
Atmos. Chem. Phys., 23, 8325–8339, https://doi.org/10.5194/acp-23-8325-2023, https://doi.org/10.5194/acp-23-8325-2023, 2023
Short summary
Short summary
This study demonstrates a strong link between local circulation, aerosol–radiation interaction (ARI), and haze pollution. Under the weak weather-scale systems, the typical local circulation driven by mountainous topography is the main cause of pollutant distribution in the Beijing–Tianjin–Hebei region, and the ARI mechanism amplifies this influence of local circulation on pollutants, making haze pollution aggravated by the superposition of both.
Yuan Zhao, Xu Yue, Yang Cao, Jun Zhu, Chenguang Tian, Hao Zhou, Yuwen Chen, Yihan Hu, Weijie Fu, and Xu Zhao
Atmos. Chem. Phys., 23, 7823–7838, https://doi.org/10.5194/acp-23-7823-2023, https://doi.org/10.5194/acp-23-7823-2023, 2023
Short summary
Short summary
We project the future changes of dust emissions and loading using an ensemble of model outputs from the Coupled Model Intercomparison Project version 6 under four scenarios. We find increased dust emissions and loading in North Africa, due to increased drought and strengthened surface wind, and decreased dust loading over Asia, following enhanced precipitation. Such a spatial pattern remains similar, though the regional intensity varies among different scenarios.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 23, 7741–7765, https://doi.org/10.5194/acp-23-7741-2023, https://doi.org/10.5194/acp-23-7741-2023, 2023
Short summary
Short summary
Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The enrichment of compounds in the surface of an aerosol particle may lead to depletion of that species in the interior bulk of the particle. We present a framework for modeling the equilibrium bulk–surface partitioning of mixed organic–inorganic particles, including cases of co-condensation of semivolatile organic compounds and species with extremely limited solubility in the bulk or surface of a particle.
Sampa Das, Peter Colarco, Huisheng Bian, and Santiago Gasso
EGUsphere, https://doi.org/10.5194/egusphere-2023-1311, https://doi.org/10.5194/egusphere-2023-1311, 2023
Short summary
Short summary
The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 23, 6743–6773, https://doi.org/10.5194/acp-23-6743-2023, https://doi.org/10.5194/acp-23-6743-2023, 2023
Short summary
Short summary
We determine what causes long-term trends in short-wave (SW) radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol, and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute to changes in clouds caused by greenhouse gas-induced warming.
Danny M. Leung, Jasper F. Kok, Longlei Li, Gregory S. Okin, Catherine Prigent, Martina Klose, Carlos Pérez García-Pando, Laurent Menut, Natalie M. Mahowald, David M. Lawrence, and Marcelo Chamecki
Atmos. Chem. Phys., 23, 6487–6523, https://doi.org/10.5194/acp-23-6487-2023, https://doi.org/10.5194/acp-23-6487-2023, 2023
Short summary
Short summary
Desert dust modeling is important for understanding climate change, as dust regulates the atmosphere's greenhouse effect and radiation. This study formulates and proposes a more physical and realistic desert dust emission scheme for global and regional climate models. By considering more aeolian processes in our emission scheme, our simulations match better against dust observations than existing schemes. We believe this work is vital in improving dust representation in climate models.
Neeldip Barman and Sharad Gokhale
Atmos. Chem. Phys., 23, 6197–6215, https://doi.org/10.5194/acp-23-6197-2023, https://doi.org/10.5194/acp-23-6197-2023, 2023
Short summary
Short summary
The study shows that during the pre-monsoon season transported aerosols, especially from the Indo-Gangetic Plain (IGP), have a greater impact with respect to air pollution, radiative forcing and rainfall over north-east (NE) India than emissions from within NE India itself. Hence, controlling emissions in the IGP will be significantly more fruitful in reducing pollution as well as climatic impacts over this region.
Cited articles
Angell, C.: Relaxation in liquids, polymers and plastic crystals – strong/fragile
patterns and problems, J. Non-Cryst. Solids, 131-133, 13–31, https://doi.org/10.1016/0022-3093(91)90266-9, 1991.
Barsanti, K. C., Kroll, J. H., and Thornton, J. A.: Formation of low-volatility
organic compounds in the atmosphere: recent advancements and insights, J. Phys.
