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ACP | 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.
https://doi.org/10.5194/acp-19-5959-2019
© Author(s) 2019. This work is distributed under
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.
https://doi.org/10.5194/acp-19-5959-2019
© Author(s) 2019. This work is distributed under
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. Discuss., https://doi.org/10.5194/acp-2020-1105, https://doi.org/10.5194/acp-2020-1105, 2020
Preprint under review for ACP
Short summary
Short summary
Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in North China Plain (NCP) in summer and winter were investigated. Our results showed that organic aerosol (OA) in winter in 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 solid in winter in Beijing, but as semi-solids in Beijing in summer and Gucheng in winter.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus Petters
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-768, https://doi.org/10.5194/acp-2020-768, 2020
Revised manuscript accepted for ACP
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 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
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
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. Discuss., https://doi.org/10.5194/acp-2020-1105, https://doi.org/10.5194/acp-2020-1105, 2020
Preprint under review for ACP
Short summary
Short summary
Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in North China Plain (NCP) in summer and winter were investigated. Our results showed that organic aerosol (OA) in winter in 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 solid in winter in Beijing, but as semi-solids in Beijing in summer and Gucheng in winter.
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
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 (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.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1000, https://doi.org/10.5194/acp-2020-1000, 2020
Preprint under review for ACP
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 and either adsorption or desorption can be the controlling process. 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.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus Petters
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-768, https://doi.org/10.5194/acp-2020-768, 2020
Revised manuscript accepted for ACP
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 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.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-536, https://doi.org/10.5194/acp-2020-536, 2020
Revised manuscript accepted for ACP
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.
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
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
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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
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
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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
Short summary
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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)
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
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
Assessment of regional aerosol radiative effects under the SWAAMI campaign – Part 2: Clear-sky direct shortwave radiative forcing using multi-year assimilated data over the Indian subcontinent
The determination of highly time-resolved and source-separated black carbon emission rates using radon as a tracer of atmospheric dynamics
Understanding processes that control dust spatial distributions with global climate models and satellite observations
Heterogeneous nucleation of water vapor on different types of black carbon particles
Impacts of atmospheric transport and biomass burning on the inter-annual variation in black carbon aerosols over the Tibetan Plateau
A complex aerosol transport event over Europe during the 2017 Storm Ophelia in CAMS forecast systems: analysis and evaluation
Sensitivity analysis of the surface ozone and fine particulate matter to meteorological parameters in China
How aerosols and greenhouse gases influence the diurnal temperature range
Evaluation of climate model aerosol trends with ground-based observations over the last 2 decades – an AeroCom and CMIP6 analysis
Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions
Direct and semi-direct radiative forcing of biomass-burning aerosols over the southeast Atlantic (SEA) and its sensitivity to absorbing properties: a regional climate modeling study
Technical note: Estimating aqueous solubilities and activity coefficients of mono- and α,ω-dicarboxylic acids using COSMOtherm
Models transport Saharan dust too low in the atmosphere: a comparison of the MetUM and CAMS forecasts with observations
Dependency of particle size distribution at dust emission on friction velocity and atmospheric boundary-layer stability
Using machine learning to derive cloud condensation nuclei number concentrations from commonly available measurements
Impacts of aerosol–radiation interaction on meteorological forecasts over northern China by offline coupling of the WRF-Chem-simulated aerosol optical depth into WRF: a case study during a heavy pollution event
Accelerated increases in global and Asian summer monsoon precipitation from future aerosol reductions
Distinct responses of Asian summer monsoon to black carbon aerosols and greenhouse gases
Modulation of springtime surface sensible heating over the Tibetan Plateau on the interannual variability of East Asian dust cycle
