Articles | Volume 23, issue 13
https://doi.org/10.5194/acp-23-7741-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-7741-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
A thermodynamic framework for bulk–surface partitioning in finite-volume mixed organic–inorganic aerosol particles and cloud droplets
Ryan Schmedding
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Related authors
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
Short summary
Short summary
Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
Short summary
Short summary
In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233, https://doi.org/10.5194/acp-22-3203-2022, https://doi.org/10.5194/acp-22-3203-2022, 2022
Short summary
Short summary
Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
Short summary
Short summary
Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
Short summary
Short summary
We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
Short summary
Short summary
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys., 21, 2179–2190, https://doi.org/10.5194/acp-21-2179-2021, https://doi.org/10.5194/acp-21-2179-2021, 2021
Short summary
Short summary
Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. However, there are few studies attempting to investigate their interactions with water molecules. Here, we investigated the effect of organic coatings on the hygroscopic behavior of the inorganic core.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
Short summary
Short summary
This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
Short summary
Short summary
Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
Short summary
Short summary
Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
Short summary
Short summary
Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Kyle Gorkowski, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 19, 13383–13407, https://doi.org/10.5194/acp-19-13383-2019, https://doi.org/10.5194/acp-19-13383-2019, 2019
Short summary
Short summary
We present the new Binary Activity Thermodynamics (BAT) model, which is a water-sensitive reduced-complexity organic aerosol thermodynamics model. It can use bulk properties like O : C, molar mass, and RH to predict organic activity coefficients and water uptake behavior. We show applications in RH-dependent organic co-condensation, liquid–liquid phase separation, and Kohler curve predictions, and we validate the BAT model against laboratory measurements.
Hoi Ki Lam, Sze Man Shum, James F. Davies, Mijung Song, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 19, 9581–9593, https://doi.org/10.5194/acp-19-9581-2019, https://doi.org/10.5194/acp-19-9581-2019, 2019
Short summary
Short summary
We show the presence of dissolved inorganic salts could reduce the overall heterogeneous reactivity of organic compounds with gas–phase OH radicals at the surface by lowering the surface concentration of organic compounds. Until recently, the kinetic parameters reported in the literature were mostly measured based on experiments with pure organic particles. The lifetime of organic compounds or chemical tracers against heterogeneous OH reaction in the atmosphere could be longer than expected.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
Short summary
Short summary
The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
Ting Lei, Andreas Zuend, Yafang Cheng, Hang Su, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys., 18, 1045–1064, https://doi.org/10.5194/acp-18-1045-2018, https://doi.org/10.5194/acp-18-1045-2018, 2018
Short summary
Short summary
Measurements and thermodynamic equilibrium predictions for organic–inorganic aerosols related to components from biomass burning emissions demonstrate a diversity of hygroscopic growth and shrinking behavior, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). Controlled laboratory experiments with single solutes and/or with mixed organic–inorganic systems of known phase state will be useful to constrain model parameters of thermodynamic equilibrium models.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
Short summary
Short summary
Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
Short summary
Short summary
In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
Short summary
Short summary
Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
N. Hodas, A. Zuend, W. Mui, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, https://doi.org/10.5194/acp-15-5027-2015, 2015
G. Ganbavale, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 15, 447–493, https://doi.org/10.5194/acp-15-447-2015, https://doi.org/10.5194/acp-15-447-2015, 2015
Short summary
Short summary
This study presents a new, improved parameterisation of the temperature dependence of activity coefficients implemented in the AIOMFAC group-contribution model. The AIOMFAC model with the improved parameterisation is applicable for a large variety of aqueous organic as well as water-free organic solutions of relevance for atmospheric aerosols. The new model parameters were determined based on published and new thermodynamic equilibrium data covering a temperature range from ~190 to 440 K.