Chem. Lett., 8, 1503–1511, https://doi.org/10.1021/acs.jpclett.6b02969, 2017.
Bastelberger, S., Krieger, U. K., Luo, B., and Peter, T.: Diffusivity
measurements of volatile organics in levitated viscous aerosol particles, Atmos.
Chem. Phys., 17, 8453–8471, https://doi.org/10.5194/acp-17-8453-2017, 2017.
Bateman, A. P., Gong, Z., Harder, T. H., de Sá, S. S., Wang, B., Castillo,
P., China, S., Liu, Y., O'Brien, R. E., Palm, B. B., Shiu, H. W., Cirino, G. G.,
Thalman, R., Adachi, K., Alexander, M. L., Artaxo, P., Bertram, A. K., Buseck,
P. R., Gilles, M. K., Jimenez, J. L., Laskin, A., Manzi, A. O., Sedlacek, A.,
Souza, R. A. F., Wang, J., Zaveri, R., and Martin, S. T.: Anthropogenic
influences on the physical state of submicron particulate matter over a
tropical forest, Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, 2017.
Bianchi, F., Tröstl, J., Junninen, H., Frege, C., Henne, S., Hoyle, C. R.,
Molteni, U., Herrmann, E., Adamov, A., Bukowiecki, N., Chen, X., Duplissy, J.,
Gysel, M., Hutterli, M., Kangasluoma, J., Kontkanen, J., Kürten, A.,
Manninen, H. E., Münch, S., Peräkylä, O., Petäjä, T., Rondo,
L., Williamson, C., Weingartner, E., Curtius, J., Worsnop, D. R., Kulmala, M.,
Dommen, J., and Baltensperger, U.: New particle formation in the free troposphere:
A question of chemistry and timing, Science, 352, 1109–1112, https://doi.org/10.1126/science.aad5456, 2016.
Booth, A. M., Murphy, B., Riipinen, I., Percival, C. J., and Topping, D. O.:
Connecting bulk viscosity measurements to kinetic limitations on attaining
equilibrium for a model aerosol composition, Environ. Sci. Technol., 48,
9298–9305, https://doi.org/10.1021/es501705c, 2014.
Boyd, C. M., Nah, T., Xu, L., Berkemeier, T., and Ng, N. L.: Secondary organic
aerosol (SOA) from nitrate radical oxidation of monoterpenes: effects of
temperature, dilution, and humidity on aerosol formation, mixing, and evaporation,
Environ. Sci. Technol., 51, 7831–7841, https://doi.org/10.1021/acs.est.7b01460, 2017.
Cheng, Y., Su, H., Koop, T., Mikhailov, E., and Pöschl, U.: Size dependence
of phase transitions in aerosol nanoparticles, Nat. Commun., 6, 5923,
https://doi.org/10.1038/ncomms6923, 2015.
Chenyakin, Y., Ullmann, D. A., Evoy, E., Renbaum-Wolff, L., Kamal, S., and
Bertram, A. K.: Diffusion coefficients of organic molecules in sucrose–water
solutions and comparison with Stokes–Einstein predictions, Atmos. Chem. Phys.,
17, 2423–2435, https://doi.org/10.5194/acp-17-2423-2017, 2017.
DeRieux, W. S. W., Li, Y., Lin, P., Laskin, J., Laskin, A., Bertram, A. K.,
Nizkorodov, S. A., and Shiraiwa, M.: Predicting the glass transition temperature
and viscosity of secondary organic material using molecular composition, Atmos.
Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, 2018.
Fowler, K., Connolly, P. J., Topping, D. O., and O'Meara, S.: Maxwell–Stefan
diffusion: a framework for predicting condensed phase diffusion and phase
separation in atmospheric aerosol, Atmos. Chem. Phys., 18, 1629–1642,
https://doi.org/10.5194/acp-18-1629-2018, 2018.
Gong, Z., Han, Y., Liu, P., Ye, J., Keutsch, F. N., McKinney, K. A., and Martin,
S. T.: Influence of particle physical state on the uptake of medium-sized
organic molecules, Environ. Sci. Technol., 52, 8381–8389, https://doi.org/10.1021/acs.est.8b02119, 2018.