Examining the atmospheric radiative and snow-darkening effects of black carbon and dust across the Rocky Mountains of the United States using WRF-Chem
Model Inter-Comparison Study for Asia (MICS-Asia) phase III: multimodel comparison of reactive nitrogen deposition over China
The global dust cycle and uncertainty in CMIP5 (Coupled Model Intercomparison Project phase 5) models
A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity
Effects of Marine Organic Aerosols as Sources of Immersion-Mode Ice Nucleating Particles on High Latitude Mixed-Phase Clouds
Evident PM2.5 Drops in the East of China due to the COVID-19 Quarantines in February
The value of remote marine aerosol measurements for constraining radiative forcing uncertainty
Aerosol concentrations variability over China: two distinct leading modes
Wildfire smoke-plume rise: a simple energy balance parameterization
The interaction between urbanization and aerosols during a typical winter haze event in Beijing
The absorption Ångstrom exponent of black carbon with brown coatings: effects of aerosol microphysics and parameterization
Quantifying the sensitivity of aerosol optical properties to the parameterizations of physico-chemical processes during the 2010 Russian wildfires and heatwave
Robust observational constraint of uncertain aerosol processes and emissions in a climate model and the effect on aerosol radiative forcing
A global model perturbed parameter ensemble study of secondary organic aerosol formation
Factors controlling marine aerosol size distributions and their climate effects over the Northwest Atlantic Ocean region
Source attribution of Arctic black carbon and sulfate aerosols and associated Arctic surface warming during 1980–2018
Large difference in aerosol radiative effects from BVOC-SOA treatment in three Earth system models
Cloudy-sky contributions to the direct aerosol effect
Estimation of cloud condensation nuclei number concentrations and comparison to in situ and lidar observations during the HOPE experiments
Aerosol radiative effects and feedbacks on boundary layer meteorology and PM2.5 chemical components during winter haze events over the Beijing-Tianjin-Hebei region
Modulation of radiative aerosols effects by atmospheric circulation over the Euro-Mediterranean region
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.
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
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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
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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
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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
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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
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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.
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
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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
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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
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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.
Han Han, Yue Wu, Jane Liu, Tianliang Zhao, Bingliang Zhuang, Honglei Wang, Yichen Li, Huimin Chen, Ye Zhu, Hongnian Liu, Qin'geng Wang, Shu Li, Tijian Wang, Min Xie, and Mengmeng Li
Atmos. Chem. Phys., 20, 13591–13610, https://doi.org/10.5194/acp-20-13591-2020, https://doi.org/10.5194/acp-20-13591-2020, 2020
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Combining simulations from a global chemical transport model and a trajectory model, we find that black carbon aerosols from South Asia and East Asia contribute 77 % of the surface black carbon in the Tibetan Plateau. The Asian monsoon largely modulates inter-annual transport of black carbon from non-local regions to the Tibetan Plateau surface in most seasons, while inter-annual fire activities in South Asia influence black carbon concentration over the Tibetan Plateau surface mainly in spring.
Dimitris Akritidis, Eleni Katragkou, Aristeidis K. Georgoulias, Prodromos Zanis, Stergios Kartsios, Johannes Flemming, Antje Inness, John Douros, and Henk Eskes
Atmos. Chem. Phys., 20, 13557–13578, https://doi.org/10.5194/acp-20-13557-2020, https://doi.org/10.5194/acp-20-13557-2020, 2020
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We assess the Copernicus Atmosphere Monitoring Service (CAMS) global and regional forecasts performance during a complex aerosol transport event over Europe induced by the passage of Storm Ophelia in mid-October 2017. Comparison with satellite observations reveals a satisfactory performance of CAMS global forecast assisted by data assimilation, while comparison with ground-based measurements indicates that the CAMS regional system over-performs compared to the global one in terms of air quality.
Zhihao Shi, Lin Huang, Jingyi Li, Qi Ying, Hongliang Zhang, and Jianlin Hu
Atmos. Chem. Phys., 20, 13455–13466, https://doi.org/10.5194/acp-20-13455-2020, https://doi.org/10.5194/acp-20-13455-2020, 2020
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Meteorological conditions play important roles in the formation of O3 and PM2.5 pollution in China. O3 is most sensitive to temperature and the sensitivity is dependent on the O3 chemistry formation or loss regime. PM2.5 is negatively sensitive to temperature, wind speed, and planetary boundary layer height and positively sensitive to humidity. The results imply that air quality in certain regions of China is sensitive to climate changes.
