Articles | Volume 19, issue 9
Atmos. Chem. Phys., 19, 5959–5971, 2019
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.
Atmos. Chem. Phys., 19, 5959–5971, 2019
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.
Research article 07 May 2019
Research article | 07 May 2019
Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities
Ying Li and Manabu Shiraiwa
Related authors
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
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-17, https://doi.org/10.5194/acp-2021-17, 2021
Revised manuscript under review for ACP
Short summary
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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 of viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
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
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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
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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
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
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
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
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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
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
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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.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-17, https://doi.org/10.5194/acp-2021-17, 2021
Revised manuscript under review for ACP
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 of viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
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
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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.
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. Discuss., https://doi.org/10.5194/acp-2020-973, https://doi.org/10.5194/acp-2020-973, 2020
Preprint under review for ACP
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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 (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
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
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
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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
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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
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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
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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
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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
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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
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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
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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
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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.
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
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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
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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 | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
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Effectiveness of emission control in reducing PM2.5 pollution in central China during winter haze episodes under various potential synoptic controls
Assessment of meteorology vs. control measures in the China fine particular matter trend from 2013 to 2019 by an environmental meteorology index
A global model perturbed parameter ensemble study of secondary organic aerosol formation
Assimilating aerosol optical properties related to size and absorption from POLDER/PARASOL with an ensemble data assimilation system
Changes in black carbon emissions over Europe due to COVID-19 lockdowns
Effects of marine organic aerosols as sources of immersion-mode ice-nucleating particles on high-latitude mixed-phase clouds
Insights into particulate matter pollution in the North China Plain during wintertime: local contribution or regional transport?
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Response of dust emissions in southwestern North America to 21st century trends in climate, CO2 fertilization, and land use: implications for air quality
Revisiting the relationship between Atlantic dust and tropical cyclone activity using aerosol optical depth reanalyses: 2003–2018
Weaker cooling by aerosols due to dust–pollution interactions
Source backtracking for dust storm emission inversion using an adjoint method: case study of Northeast China
Characteristics of surface energy balance and atmospheric circulation during hot-and-polluted episodes and their synergistic relationships with urban heat islands over the Pearl River Delta region
Study on the impact of three Asian industrial regions on PM2.5 in Taiwan and the process analysis during transport
Particle aging and aerosol–radiation interaction affect volcanic plume dispersion: evidence from the Raikoke 2019 eruption
The warming Tibetan Plateau improves winter air quality in the Sichuan Basin, China
Uncertainty in aerosol radiative forcing impacts the simulated global monsoon in the 20th century
Effects of 3D electric field on saltation during dust storms: an observational and numerical study
Air quality impact of the Northern California Camp Fire of November 2018
Amplification of South Asian haze by water vapour–aerosol interactions
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Rémy Lapere, Laurent Menut, Sylvain Mailler, and Nicolás Huneeus
Atmos. Chem. Phys., 21, 6431–6454, https://doi.org/10.5194/acp-21-6431-2021, https://doi.org/10.5194/acp-21-6431-2021, 2021
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Based on modeling, the transport dynamics of ozone and fine particles in central Chile are investigated. Santiago emissions are found to influence air quality along a 1000 km plume as far as Argentina and northern Chile. In turn, emissions outside the metropolis contribute significantly to its recorded particles concentration. Emissions of precursors from Santiago are found to lead to the formation of a persistent ozone bubble in altitude, a phenomenon which is described for the first time.
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
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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.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Tenglong Shi, Jiecan Cui, Yang Chen, Yue Zhou, Wei Pu, Xuanye Xu, Quanliang Chen, Xuelei Zhang, and Xin Wang
Atmos. Chem. Phys., 21, 6035–6051, https://doi.org/10.5194/acp-21-6035-2021, https://doi.org/10.5194/acp-21-6035-2021, 2021
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We assess the effect of dust external and internal mixing with snow grains on the absorption coefficient and albedo of snowpack. The results suggest that dust–snow internal mixing strongly enhances snow absorption coefficient and albedo reduction relative to external mixing. Meanwhile, the possible non-uniform distribution of dust in snow grains may lead to significantly different values of absorption coefficient and albedo of snowpack in the visible spectral range.