T. Lei, A. Zuend, W. G. Wang, Y. H. Zhang, and M. F. Ge
Atmos. Chem. Phys., 14, 11165–11183, https://doi.org/10.5194/acp-14-11165-2014, https://doi.org/10.5194/acp-14-11165-2014, 2014
G. Ganbavale, C. Marcolli, U. K. Krieger, A. Zuend, G. Stratmann, and T. Peter
Atmos. Chem. Phys., 14, 9993–10012, https://doi.org/10.5194/acp-14-9993-2014, https://doi.org/10.5194/acp-14-9993-2014, 2014
A. J. Huisman, U. K. Krieger, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 13, 6647–6662, https://doi.org/10.5194/acp-13-6647-2013, https://doi.org/10.5194/acp-13-6647-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Change from aerosol-driven to cloud-feedback-driven trend in short-wave radiative flux over the North Atlantic
A new process-based and scale-aware desert dust emission scheme for global climate models – Part I: Description and evaluation against inverse modeling emissions
Transported aerosols regulate the pre-monsoon rainfall over north-east India: a WRF-Chem modelling study
Collision-sticking rates of acid–base clusters in the gas phase determined from atomistic simulation and a novel analytical interacting hard-sphere model
Parameterization of size of organic and secondary inorganic aerosol for efficient representation of global aerosol optical properties
Model-based insights into aerosol perturbation on pristine continental convective precipitation
The impact of using assimilated Aeolus wind data on regional WRF-Chem dust simulations
On the differences in the vertical distribution of modeled aerosol optical depth over the southeastern Atlantic
A global evaluation of daily to seasonal aerosol and water vapor relationships using a combination of AERONET and NAAPS reanalysis data
Atlantic Multi-decadal Oscillation Modulates the Relationship Between El Niño-Southern Oscillation and Fire Weather in Australia
Impacts of reducing scattering and absorbing aerosols on the temporal extent and intensity of South and East Asian summer monsoon
Local and remote climate impacts of future African aerosol emissions
The dependence of aerosols' global and local precipitation impacts on the emitting region
Assessing the climate and air quality effects of future aerosol mitigation in India using a global climate model combined with statistical downscaling
Aggravated air pollution and health burden due to traffic congestion in urban China
Late summer transition from a free-tropospheric to boundary layer source of Aitken mode aerosol in the high Arctic
Self-lofting of wildfire smoke in the troposphere and stratosphere: simulations and space lidar observations
Aerosol emissions estimation with POLDER
Identifying climate model structural inconsistencies allows for tight constraint of aerosol radiative forcing
Multi-model ensemble projection of global dust cycle by the end of 21st century using CMIP6 data
Role of K-feldspar and quartz in global ice nucleation by mineral dust in mixed-phase clouds
Projected increases in wildfires may challenge regulatory curtailment of PM2.5 over the eastern US by 2050
Meteorological export and deposition fluxes of black carbon on glaciers of the central Chilean Andes
Future changes in atmospheric rivers over East Asia under stratospheric aerosol intervention
Modeling the influence of chain length on secondary organic aerosol (SOA) formation via multiphase reactions of alkanes
How aerosol size matters in aerosol optical depth (AOD) assimilation and the optimization using the Ångström exponent
Microphysical, macrophysical, and radiative responses of subtropical marine clouds to aerosol injections
Hemispheric-wide climate response to regional COVID-19-related aerosol emission reductions: the prominent role of atmospheric circulation adjustments
Impacts of an aerosol layer on a midlatitude continental system of cumulus clouds: how do these impacts depend on the vertical location of the aerosol layer?
Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioning
Effect of radiation interaction and aerosol processes on ventilation and aerosol concentrations in a real urban neighbourhood in Helsinki
A global climatology of ice-nucleating particles under cirrus conditions derived from model simulations with MADE3 in EMAC
Superimposed effects of typical local circulations driven by mountainous topography and aerosol-radiation interaction on heavy haze in the Beijing-Tianjin-Hebei central and southern plains in winter
Enviro-HIRLAM model estimates of elevated black carbon pollution over Ukraine resulted from forest fires
Where does the dust deposited over the Sierra Nevada snow come from?
Instant and delayed effects of March biomass burning aerosols over the Indochina Peninsula
Aerosol–cloud interaction in the atmospheric chemistry model GRAPES_Meso5.1/CUACE and its impacts on mesoscale numerical weather prediction under haze pollution conditions in Jing–Jin–Ji in China
Survival probabilities of atmospheric particles: comparison based on theory, cluster population simulations, and observations in Beijing
The simulation of mineral dust in the United Kingdom Earth System Model UKESM1
Dust pollution in China affected by different spatial and temporal types of El Niño
An improved representation of aerosol mixing state for air quality–weather interactions
Circulation-regulated impacts of aerosol pollution on urban heat island in Beijing
Size-resolved dust direct radiative effect efficiency derived from satellite observations
Modeling coarse and giant desert dust particles
Fire–climate interactions through the aerosol radiative effect in a global chemistry–climate–vegetation model
Contributions of meteorology and anthropogenic emissions to the trends in winter PM2.5 in eastern China 2013–2018
Impacts of condensable particulate matter on atmospheric organic aerosols and fine particulate matter (PM2.5) in China
Mapping the dependence of black carbon radiative forcing on emission region and season
Regional PM2.5 pollution confined by atmospheric internal boundaries in the North China Plain: boundary layer structures and numerical simulation
Toward targeted observations of the meteorological initial state for improving the PM2.5 forecast of a heavy haze event that occurred in the Beijing–Tianjin–Hebei region
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 23, 6743–6773, https://doi.org/10.5194/acp-23-6743-2023, https://doi.org/10.5194/acp-23-6743-2023, 2023
Short summary
Short summary
We determine what causes long-term trends in short-wave (SW) radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol, and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute to changes in clouds caused by greenhouse gas-induced warming.