Camilla W. Stjern, Bjørn H. Samset, Olivier Boucher, Trond Iversen, Jean-François Lamarque, Gunnar Myhre, Drew Shindell, and Toshihiko Takemura
Atmos. Chem. Phys., 20, 13467–13480, https://doi.org/10.5194/acp-20-13467-2020, https://doi.org/10.5194/acp-20-13467-2020, 2020
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The span between the warmest and coldest temperatures over a day is a climate parameter that influences both agriculture and human health. Using data from 10 models, we show how individual climate drivers such as greenhouse gases and aerosols produce distinctly different responses in this parameter in high-emission regions. Given the high uncertainty in future aerosol emissions, this improved understanding of the temperature responses may ultimately help these regions prepare for future changes.
Augustin Mortier, Jonas Gliß, Michael Schulz, Wenche Aas, Elisabeth Andrews, Huisheng Bian, Mian Chin, Paul Ginoux, Jenny Hand, Brent Holben, Hua Zhang, Zak Kipling, Alf Kirkevåg, Paolo Laj, Thibault Lurton, Gunnar Myhre, David Neubauer, Dirk Olivié, Knut von Salzen, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 20, 13355–13378, https://doi.org/10.5194/acp-20-13355-2020, https://doi.org/10.5194/acp-20-13355-2020, 2020
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We present a multiparameter analysis of the aerosol trends over the last 2 decades in the different regions of the world. In most of the regions, ground-based observations show a decrease in aerosol content in both the total atmospheric column and at the surface. The use of climate models, assessed against these observations, reveals however an increase in the total aerosol load, which is not seen with the sole use of observation due to partial coverage in space and time.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
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This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Marc Mallet, Fabien Solmon, Pierre Nabat, Nellie Elguindi, Fabien Waquet, Dominique Bouniol, Andrew Mark Sayer, Kerry Meyer, Romain Roehrig, Martine Michou, Paquita Zuidema, Cyrille Flamant, Jens Redemann, and Paola Formenti
Atmos. Chem. Phys., 20, 13191–13216, https://doi.org/10.5194/acp-20-13191-2020, https://doi.org/10.5194/acp-20-13191-2020, 2020
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This paper presents numerical simulations using two regional climate models to study the impact of biomass fire plumes from central Africa on the radiative balance of this region. The results indicate that biomass fires can either warm the regional climate when they are located above low clouds or cool it when they are located above land. They can also alter sea and land surface temperatures by decreasing solar radiation at the surface. Finally, they can also modify the atmospheric dynamics.
Noora Hyttinen, Reyhaneh Heshmatnezhad, Jonas Elm, Theo Kurtén, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 13131–13143, https://doi.org/10.5194/acp-20-13131-2020, https://doi.org/10.5194/acp-20-13131-2020, 2020
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We present aqueous solubilities and activity coefficients of mono- and dicarboxylic acids (C1–C6 and C2–C8, respectively) estimated using the COSMOtherm program. In addition, we have calculated effective equilibrium constants of dimerization and hydration of the same acids in the condensed phase. We were also able to improve the agreement between experimental and estimated properties of monocarboxylic acids in aqueous solutions by including clustering reactions in COSMOtherm calculations.
Debbie O'Sullivan, Franco Marenco, Claire L. Ryder, Yaswant Pradhan, Zak Kipling, Ben Johnson, Angela Benedetti, Melissa Brooks, Matthew McGill, John Yorks, and Patrick Selmer
Atmos. Chem. Phys., 20, 12955–12982, https://doi.org/10.5194/acp-20-12955-2020, https://doi.org/10.5194/acp-20-12955-2020, 2020
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Mineral dust is an important component of the climate system, and we assess how well it is predicted by two operational models. We flew an aircraft in the dust layers in the eastern Atlantic, and we also make use of satellites. We show that models predict the dust layer too low and that it predicts the particles to be too small. We believe that these discrepancies may be overcome if models can be constrained with operational observations of dust vertical and size-resolved distribution.
Yaping Shao, Jie Zhang, Masahide Ishizuka, Masao Mikami, John Leys, and Ning Huang
Atmos. Chem. Phys., 20, 12939–12953, https://doi.org/10.5194/acp-20-12939-2020, https://doi.org/10.5194/acp-20-12939-2020, 2020
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It has been recognized in earlier research that particle size distribution of dust at emission (dust PSD) is dependent on friction velocity. This recognition has been challenged in some recent papers. Based on the analysis of experimental data, we confirm that dust PSD is dependent on friction velocity and atmospheric boundary-layer stability. By theoretical and numerical analysis, we reveal the reasons for this dependency.