Gorkowski, K., Donahue, N. M., and Sullivan, R. C.: Emulsified and liquid–liquid
phase-separated states of α-pinene secondary organic aerosol determined
using aerosol optical tweezers, Environ. Sci. Technol., 51, 12154–12163,
https://doi.org/10.1021/acs.est.7b03250, 2017.
Gunthe, S. S., King, S. M., Rose, D., Chen, Q., Roldin, P., Farmer, D. K.,
Jimenez, J. L., Artaxo, P., Andreae, M. O., Martin, S. T., and Pöschl, U.:
Cloud condensation nuclei in pristine tropical rainforest air of Amazonia:
size-resolved measurements and modeling of atmospheric aerosol composition and
CCN activity, Atmos. Chem. Phys., 9, 7551–7575, https://doi.org/10.5194/acp-9-7551-2009, 2009.
Hosny, N., Fitzgerald, C., Vyšniauskas, A., Athanasiadis, A., Berkemeier,
T., Uygur, N., Pöschl, U., Shiraiwa, M., Kalberer, M., Pope, F., and Kuimova,
M. K.: Direct imaging of changes in aerosol particle viscosity upon hydration
and chemical aging, Chem. Sci., 7, 1357–1367, https://doi.org/10.1039/C5SC02959G, 2016.
International Organization for Standardization: Standard Atmosphere, ISO 2533:1975,
available at: https://www.iso.org/standard/7472.html (last access:
3 May 2019), 1975.
Julin, J., Winkler, P. M., Donahue, N. M., Wagner, P. E., and Riipinen, I.:
Near-unity mass accommodation coefficient of organic molecules of varying
structure, Environ. Sci. Technol., 48, 12083–12089, https://doi.org/10.1021/es501816h, 2014.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J.,
Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J.,
Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat,
G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou,
E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review,
Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Knopf, D. A., Alpert, P. A., and Wang, B.: The role of organic aerosol in
atmospheric ice nucleation: a review, ACS Earth Space Chem., 2, 168–202,
https://doi.org/10.1021/acsearthspacechem.7b00120, 2018.
Koop, T., Bookhold, J., Shiraiwa, M., and Poschl, U.: Glass transition and
phase state of organic compounds: dependency on molecular properties and
implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem.
Phys., 13, 19238–19255, https://doi.org/10.1039/C1CP22617G, 2011.
Li, Y. and Shiraiwa, M.: Molecular corridors, volatility and particle phase
state in secondary organic aerosols, in: Multiphase Environmental Chemistry
in the Atmosphere, edited by: Hunt S. W., Laskin A., and Nizkorodov S. A.,
ACS Symposium Ser., 1299, 209–244, https://doi.org/10.1021/bk-2018-1299.ch011, 2018.
Liu, C., Shi, S., Weschler, C., Zhao, B., and Zhang, Y.: Analysis of the dynamic
interaction between SVOCs and airborne particles, Aerosol Sci. Tech., 47,
125–136, https://doi.org/10.1080/02786826.2012.730163, 2013.
Liu, P., Li, Y. J., Wang, Y., Gilles, M. K., Zaveri, R. A., Bertram, A. K., and
Martin, S. T.: Lability of secondary organic particulate matter, P. Natl. Acad.
Sci. USA, 113, 12643–12648, https://doi.org/10.1021/acscentsci.7b00452, 2016.
Liu, P., Li, Y. J., Wang, Y., Bateman, A. P., Zhang, Y., Gong, Z., Bertram, A.
K., and Martin, S. T.: Highly viscous states affect the browning of atmospheric
organic particulate matter, ACS Cent. Sci., 4, 207–215, https://doi.org/10.1021/acscentsci.7b00452, 2018.
Liu, Y., Wu, Z., Wang, Y., Xiao, Y., Gu, F., Zheng, J., Tan, T., Shang, D., Wu,
Y., Zeng, L., Hu, M., Bateman, A. P., and Martin, S. T.: Submicrometer particles
are in the liquid state during heavy haze episodes in the urban atmosphere of
Beijing, China, Environ. Sci. Technol. Lett., 4, 427–432, https://doi.org/10.1021/acs.estlett.7b00352, 2017.
Loza, C. L., Coggon, M. M., Nguyen, T. B., Zuend, A., Flagan, R. C., and
Seinfeld, J. H.: On the mixing and evaporation of secondary organic aerosol
components, Environ. Sci. Technol., 47, 6173–6180, https://doi.org/10.1021/es400979k, 2013.