Danny M. Leung, Jasper F. Kok, Longlei Li, Gregory S. Okin, Catherine Prigent, Martina Klose, Carlos Pérez García-Pando, Laurent Menut, Natalie M. Mahowald, David M. Lawrence, and Marcelo Chamecki
Atmos. Chem. Phys., 23, 6487–6523, https://doi.org/10.5194/acp-23-6487-2023, https://doi.org/10.5194/acp-23-6487-2023, 2023
Short summary
Short summary
Desert dust modeling is important for understanding climate change, as dust regulates the atmosphere's greenhouse effect and radiation. This study formulates and proposes a more physical and realistic desert dust emission scheme for global and regional climate models. By considering more aeolian processes in our emission scheme, our simulations match better against dust observations than existing schemes. We believe this work is vital in improving dust representation in climate models.
Neeldip Barman and Sharad Gokhale
Atmos. Chem. Phys., 23, 6197–6215, https://doi.org/10.5194/acp-23-6197-2023, https://doi.org/10.5194/acp-23-6197-2023, 2023
Short summary
Short summary
The study shows that during the pre-monsoon season transported aerosols, especially from the Indo-Gangetic Plain (IGP), have a greater impact with respect to air pollution, radiative forcing and rainfall over north-east (NE) India than emissions from within NE India itself. Hence, controlling emissions in the IGP will be significantly more fruitful in reducing pollution as well as climatic impacts over this region.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023, https://doi.org/10.5194/acp-23-5993-2023, 2023
Short summary
Short summary
We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
Short summary
Short summary
Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Mengjiao Jiang, Yaoting Li, Weiji Hu, Yinshan Yang, Guy Brasseur, and Xi Zhao
Atmos. Chem. Phys., 23, 4545–4557, https://doi.org/10.5194/acp-23-4545-2023, https://doi.org/10.5194/acp-23-4545-2023, 2023
Short summary
Short summary
Relatively clean background aerosol over the Tibetan Plateau makes the study of aerosol–cloud–precipitation interactions distinctive. A convection on 24 July 2014 in Naqu was selected using the Weather Research Forecasting (WRF) model, including the Thompson aerosol-aware microphysical scheme. Our study uses a compromise approach to the limited observations. We show that the transformation of cloud water to graupel and the development of convective clouds are favored in a polluted situation.
Pantelis Kiriakidis, Antonis Gkikas, Georgios Papangelis, Theodoros Christoudias, Jonilda Kushta, Emmanouil Proestakis, Anna Kampouri, Eleni Marinou, Eleni Drakaki, Angela Benedetti, Michael Rennie, Christian Retscher, Anne Grete Straume, Alexandru Dandocsi, Jean Sciare, and Vasilis Amiridis
Atmos. Chem. Phys., 23, 4391–4417, https://doi.org/10.5194/acp-23-4391-2023, https://doi.org/10.5194/acp-23-4391-2023, 2023
Short summary
Short summary
With the launch of the Aeolus satellite, higher-accuracy wind products became available. This research was carried out to validate the assimilated wind products by testing their effect on the WRF-Chem model predictive ability of dust processes. This was carried out for the eastern Mediterranean and Middle East region for two 2-month periods in autumn and spring 2020. The use of the assimilated products improved the dust forecasts of the autumn season (both quantitatively and qualitatively).