Arshad Arjunan Nair and Fangqun Yu
Atmos. Chem. Phys., 20, 12853–12869, https://doi.org/10.5194/acp-20-12853-2020, https://doi.org/10.5194/acp-20-12853-2020, 2020
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Small particles in the atmosphere can affect cloud formation and properties and thus Earth's energy budget. These cloud condensation nuclei (CCN) contribute the largest uncertainties in climate change modeling. To reduce these uncertainties, it is important to quantify CCN numbers accurately, measurements of which are sparse. We propose and evaluate a machine learning method to estimate CCN, in the absence of their direct measurements, using more common measurements of weather and air quality.
Yang Yang, Min Chen, Xiujuan Zhao, Dan Chen, Shuiyong Fan, Jianping Guo, and Shaukat Ali
Atmos. Chem. Phys., 20, 12527–12547, https://doi.org/10.5194/acp-20-12527-2020, https://doi.org/10.5194/acp-20-12527-2020, 2020
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This study analyzed the impacts of aerosol–radiation interaction on radiation and meteorological forecasts using the offline coupling of WRF and high-frequency updated AOD simulated by WRF-Chem. The results revealed that aerosol–radiation interaction had a positive influence on the improvement of predictive accuracy, including 2 m temperature (~ 73.9 %) and horizontal wind speed (~ 7.8 %), showing potential prospects for its application in regional numerical weather prediction in northern China.
Laura J. Wilcox, Zhen Liu, Bjørn H. Samset, Ed Hawkins, Marianne T. Lund, Kalle Nordling, Sabine Undorf, Massimo Bollasina, Annica M. L. Ekman, Srinath Krishnan, Joonas Merikanto, and Andrew G. Turner
Atmos. Chem. Phys., 20, 11955–11977, https://doi.org/10.5194/acp-20-11955-2020, https://doi.org/10.5194/acp-20-11955-2020, 2020
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Projected changes in man-made aerosol range from large reductions to moderate increases in emissions until 2050. Rapid reductions between the present and the 2050s lead to enhanced increases in global and Asian summer monsoon precipitation relative to scenarios with continued increases in aerosol. Relative magnitude and spatial distribution of aerosol changes are particularly important for South Asian summer monsoon precipitation changes, affecting the sign of the trend in the coming decades.
Xiaoning Xie, Gunnar Myhre, Xiaodong Liu, Xinzhou Li, Zhengguo Shi, Hongli Wang, Alf Kirkevåg, Jean-Francois Lamarque, Drew Shindell, Toshihiko Takemura, and Yangang Liu
Atmos. Chem. Phys., 20, 11823–11839, https://doi.org/10.5194/acp-20-11823-2020, https://doi.org/10.5194/acp-20-11823-2020, 2020
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Black carbon (BC) and greenhouse gases (GHGs) enhance precipitation minus evaporation (P–E) of Asian summer monsoon (ASM). Further analysis reveals distinct mechanisms controlling BC- and GHG-induced ASM P–E increases. The change in ASM P–E by BC is dominated by the dynamic effect of enhanced large-scale monsoon circulation, the GHG-induced change by the thermodynamic effect of increasing atmospheric water vapor. This results from different atmospheric temperature feedbacks due to BC and GHGs.
Xiaoning Xie, Anmin Duan, Zhengguo Shi, Xinzhou Li, Hui Sun, Xiaodong Liu, Xugeng Cheng, Tianliang Zhao, Huizheng Che, and Yangang Liu
Atmos. Chem. Phys., 20, 11143–11159, https://doi.org/10.5194/acp-20-11143-2020, https://doi.org/10.5194/acp-20-11143-2020, 2020
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Observational and modeling results both show that the surface dust concentrations over the East Asian (EA) dust source region and over the northwestern Pacific (NP) in MAM are significantly positively correlated with TPSH. These atmospheric circulation anomalies induced by the increased TPSH result in increasing westerly winds over both EA and NP, which in turn increases dust emissions over the dust source and dust transport over these two regions, as well as the regional dust cycles.