Maclean, A. M., Butenhoff, C. L., Grayson, J. W., Barsanti, K., Jimenez, J. L.,
and Bertram, A. K.: Mixing times of organic molecules within secondary organic
aerosol particles: a global planetary boundary layer perspective, Atmos. Chem.
Phys., 17, 13037–13048, https://doi.org/10.5194/acp-17-13037-2017, 2017.
Mai, H., Shiraiwa, M., Flagan, R. C., and Seinfeld, J. H.: Under what conditions
can equilibrium gas–particle partitioning be expected to hold in the atmosphere?,
Environ. Sci. Technol., 49, 11485–11491, https://doi.org/10.1021/acs.est.5b02587, 2015.
Maria, S. F., Russell, L. M., Gilles, M. K., and Myneni, S. C. B.: Organic
aerosol growth mechanisms and their climate-forcing implications, Science,
306, 1921–1924, https://doi.org/10.1126/science.1103491, 2004.
Marshall, F. H., Miles, R. E., Song, Y.-C., Ohm, P. B., Power, R. M., Reid, J.
P., and Dutcher, C. S.: Diffusion and reactivity in ultraviscous aerosol and
the correlation with particle viscosity, Chem. Sci., 7, 1298–1308, https://doi.org/10.1039/C5SC03223G, 2016.
Mu, Q., Shiraiwa, M., Octaviani, M., Ma, N., Ding, A., Su, H., Lammel, G.,
Pöschl, U., and Cheng, Y.: Temperature effect on phase state and reactivity
controls atmospheric multiphase chemistry and transport of PAHs, Sci. Adv., 4,
eaap7314, https://doi.org/10.1126/sciadv.aap7314, 2018.
O'Meara, S., Topping, D. O., and McFiggans, G.: The rate of equilibration of
viscous aerosol particles, Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, 2016.
Pajunoja, A., Hu, W., Leong, Y. J., Taylor, N. F., Miettinen, P., Palm, B. B.,
Mikkonen, S., Collins, D. R., Jimenez, J. L., and Virtanen, A.: Phase state of
ambient aerosol linked with water uptake and chemical aging in the southeastern US,
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, 2016.
Pankow, J. F.: An absorption model of gas-particle partitioning of organic-compounds
in the atmosphere, Atmos. Environ., 28, 185–188, https://doi.org/10.1016/1352-2310(94)90093-0, 1994.
Perraud, V., Bruns, E. A., Ezell, M. J., Johnson, S. N., Yu, Y., Alexander, M.
L., Zelenyuk, A., Imre, D., Chang, W. L., Dabdub, D., Pankow, J. F., and
Finlayson-Pitts, B. J.: Nonequilibrium atmospheric secondary organic aerosol
formation and growth, P. Natl. Acad. Sci. USA, 109, 2836–2841, https://doi.org/10.1073/pnas.1119909109, 2012.
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of
hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys.,
7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007.
Petters, S. S., Kreidenweis, S. M., Grieshop, A. P., Ziemann, P. J., and Petters,
M. D.: Temperature- and humidity-dependent phase states of secondary organic
aerosols, Geophys. Res. Lett., 46, 1005–1013, https://doi.org/10.1029/2018GL080563, 2019.
Pfrang, C., Shiraiwa, M., and Pöschl, U.: Chemical ageing and transformation
of diffusivity in semi-solid multi-component organic aerosol particles, Atmos.
Chem. Phys., 11, 7343–7354, https://doi.org/10.5194/acp-11-7343-2011, 2011.
Pöhlker, C., Wiedemann, K. T., Sinha, B., Shiraiwa, M., Gunthe, S. S.,
Smith, M., Su, H., Artaxo, P., Chen, Q., Cheng, Y., Elbert, W., Gilles, M. K.,
Kilcoyne, A. L. D., Moffet, R. C., Weigand, M., Martin, S. T., Pöschl, U.,
and Andreae, M. O.: Biogenic potassium salt particles as seeds for secondary
organic aerosol in the Amazon, Science, 337, 1075–1078, https://doi.org/10.1126/science.1223264, 2012.