Sonya L. Fiddes, Matthew T. Woodhouse, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 21, 5883–5903, https://doi.org/10.5194/acp-21-5883-2021, https://doi.org/10.5194/acp-21-5883-2021, 2021
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Coral reefs are known to produce the aerosol precursor dimethyl sulfide (DMS). Currently, this source of coral DMS is unaccounted for in climate modelling, and the impact of coral reef extinction on aerosol and climate is unknown. In this study, we address this problem using a coupled chemistry–climate model for the first time. We find that coral reefs make a minimal contribution to the aerosol population and are unlikely to play a role in climate modulation.
Joonas Merikanto, Kalle Nordling, Petri Räisänen, Jouni Räisänen, Declan O'Donnell, Antti-Ilari Partanen, and Hannele Korhonen
Atmos. Chem. Phys., 21, 5865–5881, https://doi.org/10.5194/acp-21-5865-2021, https://doi.org/10.5194/acp-21-5865-2021, 2021
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Human-induced aerosols concentrate around their emission sources, yet their climate effects span far and wide. Here, we use two climate models to robustly identify the mechanisms of how Asian anthropogenic aerosols impact temperatures across the globe. A total removal of Asian anthropogenic aerosols increases the global temperatures by 0.26 ± 0.04 °C in the models, with the strongest warming taking place over the Arctic due to increased atmospheric transport of energy towards the high north.
Pontus von Schoenberg, Peter Tunved, Håkan Grahn, Alfred Wiedensohler, Radovan Krejci, and Niklas Brännström
Atmos. Chem. Phys., 21, 5173–5193, https://doi.org/10.5194/acp-21-5173-2021, https://doi.org/10.5194/acp-21-5173-2021, 2021
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In a radiological emergency preparedness system, Lagrangian particle dispersion models are often used to track the dispersion of radioactive material. In this study we have shown the importance of simulating advanced aerosol dynamic processes that are commonly neglected or simplified in these simulations. We show that inclusion of detailed ambient-aerosol dynamics can play a large role in the model result in simulations adopting a more detailed representation of aerosol–cloud interactions.
Zhiyuan Li, Kin-Fai Ho, Hsiao-Chi Chuang, and Steve Hung Lam Yim
Atmos. Chem. Phys., 21, 5063–5078, https://doi.org/10.5194/acp-21-5063-2021, https://doi.org/10.5194/acp-21-5063-2021, 2021
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This study established land-use regression (LUR) models using only routine air quality measurement data to support long-term health studies in an Asian metropolitan area. The established LUR models captured the spatial variability in exposure to air pollution with remarkable predictive accuracy. This is the first Asian study to evaluate intercity transferability of LUR models, and it highlights that there exist uncertainties when transferring LUR models between nearby cities.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Thomas Schwitalla, Hans-Stefan Bauer, Kirsten Warrach-Sagi, Thomas Bönisch, and Volker Wulfmeyer
Atmos. Chem. Phys., 21, 4575–4597, https://doi.org/10.5194/acp-21-4575-2021, https://doi.org/10.5194/acp-21-4575-2021, 2021
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A prototype of an air quality forecasting system (AQFS) on a turbulence-permitting (TP) horizontal resolution of 50 m is developed. AQFS is based on the WRF-Chem model and uses high-resolution emission data from different pollution sources. A simulation case study of a typical winter day in south Germany serves as a test bed. Results indicate that the complex topography plays an important role for the horizontal and vertical pollution distribution over the Stuttgart metropolitan area.
Tabish Umar Ansari, Oliver Wild, Edmund Ryan, Ying Chen, Jie Li, and Zifa Wang
Atmos. Chem. Phys., 21, 4471–4485, https://doi.org/10.5194/acp-21-4471-2021, https://doi.org/10.5194/acp-21-4471-2021, 2021
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We use novel modelling approaches to quantify the lingering effects of 1 d local and regional emission controls on subsequent days, the effects of longer continuous emission controls of individual sectors over different regions, and the effects of combined emission controls of multiple sectors and regions on air quality in Beijing under varying weather conditions to inform precise short-term emission control policies for avoiding heavy haze pollution in Beijing.