Stefan Rahimi, Xiaohong Liu, Chun Zhao, Zheng Lu, and Zachary J. Lebo
Atmos. Chem. Phys., 20, 10911–10935, https://doi.org/10.5194/acp-20-10911-2020, https://doi.org/10.5194/acp-20-10911-2020, 2020
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Dark particles emitted to the atmosphere can absorb sunlight and heat the air. As these particles settle, they may darken the surface, especially over snow-covered regions like the Rocky Mountains. This darkening of the surface may lead to changes in snowpack, affecting the local meteorology and hydrology. We seek to evaluate whether these light-absorbing particles more prominently affect this region through their atmospheric presence or their on-snow presence.
Baozhu Ge, Syuichi Itahashi, Keiichi Sato, Danhui Xu, Junhua Wang, Fan Fan, Qixin Tan, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Hong Liao, Meigen Zhang, Zhe Wang, Meng Li, Jung-Hun Woo, Junichi Kurokawa, Yuepeng Pan, Qizhong Wu, Xuejun Liu, and Zifa Wang
Atmos. Chem. Phys., 20, 10587–10610, https://doi.org/10.5194/acp-20-10587-2020, https://doi.org/10.5194/acp-20-10587-2020, 2020
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Performances of the simulated deposition for different reduced N (Nr) species in China were conducted with the Model Inter-Comparison Study for Asia. Results showed that simulated wet deposition of oxidized N was overestimated in northeastern China and underestimated in south China, but Nr was underpredicted in all regions by all models. Oxidized N has larger uncertainties than Nr, indicating that the chemical reaction process is one of the most importance factors affecting model performance.
Chenglai Wu, Zhaohui Lin, and Xiaohong Liu
Atmos. Chem. Phys., 20, 10401–10425, https://doi.org/10.5194/acp-20-10401-2020, https://doi.org/10.5194/acp-20-10401-2020, 2020
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This study provides a comprehensive evaluation of the global dust cycle in 15 models participating in the fifth phase of the Coupled Model Intercomparison Project (CMIP5). We assess the global budget and associated uncertainties. We also quantify the discrepancies in each model. The results highlight the large uncertainties in both the locations and intensities of dust emission. Our study will serve as a useful reference for model communities and help further model improvements.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Xi Zhao, Xiaohong Liu, Susannah Burrows, and Yang Shi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-674, https://doi.org/10.5194/acp-2020-674, 2020
Revised manuscript accepted for ACP
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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 of marine organic aerosol (MOA) into the Community Earth System Model. Our results indicate that MOA INPs dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer. MOA enhances the longwave/shortwave cloud forcing by 0.35/−2.78 W m–2 over the Southern Ocean in the austral winter/summer.
Zhicong Yin, Yijia Zhang, Huijun Wang, and Yuyan Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-695, https://doi.org/10.5194/acp-2020-695, 2020
Revised manuscript accepted for ACP
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The PM2.5 drops were decomposed into the impacts of routine emission reductions, meteorology and COVID-19 quarantines. Meteorological conditions caused a 30 % and 14 % increase of PM2.5 in North China and Hubei Province. PM2.5 dropped by 30–60 μg/m3 in North China and 0–30 μg/m3 in the south due to the COVID-19 quarantines.
Leighton A. Regayre, Julia Schmale, Jill S. Johnson, Christian Tatzelt, Andrea Baccarini, Silvia Henning, Masaru Yoshioka, Frank Stratmann, Martin Gysel-Beer, Daniel P. Grosvenor, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10063–10072, https://doi.org/10.5194/acp-20-10063-2020, https://doi.org/10.5194/acp-20-10063-2020, 2020
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The amount of energy reflected back into space because of man-made particles is highly uncertain. Processes related to naturally occurring particles cause most of the uncertainty, but these processes are poorly constrained by present-day measurements. We show that measurements over the Southern Ocean, far from pollution sources, efficiently reduce climate model uncertainties. Our results pave the way to designing experiments and measurement campaigns that reduce this uncertainty even further.
Juan Feng, Jianlei Zhu, Jianping Li, and Hong Liao
Atmos. Chem. Phys., 20, 9883–9893, https://doi.org/10.5194/acp-20-9883-2020, https://doi.org/10.5194/acp-20-9883-2020, 2020
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This paper explores the month-to-month variability of aerosol concentrations (ACs) over China. The AC variability is dominated by the monopole mode and the meridional dipole mode. The associated dynamic and thermal impacts of the climate systems are examined to explain their contributions to the formation of the two modes. The result suggests the variations are originating from the tropical Pacific, and extratropical atmospheric systems contribute to the dominant variabilities of ACs over China.