Price, H. C., Mattsson, J., Zhang, Y., Bertram, A. K., Davies, J. F., Grayson,
J. W., Martin, S. T., O'Sullivan, D., Reid, J. P., Rickards, A. M., and Murray,
B. J.: Water diffusion in atmospherically relevant α-pinene secondary
organic material, Chem. Sci., 6, 4876–4883, https://doi.org/10.1039/c5sc00685f, 2015.
Pye, H. O. T., Murphy, B. N., Xu, L., Ng, N. L., Carlton, A. G., Guo, H., Weber,
R., Vasilakos, P., Appel, K. W., Budisulistiorini, S. H., Surratt, J. D., Nenes,
A., Hu, W., Jimenez, J. L., Isaacman-VanWertz, G., Misztal, P. K., and Goldstein,
A. H.: On the implications of aerosol liquid water and phase separation for
organic aerosol mass, Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, 2017.
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters,
M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant
organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018.
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.
Riedel, T. P., Lin, Y. H., Zhang, Z., Chu, K., Thornton, J. A., Vizuete, W.,
Gold, A., and Surratt, J. D.: Constraining condensed-phase formation kinetics
of secondary organic aerosol components from isoprene epoxydiols, Atmos. Chem.
Phys., 16, 1245–1254, https://doi.org/10.5194/acp-16-1245-2016, 2016.
Riipinen, I., Pierce, J. R., Yli-Juuti, T., Nieminen, T., Hakkinen, S., Ehn,
M., Junninen, H., Lehtipalo, K., Petaja, T., Slowik, J., Chang, R., Shantz, N.
C., Abbatt, J., Leaitch, W. R., Kerminen, V. M., Worsnop, D. R., Pandis, S. N.,
Donahue, N. M., and Kulmala, M.: Organic condensation: a vital link connecting
aerosol formation to cloud condensation nuclei (CCN) concentrations, Atmos.
Chem. Phys., 11, 3865–3878, https://doi.org/10.5194/acp-11-3865-2011, 2011.
Riipinen, I., Yli-Juuti, T., Pierce, J. R., Petaja, T., Worsnop, D. R., Kulmala,
M., and Donahue, N. M.: The contribution of organics to atmospheric nanoparticle
growth, Nat. Geosci., 5, 453–458, https://doi.org/10.1038/ngeo1499, 2012.
Roldin, P., Eriksson, A. C., Nordin, E. Z., Hermansson, E., Mogensen, D.,
Rusanen, A., Boy, M., Swietlicki, E., Svenningsson, B., Zelenyuk, A., and
Pagels, J.: Modelling non-equilibrium secondary organic aerosol formation and
evaporation with the aerosol dynamics, gas- and particle-phase chemistry
kinetic multilayer model ADCHAM, Atmos. Chem. Phys., 14, 7953–7993,
https://doi.org/10.5194/acp-14-7953-2014, 2014.
Rothfuss, N. E. and Petters, M. D.: Characterization of the temperature and
humidity-dependent phase diagram of amorphous nanoscale organic aerosols, Phys.
Chem. Chem. Phys., 19, 6532–6545, https://doi.org/10.1039/C6CP08593H, 2017.
Saha, P. K. and Grieshop, A. P.: Exploring divergent volatility properties
from yield and thermodenuder measurements of secondary organic aerosol from
α-pinene ozonolysis, Environ. Sci. Technol., 50, 5740–5749,
https://doi.org/10.1021/acs.est.6b00303, 2016.
Saleh, R., Donahue, N. M., and Robinson, A. L.: Time scales for gas-particle
partitioning equilibration of secondary organic aerosol formed from alpha-pinene
ozonolysis, Environ. Sci. Technol., 47, 5588–5594, https://doi.org/10.1021/es400078d, 2013.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics – From
air pollution to climate change, John Wiley & Sons, Inc., New York, 2006.
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric
secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801,
https://doi.org/10.1029/2012GL054008, 2012.
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, https://doi.org/10.1073/pnas.1103045108, 2011.
Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer
model of gas-particle interactions in aerosols and clouds (KM-GAP): linking
condensation, evaporation and chemical reactions of organics, oxidants and
water, Atmos. Chem. Phys., 12, 2777–2794, https://doi.org/10.5194/acp-12-2777-2012, 2012.
Shiraiwa, M., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend,
A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal
particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA,
110, 11746–11750, https://doi.org/10.1073/pnas.1307501110, 2013a.
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, https://doi.org/10.1039/C3CP51595H, 2013b.