Ruud H. H. Janssen, Colette L. Heald, Allison L. Steiner, Anne E. Perring, J. Alex Huffman, Ellis S. Robinson, Cynthia H. Twohy, and Luke D. Ziemba
Atmos. Chem. Phys., 21, 4381–4401, https://doi.org/10.5194/acp-21-4381-2021, https://doi.org/10.5194/acp-21-4381-2021, 2021
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Bioaerosols are ubiquitous in the atmosphere and have the potential to affect cloud formation, as well as human and ecosystem health. However, their emissions are not well quantified, which hinders the assessment of their role in atmospheric processes. Here, we develop two new emission schemes for fungal spores based on multi-annual datasets of spore counts. We find that our modeled global emissions and burden are an order of magnitude lower than previous estimates.
Wenyuan Chang, Ying Zhang, Zhengqiang Li, Jie Chen, and Kaitao Li
Atmos. Chem. Phys., 21, 4403–4430, https://doi.org/10.5194/acp-21-4403-2021, https://doi.org/10.5194/acp-21-4403-2021, 2021
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Aerosol simulation in WRF-Chem often uses the MOSAIC aerosol mechanism. Still, we need variational data assimilation (DA) for the MOSAIC aerosols to blend aerosol optical measurements. This study provides a developed GSI variational DA system, with a tangent linear operator designed for multi-source and multi-wavelength aerosol optical measurements. We successfully applied the DA system in an aerosol field campaign to assimilate aerosol optical data in northwestern China.
Rong Tian, Xiaoyan Ma, and Jianqi Zhao
Atmos. Chem. Phys., 21, 4319–4337, https://doi.org/10.5194/acp-21-4319-2021, https://doi.org/10.5194/acp-21-4319-2021, 2021
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We improve the treatment of the dust emission process in GEOS-Chem by considering the effect of geographical variation of aerodynamic roughness length, smooth roughness length and soil texture, as well as the Owen effect and a more physically based formulation of sandblasting efficiency, which improve estimated threshold friction velocity and dust concentrations over China. Our study highlights the importance of incorporation of realistic land-surface properties into the dust emission scheme.
Longlei Li, Natalie M. Mahowald, Ron L. Miller, Carlos Pérez García-Pando, Martina Klose, Douglas S. Hamilton, Maria Gonçalves Ageitos, Paul Ginoux, Yves Balkanski, Robert O. Green, Olga Kalashnikova, Jasper F. Kok, Vincenzo Obiso, David Paynter, and David R. Thompson
Atmos. Chem. Phys., 21, 3973–4005, https://doi.org/10.5194/acp-21-3973-2021, https://doi.org/10.5194/acp-21-3973-2021, 2021
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For the first time, this study quantifies the range of the dust direct radiative effect due to uncertainty in the soil mineral abundance using all currently available information. We show that the majority of the estimated direct radiative effect range is due to uncertainty in the simulated mass fractions of iron oxides and thus their soil abundance, which is independent of the model employed. We therefore prove the necessity of considering mineralogy for understanding dust–climate interactions.
Naser G. A. Mahfouz and Neil M. Donahue
Atmos. Chem. Phys., 21, 3827–3832, https://doi.org/10.5194/acp-21-3827-2021, https://doi.org/10.5194/acp-21-3827-2021, 2021
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In this technical note, we show that the limit of the coagulation scavenging enhancement of charged particles is asymptotically 2; that is, at the limit, charged particles are lost at twice the rate of their neutral counterparts. This has serious implications for aerosol particle survivability where ions play a role in nucleation and growth. Such cases can happen readily in experiments and cannot be neglected in the atmosphere.
Dimitrios Bousiotis, James Brean, Francis D. Pope, Manuel Dall'Osto, Xavier Querol, Andrés Alastuey, Noemi Perez, Tuukka Petäjä, Andreas Massling, Jacob Klenø Nøjgaard, Claus Nordstrøm, Giorgos Kouvarakis, Stergios Vratolis, Konstantinos Eleftheriadis, Jarkko V. Niemi, Harri Portin, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys., 21, 3345–3370, https://doi.org/10.5194/acp-21-3345-2021, https://doi.org/10.5194/acp-21-3345-2021, 2021
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New particle formation events from 16 sites over Europe have been studied, and the influence of meteorological and atmospheric composition variables has been investigated. Some variables, like solar radiation intensity and temperature, have a positive effect on the occurrence of these events, while others have a negative effect, affecting different aspects such as the rate at which particles are formed or grow. This effect varies depending on the site type and magnitude of these variables.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
Sunling Gong, Hongli Liu, Bihui Zhang, Jianjun He, Hengde Zhang, Yaqiang Wang, Shuxiao Wang, Lei Zhang, and Jie Wang
Atmos. Chem. Phys., 21, 2999–3013, https://doi.org/10.5194/acp-21-2999-2021, https://doi.org/10.5194/acp-21-2999-2021, 2021
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Surface concentrations of PM2.5 in China have had a declining trend since 2013 across the country. This research found that the control measures of emission reduction are the dominant factors in the PM2.5 declining trends in various regions. The contribution by the meteorology to the surface PM2.5 concentrations from 2013 to 2019 was not found to show a consistent trend, fluctuating positively or negatively by about 5% on the annual average and 10–20% for the fall–winter heavy-pollution seasons.