Nadya Moisseeva and Roland Stull
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-827, https://doi.org/10.5194/acp-2020-827, 2020
Revised manuscript accepted for ACP
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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.
Miao Yu, Guiqian Tang, Yang Yang, Qingchun Li, Yonghong Wang, Shiguang Miao, Yizhou Zhang, and Yuesi Wang
Atmos. Chem. Phys., 20, 9855–9870, https://doi.org/10.5194/acp-20-9855-2020, https://doi.org/10.5194/acp-20-9855-2020, 2020
Xiaolin Zhang, Mao Mao, Yan Yin, and Shihao Tang
Atmos. Chem. Phys., 20, 9701–9711, https://doi.org/10.5194/acp-20-9701-2020, https://doi.org/10.5194/acp-20-9701-2020, 2020
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The understanding of the absorption Ångstrom exponent (AAE) of aged black carbon (BC) particles affected by their microphysics is numerically evaluated. With key sensitive microphysical parameters, a simple parameterization of the AAE of coated BC with a size distribution is proposed. It is found that BC coated by thin brown carbon with more large particles shows an AAE smaller than pure BC particles. Our findings improve the understanding and application of the AAE of BC with brown coatings.
Laura Palacios-Peña, Philip Stier, Raquel Lorente-Plazas, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 20, 9679–9700, https://doi.org/10.5194/acp-20-9679-2020, https://doi.org/10.5194/acp-20-9679-2020, 2020
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It is widely known that the impact of aerosol–radiation and aerosol–cloud interactions on the radiative forcing is subject to large uncertainties. This is mainly due to the lack of understanding of aerosol optical properties and vertical distribution, whose uncertainties come from different processes. This work attempts to quantify the sensitivity of aerosol optical properties and their vertical distribution to key physico-chemical processes.
Jill S. Johnson, Leighton A. Regayre, Masaru Yoshioka, Kirsty J. Pringle, Steven T. Turnock, Jo Browse, David M. H. Sexton, John W. Rostron, Nick A. J. Schutgens, Daniel G. Partridge, Dantong Liu, James D. Allan, Hugh Coe, Aijun Ding, David D. Cohen, Armand Atanacio, Ville Vakkari, Eija Asmi, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 9491–9524, https://doi.org/10.5194/acp-20-9491-2020, https://doi.org/10.5194/acp-20-9491-2020, 2020
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We use over 9000 monthly aggregated grid-box measurements of aerosol to constrain the uncertainty in the HadGEM3-UKCA climate model. Measurements of AOD, PM2.5, particle number concentrations, sulfate and organic mass concentrations are compared to 1 million
variantsof the model using an implausibility metric. Despite many compensating effects in the model, the procedure constrains the probability distributions of many parameters, and direct radiative forcing uncertainty is reduced by 34 %.
Kamalika Sengupta, Kirsty Pringle, Jill S. Johnson, Carly Reddington, Jo Browse, Catherine E. Scott, and Ken Carslaw
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-756, https://doi.org/10.5194/acp-2020-756, 2020
Revised manuscript accepted for ACP
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Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which have 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.
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. Discuss., https://doi.org/10.5194/acp-2020-811, https://doi.org/10.5194/acp-2020-811, 2020
Revised manuscript accepted for ACP
Short summary
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Atmospheric particles over Earth's ocean surfaces have important climate effects. We examine key factors contributing to particle number, size and radiative effects over the Northwest Atlantic Ocean. Our results suggest key contributors are (1) particle formation near the marine boundary layer top, (2) particle growth by marine secondary organic aerosol, (3) dimethyl sulfide oxidation products and (4) ship emissions. We interpret NAAMES ship and aircraft measurements with the GEOS-Chem-TOMAS model.