Shiraiwa, M., Li, Y., Tsimpidi, A. P., Karydis, V. A., Berkemeier, T., Pandis,
S. N., Lelieveld, J., Koop, T., and Pöschl, U.: Global distribution of
particle phase state in atmospheric secondary organic aerosols, Nat. Commun.,
8, 15002, https://doi.org/10.1038/ncomms15002, 2017.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B.,
Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T.,
Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J., Smith,
J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R., Zaveri, R. A.,
Zelenyuk, A., and Zhang, Q.: Recent advances in understanding secondary organic
aerosol: Implications for global climate forcing, Rev. Geophys., 55, 509–559,
https://doi.org/10.1002/2016RG000540, 2017a.
Shrivastava, M., Lou, S., Zelenyuk, A., Easter, R. C., Corley, R. A., Thrall,
B. D., Rasch, P. J., Fast, J. D., Simonich, S. L. M., Shen, H., and Tao, S.:
Global long-range transport and lung cancer risk from polycyclic aromatic
hydrocarbons shielded by coatings of organic aerosol, P. Natl. Acad. Sci. USA,
114, 1246–1251, https://doi.org/10.1073/pnas.1618475114, 2017b.
Slade, J. H., Shiraiwa, M., Arangio, A., Su, H., Pöschl, U., Wang, J., and
Knopf, D. A.: Cloud droplet activation through oxidation of organic aerosol
influenced by temperature and particle phase state, Geophys. Res. Lett., 41,
5297–5306, https://doi.org/10.1002/2014GL060582, 2017.
Tong, H., Arangio, A. M., Lakey, P. S. J., Berkemeier, T., Liu, F., Kampf, C.
J., Brune, W. H., Pöschl, U., and Shiraiwa, M.: Hydroxyl radicals from
secondary organic aerosol decomposition in water, Atmos. Chem. Phys., 16,
1761–1771, https://doi.org/10.5194/acp-16-1761-2016, 2016.
Tröstl, J., Chuang, W. K., Gordon, H., Heinritzi, M., Yan, C., Molteni, U.,
Ahlm, L., Frege, C., Bianchi, F., Wagner, R., Simon, M., Lehtipalo, K.,
Williamson, C., Craven, J. S., Duplissy, J., Adamov, A., Almeida, J., Bernhammer,
A.-K., Breitenlechner, M., Brilke, S., Dias, A., Ehrhart, S., Flagan, R. C.,
Franchin, A., Fuchs, C., Guida, R., Gysel, M., Hansel, A., Hoyle, C. R., Jokinen,
T., Junninen, H., Kangasluoma, J., Keskinen, H., Kim, J., Krapf, M., Kürten,
A., Laaksonen, A., Lawler, M., Leiminger, M., Mathot, S., Möhler, O.,
Nieminen, T., Onnela, A., Petäjä, T., Piel, F. M., Miettinen, P.,
Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Sengupta, K.,
Sipilä, M., Smith, J. N., Steiner, G., Tomè, A., Virtanen, A., Wagner,
A. C., Weingartner, E., Wimmer, D., Winkler, P. M., Ye, P., Carslaw, K. S.,
Curtius, J., Dommen, J., Kirkby, J., Kulmala, M., Riipinen, I., Worsnop, D. R.,
Donahue, N. M., and Baltensperger, U.: The role of low-volatility organic
compounds in initial particle growth in the atmosphere, Nature, 533, 527–531,
https://doi.org/10.1038/nature18271, 2016.
Vaden, T. D., Imre, D., Beránek, J., Shrivastava, M., and Zelenyuk, A.:
Evaporation kinetics and phase of laboratory and ambient secondary organic
aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195, https://doi.org/10.1073/pnas.1013391108, 2011.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P.,
Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U., and
Kulmala, M.: An amorphous solid state of biogenic secondary organic aerosol
particles, Nature, 467, 824–827, https://doi.org/10.1038/nature09455, 2010.