Ian Chang, Lan Gao, Connor J. Flynn, Yohei Shinozuka, Sarah J. Doherty, Michael S. Diamond, Karla M. Longo, Gonzalo A. Ferrada, Gregory R. Carmichael, Patricia Castellanos, Arlindo M. da Silva, Pablo E. Saide, Calvin Howes, Zhixin Xue, Marc Mallet, Ravi Govindaraju, Qiaoqiao Wang, Yafang Cheng, Yan Feng, Sharon P. Burton, Richard A. Ferrare, Samuel E. LeBlanc, Meloë S. Kacenelenbogen, Kristina Pistone, Michal Segal-Rozenhaimer, Kerry G. Meyer, Ju-Mee Ryoo, Leonhard Pfister, Adeyemi A. Adebiyi, Robert Wood, Paquita Zuidema, Sundar A. Christopher, and Jens Redemann
Atmos. Chem. Phys., 23, 4283–4309, https://doi.org/10.5194/acp-23-4283-2023, https://doi.org/10.5194/acp-23-4283-2023, 2023
Short summary
Short summary
Abundant aerosols are present above low-level liquid clouds over the southeastern Atlantic during late austral spring. The model simulation differences in the proportion of aerosol residing in the planetary boundary layer and in the free troposphere can greatly affect the regional aerosol radiative effects. This study examines the aerosol loading and fractional aerosol loading in the free troposphere among various models and evaluates them against measurements from the NASA ORACLES campaign.
Juli I. Rubin, Jeffrey S. Reid, Peng Xian, Christopher M. Selman, and Thomas F. Eck
Atmos. Chem. Phys., 23, 4059–4090, https://doi.org/10.5194/acp-23-4059-2023, https://doi.org/10.5194/acp-23-4059-2023, 2023
Short summary
Short summary
This work aims to quantify the covariability between aerosol optical depth/extinction with water vapor (PW) globally, using NASA AERONET observations and NAAPS model data. Findings are important for data assimilation and radiative transfer. The study shows statistically significant and positive AOD–PW relationships are found across the globe, varying in strength with location and season and tied to large-scale aerosol events. Hygroscopic growth was also found to be an important factor.
Guanyu Liu, Jing Li, and Tong Ying
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-858, https://doi.org/10.5194/acp-2022-858, 2023
Revised manuscript accepted for ACP
Short summary
Short summary
Fire weather in Australia is positively correlated with El Niño-Southern Oscillation (ENSO). However, their correlation is strengthened in the last two decades. Here, we show the correlation between ENSO and Australia fire weather index (FWI) increases from 0.17 to 0.70 when AMO shifts from its negative to positive phase. This is explained by the teleconnection effect. Warmer Atlantic generates Rossby wave trains and results in high pressures and a weather condition conducive to wildfires.
Chenwei Fang, Jim M. Haywood, Ju Liang, Ben T. Johnson, Ying Chen, and Bin Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2023-407, https://doi.org/10.5194/egusphere-2023-407, 2023
Short summary
Short summary
The responses of Asian summer monsoon duration and intensity to air pollution mitigation are identified given the Net-Zero future. We show that reducing scattering aerosols makes the rainy season longer and stronger across South and East Asia but absorbing aerosols reduction acts in the opposite way. Asian monsoon changes are ruled by scattering effects under the emission control of total aerosols. Our results hint distinct monsoon responses to emission controls that target different aerosols.
Christopher D. Wells, Matthew Kasoar, Nicolas Bellouin, and Apostolos Voulgarakis
Atmos. Chem. Phys., 23, 3575–3593, https://doi.org/10.5194/acp-23-3575-2023, https://doi.org/10.5194/acp-23-3575-2023, 2023
Short summary
Short summary
The climate is altered by greenhouse gases and air pollutant particles, and such emissions are likely to change drastically in the future over Africa. Air pollutants do not travel far, so their climate effect depends on where they are emitted. This study uses a climate model to find the climate impacts of future African pollutant emissions being either high or low. The particles absorb and scatter sunlight, causing the ground nearby to be cooler, but elsewhere the increased heat causes warming.
Geeta G. Persad
Atmos. Chem. Phys., 23, 3435–3452, https://doi.org/10.5194/acp-23-3435-2023, https://doi.org/10.5194/acp-23-3435-2023, 2023
Short summary
Short summary
Human-induced aerosol pollution has major impacts on both local and global precipitation. This study demonstrates using a global climate model that both the strength and localization of aerosols' precipitation impacts are highly dependent on which region the aerosols are emitted from. The findings highlight that the geographic distribution of human-induced aerosol emissions must be accounted for when quantifying their influence on global precipitation.