Kamalika Sengupta, Kirsty Pringle, Jill S. Johnson, Carly Reddington, Jo Browse, Catherine E. Scott, and Ken Carslaw
Atmos. Chem. Phys., 21, 2693–2723, https://doi.org/10.5194/acp-21-2693-2021, https://doi.org/10.5194/acp-21-2693-2021, 2021
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Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which has significant climatic implications. We use a perturbed parameter model ensemble and ground-based observations to reduce the uncertainty in modelling SOA formation from oxidation of volatile organic compounds. We identify plausible parameter spaces for the yields of extremely low-volatility, low-volatility, and semi-volatile organic compounds based on model–observation match for three key model outputs.
Athanasios Tsikerdekis, Nick A. J. Schutgens, and Otto P. Hasekamp
Atmos. Chem. Phys., 21, 2637–2674, https://doi.org/10.5194/acp-21-2637-2021, https://doi.org/10.5194/acp-21-2637-2021, 2021
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Accurate representation of aerosols in the atmosphere is hard to achieve due to their complex microphysical and optical properties and uncertain emissions. In our work, we employ a data assimilation method which integrates model simulations with satellite observation related to the amount, size and the light absorption of aerosol. The use of these observations in an experiment improves aerosol representation and it is recommended for utilization in future data assimilation practices.
Nikolaos Evangeliou, Stephen M. Platt, Sabine Eckhardt, Cathrine Lund Myhre, Paolo Laj, Lucas Alados-Arboledas, John Backman, Benjamin T. Brem, Markus Fiebig, Harald Flentje, Angela Marinoni, Marco Pandolfi, Jesus Yus-Dìez, Natalia Prats, Jean P. Putaud, Karine Sellegri, Mar Sorribas, Konstantinos Eleftheriadis, Stergios Vratolis, Alfred Wiedensohler, and Andreas Stohl
Atmos. Chem. Phys., 21, 2675–2692, https://doi.org/10.5194/acp-21-2675-2021, https://doi.org/10.5194/acp-21-2675-2021, 2021
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Following the transmission of SARS-CoV-2 to Europe, social distancing rules were introduced to prevent further spread. We investigate the impacts of the European lockdowns on black carbon (BC) emissions by means of in situ observations and inverse modelling. BC emissions declined by 23 kt in Europe during the lockdowns as compared with previous years and by 11 % as compared to the period prior to lockdowns. Residential combustion prevailed in Eastern Europe, as confirmed by remote sensing data.
Xi Zhao, Xiaohong Liu, Susannah M. Burrows, and Yang Shi
Atmos. Chem. Phys., 21, 2305–2327, https://doi.org/10.5194/acp-21-2305-2021, https://doi.org/10.5194/acp-21-2305-2021, 2021
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Organic sea spray particles influence aerosol and cloud processes over the ocean. This study introduces the emission, cloud droplet activation, and ice nucleation (IN) of marine organic aerosol (MOA) into the Community Earth System Model. Our results indicate that MOA IN particles dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer. MOA enhances cloud forcing over the Southern Ocean in the austral winter and summer.
Jiarui Wu, Naifang Bei, Yuan Wang, Xia Li, Suixin Liu, Lang Liu, Ruonan Wang, Jiaoyang Yu, Tianhao Le, Min Zuo, Zhenxing Shen, Junji Cao, Xuexi Tie, and Guohui Li
Atmos. Chem. Phys., 21, 2229–2249, https://doi.org/10.5194/acp-21-2229-2021, https://doi.org/10.5194/acp-21-2229-2021, 2021
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A source-oriented version of the WRF-Chem model is developed to conduct source identification of wintertime PM2.5 in the North China Plain. Trans-boundary transport of air pollutants generally dominates the haze pollution in Beijing and Tianjin. The air quality in Hebei, Shandong, and Shanxi is generally controlled by local emissions. Primary aerosol species, such as EC and POA, are generally controlled by local emissions, while secondary aerosol shows evident regional characteristics.