Wang, J., Krejci, R., Giangrande, S., Kuang, C., Barbosa, H. M. J., Brito, J.,
Carbone, S., Chi, X., Comstock, J., Ditas, F., Lavric, J., Manninen, H. E.,
Mei, F., Moran-Zuloaga, D., Pöhlker, C., Pöhlker, M. L., Saturno, J.,
Schmid, B., Souza, R. A. F., Springston, S. R., Tomlinson, J. M., Toto, T.,
Walter, D., Wimmer, D., Smith, J. N., Kulmala, M., Machado, L. A. T., Artaxo,
P., Andreae, M. O., Petäjä, T., and Martin, S. T.: Amazon boundary layer
aerosol concentration sustained by vertical transport during rainfall, Nature,
539, 416–419, https://doi.org/10.1038/nature19819, 2016.
Ye, J., Gordon, C. A., and Chan, A. W. H.: Enhancement in secondary organic
aerosol formation in the presence of preexisting organic particle, Environ. Sci.
Technol., 50, 3572–3579, https://doi.org/10.1021/acs.est.5b05512, 2016.
Ye, Q., Robinson, E. S., Ding, X., Ye, P., Sullivan, R. C., and Donahue, N. M.:
Mixing of secondary organic aerosols versus relative humidity, P. Natl. Acad.
Sci. USA, 113, 12649–12654, https://doi.org/10.1073/pnas.1604536113, 2016.
Ye, Q., Upshur, M. A., Robinson, E. S., Geiger, F. M., Sullivan, R. C., Thomson,
R. J., and Donahue, N. M.: Following particle-particle mixing in atmospheric
secondary organic aerosols by using isotopically labeled terpenes, Chemistry,
4, 318–333, https://doi.org/10.1016/j.chempr.2017.12.008, 2018.
Yli-Juuti, T., Pajunoja, A., Tikkanen, O.-P., Buchholz, A., Faiola, C.,
Väisänen, O., Hao, L., Kari, E., Peräkylä, O., Garmash, O.,
Shiraiwa, M., Ehn, M., Lehtinen, K., and Virtanen, A.: Factors controlling the
evaporation of secondary organic aerosol from α-pinene ozonolysis,
Geophys. Res. Lett., 44, 2562–2570, https://doi.org/10.1002/2016GL072364, 2017.
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, https://doi.org/10.1073/pnas.1206414109, 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,
https://doi.org/10.1080/0144235X.2014.890786, 2014.
Zaveri, R. A., Easter, R. C., Shilling, J. E., and Seinfeld, J. H.: Modeling
kinetic partitioning of secondary organic aerosol and size distribution dynamics:
representing effects of volatility, phase state, and particle-phase reaction,
Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, 2014.
Zaveri, R. A., Shilling, J. E., Zelenyuk, A., Liu, J., Bell, D. M., D'Ambro, E.
L., Gaston, C. J., Thornton, J. A., Laskin, A., Lin, P., Wilson, J., Easter, R.
C., Wang, J., Bertram, A. K., Martin, S. T., Seinfeld, J. H., and Worsnop, D.
R.: Growth kinetics and size distribution dynamics of viscous secondary organic
aerosol, Environ. Sci. Technol., 52, 1191–1199, https://doi.org/10.1021/acs.est.7b04623, 2018.
Zhang, X., Pandis, S. N., and Seinfeld, J. H.: Diffusion-limited versus
quasi-equilibrium aerosol growth, Aerosol Sci. Tech., 46, 874–885,
https://doi.org/10.1080/02786826.2012.679344, 2012.
Zhang, Y., Sanchez, M. S., Douet, C., Wang, Y., Bateman, A. P., Gong, Z., Kuwata,
M., Renbaum-Wolff, L., Sato, B. B., Liu, P. F., Bertram, A. K., Geiger, F. M.,
and Martin, S. T.: Changing shapes and implied viscosities of suspended submicron
particles, Atmos. Chem. Phys., 15, 7819–7829, https://doi.org/10.5194/acp-15-7819-2015, 2015.
Zhang, Y., Chen, Y., Lambe, A. T., Olson, N. E., Lei, Z., Craig, R. L., Zhang,
Z., Gold, A., Onasch, T. B., Jayne, J. T., Worsnop, D. R., Gaston, C. J.,
Thornton, J. A., Vizuete, W., Ault, A. P., and Surratt, J. D.: Effect of the
Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive
Uptake of Isoprene-Derived Epoxydiols (IEPOX), Environ. Sci. Technol. Lett.,
5, 167–174, https://doi.org/10.1021/acs.estlett.8b00044, 2018.
Short summary
Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under...
Altmetrics
Final-revised paper
Preprint