Lili Ren, Yang Yang, Hailong Wang, Rudong Zhang, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 20, 9067–9085, https://doi.org/10.5194/acp-20-9067-2020, https://doi.org/10.5194/acp-20-9067-2020, 2020
Short summary
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Observations show that the concentrations of Arctic aerosols have declined since the early 1980s, which potentially contributed to the recent, rapid Arctic warming. We found that changes in sulfate and black carbon aerosols over the midlatitudes of the Northern Hemisphere had a larger impact on Arctic temperature than other regions and that the aerosol-induced temperature change explained approximately 20 % of the observed Arctic warming during 1980–2018.
Moa K. Sporre, Sara M. Blichner, Roland Schrödner, Inger H. H. Karset, Terje K. Berntsen, Twan van Noije, Tommi Bergman, Declan O'Donnell, and Risto Makkonen
Atmos. Chem. Phys., 20, 8953–8973, https://doi.org/10.5194/acp-20-8953-2020, https://doi.org/10.5194/acp-20-8953-2020, 2020
Short summary
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We investigate how emissions and parameters in current
SOA parameterisations in three ESMs affect both the resulting SOA in the models and the impact this has on climate through the direct and indirect aerosol effects. The SOA changes induce very different responses in the models, especially in terms of the indirect aerosol effect. This introduces uncertainties in ESM estimates of SOA climate impact through feedbacks in a warming climate and through anthropogenic land use change.
Gunnar Myhre, Bjørn H. Samset, Christian W. Mohr, Kari Alterskjær, Yves Balkanski, Nicolas Bellouin, Mian Chin, James Haywood, Øivind Hodnebrog, Stefan Kinne, Guangxing Lin, Marianne T. Lund, Joyce E. Penner, Michael Schulz, Nick Schutgens, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, and Kai Zhang
Atmos. Chem. Phys., 20, 8855–8865, https://doi.org/10.5194/acp-20-8855-2020, https://doi.org/10.5194/acp-20-8855-2020, 2020
Short summary
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The radiative forcing of the direct aerosol effects can be decomposed into clear-sky and cloudy-sky portions. In this study we use observational methods and two sets of multi-model global aerosol simulations over the industrial era to show that the contribution from cloudy-sky regions is likely weak.
Christa Genz, Roland Schrödner, Bernd Heinold, Silvia Henning, Holger Baars, Gerald Spindler, and Ina Tegen
Atmos. Chem. Phys., 20, 8787–8806, https://doi.org/10.5194/acp-20-8787-2020, https://doi.org/10.5194/acp-20-8787-2020, 2020
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Atmospheric aerosols are the precondition for the formation of cloud droplets and thus have a large influence on cloud properties. Concentrations of cloud condensation nuclei of the period with highest aerosol concentrations over central Europe are uncertain. In this work, modeled estimates of CCN from today and the mid-1980s are compared to available in situ and remote sensing observations. A scaling factor between today and the 1980s for the CCN concentrations has been derived.
Jiawei Li, Zhiwei Han, Yunfei Wu, Zhe Xiong, Xiangao Xia, Jie Li, Lin Liang, and Renjian Zhang
Atmos. Chem. Phys., 20, 8659–8690, https://doi.org/10.5194/acp-20-8659-2020, https://doi.org/10.5194/acp-20-8659-2020, 2020
Short summary
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Aerosol–radiation–climate interaction is one of the least understood mechanisms in air pollution and climate change. A coupled chemistry–climate model is developed to explore the mechanisms of haze evolution and aerosol radiative feedback in north China. The feedback exerts a significant impact on haze evolution. The contributions of physical and chemical processes to the feedback-induced aerosol changes are elucidated and quantified, providing new insights into the feedback mechanism.
Pierre Nabat, Samuel Somot, Christophe Cassou, Marc Mallet, Martine Michou, Dominique Bouniol, Bertrand Decharme, Thomas Drugé, Romain Roehrig, and David Saint-Martin
Atmos. Chem. Phys., 20, 8315–8349, https://doi.org/10.5194/acp-20-8315-2020, https://doi.org/10.5194/acp-20-8315-2020, 2020
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The present work aims at better understanding regional climate–aerosol interactions over the Euro-Mediterranean region by studying the relationships between aerosols and atmospheric circulation. Based on 40-year regional climate simulations (1979–2018), our results show the role of the North Atlantic Oscillation in driving the interannual aerosol variability, and that of weather regimes for the daily variability, with ensuing effects on shortwave surface radiation and surface temperature.
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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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