Betty Croft, Randall V. Martin, Richard H. Moore, Luke D. Ziemba, Ewan C. Crosbie, Hongyu Liu, Lynn M. Russell, Georges Saliba, Armin Wisthaler, Markus Müller, Arne Schiller, Martí Galí, Rachel Y.-W. Chang, Erin E. McDuffie, Kelsey R. Bilsback, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 1889–1916, https://doi.org/10.5194/acp-21-1889-2021, https://doi.org/10.5194/acp-21-1889-2021, 2021
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North Atlantic Aerosols and Marine Ecosystems Study measurements combined with GEOS-Chem-TOMAS modeling suggest that several not-well-understood key factors control northwest Atlantic aerosol number and size. These synergetic and climate-relevant factors include particle formation near and above the marine boundary layer top, particle growth by marine secondary organic aerosol on descent, particle formation/growth related to dimethyl sulfide, sea spray aerosol, and ship emissions.
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
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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.
Zhicong Yin, Yijia Zhang, Huijun Wang, and Yuyan Li
Atmos. Chem. Phys., 21, 1581–1592, https://doi.org/10.5194/acp-21-1581-2021, https://doi.org/10.5194/acp-21-1581-2021, 2021
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It is a must to disentangle the contributions of stable meteorology from the effects of the COVID-19 lockdown. A 59 % decline in PM2.5 related to the COVID-19 pandemic was found in North China. The COVID-19 quarantine measures decreased the PM2.5 in the Yangtze River Delta by 72 %. In Hubei Province where most pneumonia cases were confirmed, the impact of the total emission reduction (72 %) evidently exceeded the rising percentage of PM2.5 driven by meteorology (13 %).
Nadya Moisseeva and Roland Stull
Atmos. Chem. Phys., 21, 1407–1425, https://doi.org/10.5194/acp-21-1407-2021, https://doi.org/10.5194/acp-21-1407-2021, 2021
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Wildfire smoke-plume rise, which determines the emissions injection height, is widely recognized as an area of uncertainty within regional and global chemical transport models. In this work we propose a simple energy balance parameterization to predict the mean smoke equilibrium height for fires of arbitrary shape and intensity.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Jasper F. Kok, Adeyemi A. Adebiyi, Samuel Albani, Yves Balkanski, Ramiro Checa-Garcia, Mian Chin, Peter R. Colarco, Douglas S. Hamilton, Yue Huang, Akinori Ito, Martina Klose, Longlei Li, Natalie M. Mahowald, Ron L. Miller, Vincenzo Obiso, Carlos Pérez García-Pando, Adriana Rocha-Lima, and Jessica S. Wan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-4, https://doi.org/10.5194/acp-2021-4, 2021
Revised manuscript accepted for ACP
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The many impacts of dust on the Earth system depend on dust mineralogy, which varies between dust source regions. We constrain the contribution of the world's main dust source regions by integrating dust observations with global model simulations. We find that Asian dust contributes more, and that North African dust contributes less, than models account for. We obtain a data set of each source region's contribution to the dust cycle that can be used to constrain dust impacts on the Earth system.
Lena Frey, Frida A.-M. Bender, and Gunilla Svensson
Atmos. Chem. Phys., 21, 577–595, https://doi.org/10.5194/acp-21-577-2021, https://doi.org/10.5194/acp-21-577-2021, 2021
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We investigate the vertical distribution of aerosol in the climate model NorESM1-M in five regions of marine stratocumulus clouds. We thereby analyze the total aerosol extinction to facilitate a comparison with satellite data. We find that the model underestimates aerosol extinction throughout the troposphere, especially elevated aerosol layers. Further, we perform sensitivity experiments to identify the processes most important for vertical aerosol distribution in our model.
José María López-Romero, Juan Pedro Montávez, Sonia Jerez, Raquel Lorente-Plazas, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 21, 415–430, https://doi.org/10.5194/acp-21-415-2021, https://doi.org/10.5194/acp-21-415-2021, 2021
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The effect of aerosols on regional climate simulations presents large uncertainties due to their complex and non-linear interactions with a wide variety of factors, including aerosol–radiation and aerosol–cloud interactions. We show how these interactions are strongly conditioned by the meteorological situation and the type of aerosol. While natural aerosols tend to increase precipitation in some areas, anthropogenic aerosols decrease the number of rainy days in some pollutant regions.
Jonas Gliß, Augustin Mortier, Michael Schulz, Elisabeth Andrews, Yves Balkanski, Susanne E. Bauer, Anna M. K. Benedictow, Huisheng Bian, Ramiro Checa-Garcia, Mian Chin, Paul Ginoux, Jan J. Griesfeller, Andreas Heckel, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Paolo Laj, Philippe Le Sager, Marianne Tronstad Lund, Cathrine Lund Myhre, Hitoshi Matsui, Gunnar Myhre, David Neubauer, Twan van Noije, Peter North, Dirk J. L. Olivié, Samuel Rémy, Larisa Sogacheva, Toshihiko Takemura, Kostas Tsigaridis, and Svetlana G. Tsyro
Atmos. Chem. Phys., 21, 87–128, https://doi.org/10.5194/acp-21-87-2021, https://doi.org/10.5194/acp-21-87-2021, 2021
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Simulated aerosol optical properties as well as the aerosol life cycle are investigated for 14 global models participating in the AeroCom initiative. Considerable diversity is found in the simulated aerosol species emissions and lifetimes, also resulting in a large diversity in the simulated aerosol mass, composition, and optical properties. A comparison with observations suggests that, on average, current models underestimate the direct effect of aerosol on the atmosphere radiation budget.
Yang Li, Loretta J. Mickley, and Jed O. Kaplan
Atmos. Chem. Phys., 21, 57–68, https://doi.org/10.5194/acp-21-57-2021, https://doi.org/10.5194/acp-21-57-2021, 2021
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Climate models predict a shift toward warmer, drier environments in southwestern North America. Under future climate, the two main drivers of dust trends play opposing roles: (1) CO2 fertilization enhances vegetation and, in turn, decreases dust, and (2) increasing land use enhances dust emissions from northern Mexico. In the worst-case scenario, elevated dust concentrations spread widely over the domain by 2100 in spring, suggesting a large climate penalty on air quality and human health.
Peng Xian, Philip J. Klotzbach, Jason P. Dunion, Matthew A. Janiga, Jeffrey S. Reid, Peter R. Colarco, and Zak Kipling
Atmos. Chem. Phys., 20, 15357–15378, https://doi.org/10.5194/acp-20-15357-2020, https://doi.org/10.5194/acp-20-15357-2020, 2020
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Using dust AOD (DAOD) data from three aerosol reanalyses, we explored the correlative relationships between DAOD and multiple indices representing seasonal Atlantic TC activities. A robust negative correlation with Caribbean DAOD and Atlantic TC activity was found. We documented for the first time the regional differences of this relationship for over the Caribbean and the tropical North Atlantic. We also evaluated the impacts of potential confounding climate factors in this relationship.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Jianbing Jin, Arjo Segers, Hong Liao, Arnold Heemink, Richard Kranenburg, and Hai Xiang Lin
Atmos. Chem. Phys., 20, 15207–15225, https://doi.org/10.5194/acp-20-15207-2020, https://doi.org/10.5194/acp-20-15207-2020, 2020
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Data assimilation provides a powerful tool to estimate emission inventories by feeding observations. This emission inversion relies on the correct assumption about the emission uncertainty, which describes the potential spatiotemporal spreads of sources. However, an unrepresentative uncertainty is unavoidable. Especially in the complex dust emission, the uncertainties can hardly all be taken into account. This study reports how adjoint can be used to detect errors in the emission uncertainty.
Ifeanyichukwu C. Nduka, Steve Hung Lam Yim, Chi-Yung Tam, and Jianping Guo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1068, https://doi.org/10.5194/acp-2020-1068, 2020
Revised manuscript accepted for ACP
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This study analyzed the nature, mechanisms and drivers for Hot-and-Polluted episodes (HPEs) in the Pearl River Delta, China. A total of eight HPEs were identified and can be grouped into three clusters of HPEs that were respectively driven (1) by weak subsidence and convection induced by approaching tropical cyclones, (2) by calm conditions with low wind speed at the lower atmosphere, and (3) by the combination of both aforementioned conditions.
Ming-Tung Chuang, Maggie Chel Gee Ooi, Neng-Huei Lin, Joshua S. Fu, Chung-Te Lee, Sheng-Hsiang Wang, Ming-Cheng Yen, Steven Soon-Kai Kong, and Wei-Syun Huang
Atmos. Chem. Phys., 20, 14947–14967, https://doi.org/10.5194/acp-20-14947-2020, https://doi.org/10.5194/acp-20-14947-2020, 2020
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This study evaluated the impact of Asian haze from the three biggest industrial regions on Taiwan and analyzed the process during transport. The production and removal process revealed the mechanisms of long-range transport. This is the first time that the brute force method and process analysis technique has been applied in a Community Multiscale Air Quality Modeling System. Also, this study simulated the interesting transboundary transport of pollutants from southern mainland China to Taiwan.
Lukas O. Muser, Gholam Ali Hoshyaripour, Julia Bruckert, Ákos Horváth, Elizaveta Malinina, Sandra Wallis, Fred J. Prata, Alexei Rozanov, Christian von Savigny, Heike Vogel, and Bernhard Vogel
Atmos. Chem. Phys., 20, 15015–15036, https://doi.org/10.5194/acp-20-15015-2020, https://doi.org/10.5194/acp-20-15015-2020, 2020
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Volcanic aerosols endanger aircraft and thus disrupt air travel globally. For aviation safety, it is vital to know the location and lifetime of such aerosols in the atmosphere. Here we show that the interaction of volcanic particles with each other eventually reduces their atmospheric lifetime. Moreover, we demonstrate that sunlight heats these particles, which lifts them several kilometers in the atmosphere. These findings support a more reliable forecast of volcanic aerosol dispersion.
Shuyu Zhao, Tian Feng, Xuexi Tie, and Zebin Wang
Atmos. Chem. Phys., 20, 14873–14887, https://doi.org/10.5194/acp-20-14873-2020, https://doi.org/10.5194/acp-20-14873-2020, 2020
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The Tibetan Plateau has been experiencing a rapid warming during the last 40 years, particularly in winter. The warming leads to an increase in the planetary boundary layer height and a decrease in the relative humidity in the Sichuan Basin, causing a reduction of PM2.5 concentration by 17.5 % (~25.1 μg m−3), of which the reduction in secondary aerosols is 19.7 μg m−3. These findings indicate that the warming plateau plays an important role in mitigating air quality in downstream.
Jonathan K. P. Shonk, Andrew G. Turner, Amulya Chevuturi, Laura J. Wilcox, Andrea J. Dittus, and Ed Hawkins
Atmos. Chem. Phys., 20, 14903–14915, https://doi.org/10.5194/acp-20-14903-2020, https://doi.org/10.5194/acp-20-14903-2020, 2020
Short summary
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We use a set of model simulations of the 20th century to demonstrate that the uncertainty in the cooling effect of man-made aerosol emissions has a wide range of impacts on global monsoons. For the weakest cooling, the impact of aerosol is overpowered by greenhouse gas (GHG) warming and monsoon rainfall increases in the late 20th century. For the strongest cooling, aerosol impact dominates over GHG warming, leading to reduced monsoon rainfall, particularly from 1950 to 1980.
Huan Zhang and You-He Zhou
Atmos. Chem. Phys., 20, 14801–14820, https://doi.org/10.5194/acp-20-14801-2020, https://doi.org/10.5194/acp-20-14801-2020, 2020
Short summary
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We assess the effects of triboelectric charging on wind-blown sand via observations and a numerical model. The 3D electric field within a few centimetres of the ground is characterized for the first time. By using the discrete element method together with the particle-charging model, we explicitly account for the particle–particle charging during collisions. We find that triboelectric charging could enhance the total mass flux and saltation height by up to 20 % and 15 %, respectively.
Brigitte Rooney, Yuan Wang, Jonathan H. Jiang, Bin Zhao, Zhao-Cheng Zeng, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14597–14616, https://doi.org/10.5194/acp-20-14597-2020, https://doi.org/10.5194/acp-20-14597-2020, 2020
Short summary
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Wildfires have become increasingly prevalent. Intense smoke consisting of particulate matter (PM) leads to an increased risk of morbidity and mortality. The record-breaking Camp Fire ravaged Northern California for two weeks in 2018. Here, we employ a comprehensive chemical transport model along with ground-based and satellite observations to characterize the PM concentrations across Northern California and to investigate the pollution sensitivity predictions to key parameters of the model.
Vijayakumar Sivadasan Nair, Filippo Giorgi, and Usha Keshav Hasyagar
Atmos. Chem. Phys., 20, 14457–14471, https://doi.org/10.5194/acp-20-14457-2020, https://doi.org/10.5194/acp-20-14457-2020, 2020
Short summary
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Air pollution and wintertime fog over South Asia is a major concern due to its significant implications on air quality, visibility and health. Coupled model simulations show that hygroscopic growth of aerosols contributes significantly to the aerosol-induced cooling at the surface. Our analysis demonstrates that the aerosol–moisture interaction is the most significant contributor favouring and strengthening the high-aerosol conditions (poor air quality) prevailing over South Asia during winter.
Harshavardhana Sunil Pathak, Sreedharan Krishnakumari Satheesh, Krishnaswamy Krishna Moorthy, and Ravi Shankar Nanjundiah
Atmos. Chem. Phys., 20, 14237–14252, https://doi.org/10.5194/acp-20-14237-2020, https://doi.org/10.5194/acp-20-14237-2020, 2020
Short summary
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We have estimated the aerosol radiative forcing (ARF) by employing the assimilated, gridded aerosol datasets over the Indian region. The present ARF estimates are more accurate and certain than those estimated using the currently available, latest satellite-retrieved aerosol products. Therefore, the present ARF estimates and corresponding assimilated aerosol products emerge as potential candidates for improving the aerosol climate impact assessment at regional, subregional and seasonal scales.
Jasper F. Kok, Adeyemi A. Adebiyi, Samuel Albani, Yves Balkanski, Ramiro Checa-Garcia, Mian Chin, Peter R. Colarco, Douglas Stephen Hamilton, Yue Huang, Akinori Ito, Martina Klose, Danny M. Leung, Longlei Li, Natalie M. Mahowald, Ron L. Miller, Vincenzo Obiso, Carlos Pérez García-Pando, Adriana Rocha-Lima, Jessica S. Wan, and Chloe A. Whicker
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1131, https://doi.org/10.5194/acp-2020-1131, 2020
Revised manuscript accepted for ACP
Short summary
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Desert dust interacts with virtually every component of the Earth system, including the climate system. We develop a new methodology to represent the global dust cycle that integrates observational constraints on the properties and abundance of desert dust with global atmospheric model simulations. We show that the resulting representation of the global dust cycle is more accurate than can be obtained from a large number of current climate global atmospheric models.
Asta Gregorič, Luka Drinovec, Irena Ježek, Janja Vaupotič, Matevž Lenarčič, Domen Grauf, Longlong Wang, Maruška Mole, Samo Stanič, and Griša Močnik
Atmos. Chem. Phys., 20, 14139–14162, https://doi.org/10.5194/acp-20-14139-2020, https://doi.org/10.5194/acp-20-14139-2020, 2020
Short summary
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We present a new method for the determination of highly time-resolved and source-separated black carbon emission rates. The atmospheric dynamics is quantified using the atmospheric radon concentration. Different intensity and daily dynamics of black carbon emission rates for two different environments are presented: urban and rural area. The method can be used to assess the efficiency of pollution mitigation measures, thereby avoiding the influence of variable meteorology.
Mingxuan Wu, Xiaohong Liu, Hongbin Yu, Hailong Wang, Yang Shi, Kang Yang, Anton Darmenov, Chenglai Wu, Zhien Wang, Tao Luo, Yan Feng, and Ziming Ke
Atmos. Chem. Phys., 20, 13835–13855, https://doi.org/10.5194/acp-20-13835-2020, https://doi.org/10.5194/acp-20-13835-2020, 2020
Short summary
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The spatiotemporal distributions of dust aerosol simulated by global climate models (GCMs) are highly uncertain. In this study, we evaluate dust extinction profiles, optical depth, and surface concentrations simulated in three GCMs and one reanalysis against multiple satellite retrievals and surface observations to gain process-level understanding. Our results highlight the importance of correctly representing dust emission, dry/wet deposition, and size distribution in GCMs.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
Short summary
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
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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...
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