Tuuli Miinalainen, Harri Kokkola, Antti Lipponen, Antti-Pekka Hyvärinen, Vijay Kumar Soni, Kari E. J. Lehtinen, and Thomas Kühn
Atmos. Chem. Phys., 23, 3471–3491, https://doi.org/10.5194/acp-23-3471-2023, https://doi.org/10.5194/acp-23-3471-2023, 2023
Short summary
Short summary
We simulated the effects of aerosol emission mitigation on both global and regional radiative forcing and city-level air quality with a global-scale climate model. We used a machine learning downscaling approach to bias-correct the PM2.5 values obtained from the global model for the Indian megacity New Delhi. Our results indicate that aerosol mitigation could result in both improved air quality and less radiative heating for India.
Peng Wang, Ruhan Zhang, Shida Sun, Meng Gao, Bo Zheng, Dan Zhang, Yanli Zhang, Gregory R. Carmichael, and Hongliang Zhang
Atmos. Chem. Phys., 23, 2983–2996, https://doi.org/10.5194/acp-23-2983-2023, https://doi.org/10.5194/acp-23-2983-2023, 2023
Short summary
Short summary
In China, the number of vehicles has jumped significantly in the last decade. This caused severe traffic congestion and aggravated air pollution. In this study, we developed a new temporal allocation approach to quantify the impacts of traffic congestion. We found that traffic congestion worsens air quality and the health burden across China, especially in the urban clusters. More effective and comprehensive vehicle emission control policies should be implemented to improve air quality in China.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
Short summary
Short summary
Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Kevin Ohneiser, Albert Ansmann, Jonas Witthuhn, Hartwig Deneke, Alexandra Chudnovsky, Gregor Walter, and Fabian Senf
Atmos. Chem. Phys., 23, 2901–2925, https://doi.org/10.5194/acp-23-2901-2023, https://doi.org/10.5194/acp-23-2901-2023, 2023
Short summary
Short summary
This study shows that smoke layers can reach the tropopause via the self-lofting effect within 3–7 d in the absence of pyrocumulonimbus convection if the
aerosol optical thickness is larger than approximately 2 for a longer time period. When reaching the stratosphere, wildfire smoke can sensitively influence the stratospheric composition on a hemispheric scale and thus can affect the Earth’s climate and the ozone layer.
Athanasios Tsikerdekis, Otto P. Hasekamp, Nick A. J. Schutgens, and Qirui Zhong
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2023-41, https://doi.org/10.5194/acp-2023-41, 2023
Revised manuscript accepted for ACP
Short summary
Short summary
Aerosol are tiny particles of different substance (species) that can be emitted into the atmosphere by natural processes or by anthropogenic activities. However, the actual aerosol emission amount per species is highly uncertain. Thus in this work we are correcting the aerosol emissions used to drive a global aerosol/climate model using satellite observations through a process called data assimilation. These more accurate aerosol emissions can lead to a more accurate weather/climate prediction.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2023-77, https://doi.org/10.5194/egusphere-2023-77, 2023
Short summary
Short summary
Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty, and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
Yuan Zhao, Xu Yue, Yang Cao, Jun Zhu, Chenguang Tian, Hao Zhou, Yuwen Chen, Yihan Hu, Weijie Fu, and Xu Zhao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-760, https://doi.org/10.5194/acp-2022-760, 2023
Revised manuscript accepted for ACP
Short summary
Short summary
We project the future changes of dust emissions and loading using an ensemble of model outputs from CMIP6 under four scenarios. We find increased dust emissions and loading in North Africa due to increased drought but strengthened surface wind, while decreased dust loading over Asia following the enhanced precipitation. Such spatial pattern remains similar though the regional intensity varies among different scenarios.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
Short summary
Short summary
Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
Chandan Sarangi, Yun Qian, L. Ruby Leung, Yang Zhang, Yufei Zou, and Yuhang Wang
Atmos. Chem. Phys., 23, 1769–1783, https://doi.org/10.5194/acp-23-1769-2023, https://doi.org/10.5194/acp-23-1769-2023, 2023
Short summary
Short summary
We show that for air quality, the densely populated eastern US may see even larger impacts of wildfires due to long-distance smoke transport and associated positive climatic impacts, partially compensating the improvements from regulations on anthropogenic emissions. This study highlights the tension between natural and anthropogenic contributions and the non-local nature of air pollution that complicate regulatory strategies for improving future regional air quality for human health.
Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
Atmos. Chem. Phys., 23, 1749–1768, https://doi.org/10.5194/acp-23-1749-2023, https://doi.org/10.5194/acp-23-1749-2023, 2023
Short summary
Short summary
Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Ju Liang and Jim Haywood
Atmos. Chem. Phys., 23, 1687–1703, https://doi.org/10.5194/acp-23-1687-2023, https://doi.org/10.5194/acp-23-1687-2023, 2023
Short summary
Short summary
The recent record-breaking flood events in China during the summer of 2021 highlight the importance of mitigating the risks from future changes in high-impact weather systems under global warming. Based on a state-of-the-art Earth system model, we demonstrate a pilot study on the responses of atmospheric rivers and extreme precipitation over East Asia to anthropogenically induced climate warming and an unconventional mitigation strategy – stratospheric aerosol injection.
Azad Madhu, Myoseon Jang, and David Deacon
Atmos. Chem. Phys., 23, 1661–1675, https://doi.org/10.5194/acp-23-1661-2023, https://doi.org/10.5194/acp-23-1661-2023, 2023
Short summary
Short summary
SOA formation is simulated using the UNIPAR model for series of linear alkanes. The inclusion of autoxidation reactions within the explicit gas mechanisms of C9–C12 was found to significantly improve predictions. Available product distributions were extrapolated with an incremental volatility coefficient (IVC) to predict SOA formation of alkanes without explicit mechanisms. These product distributions were used to simulate SOA formation from C13 and C15 and had good agreement with chamber data.
Jianbing Jin, Bas Henzing, and Arjo Segers
Atmos. Chem. Phys., 23, 1641–1660, https://doi.org/10.5194/acp-23-1641-2023, https://doi.org/10.5194/acp-23-1641-2023, 2023
Short summary
Short summary
Aerosol models and satellite retrieval algorithms rely on different aerosol size assumptions. In practice, differences between simulations and observations do not always reflect the difference in aerosol amount. To avoid inconsistencies, we designed a hybrid assimilation approach. Different from a standard aerosol optical depth (AOD) assimilation that directly assimilates AODs, the hybrid one estimates aerosol size parameters by assimilating Ängström observations before assimilating the AODs.
Je-Yun Chun, Robert Wood, Peter Blossey, and Sarah J. Doherty
Atmos. Chem. Phys., 23, 1345–1368, https://doi.org/10.5194/acp-23-1345-2023, https://doi.org/10.5194/acp-23-1345-2023, 2023
Short summary
Short summary
We investigate the impact of injected aerosol on subtropical low marine clouds under a variety of meteorological conditions using high-resolution model simulations. This study illustrates processes perturbed by aerosol injections and their impact on cloud properties (e.g., cloud number concentration, thickness, and cover). We show that those responses are highly sensitive to background meteorological conditions, such as precipitation, and background cloud properties.
Nora L. S. Fahrenbach and Massimo A. Bollasina
Atmos. Chem. Phys., 23, 877–894, https://doi.org/10.5194/acp-23-877-2023, https://doi.org/10.5194/acp-23-877-2023, 2023
Short summary
Short summary
We studied the monthly-scale climate response to COVID-19 aerosol emission reductions during January–May 2020 using climate models. Our results show global temperature and rainfall anomalies driven by circulation changes. The climate patterns reverse polarity from JF to MAM due to a shift in the main SO2 reduction region from China to India. This real-life example of rapid climate adjustments to abrupt, regional aerosol emission reduction has large implications for future climate projections.
Seoung Soo Lee, Junshik Um, Won Jun Choi, Kyung-Ja Ha, Chang Hoon Jung, Jianping Guo, and Youtong Zheng
Atmos. Chem. Phys., 23, 273–286, https://doi.org/10.5194/acp-23-273-2023, https://doi.org/10.5194/acp-23-273-2023, 2023
Short summary
Short summary
This paper elaborates on process-level mechanisms regarding how the interception of radiation by aerosols interacts with the surface heat fluxes and atmospheric instability in warm cumulus clouds. This paper elucidates how these mechanisms vary with the location or altitude of an aerosol layer. This elucidation indicates that the location of aerosol layers should be taken into account for parameterizations of aerosol–cloud interactions.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
Short summary
Short summary
Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Jani Strömberg, Xiaoyu Li, Mona Kurppa, Heino Kuuluvainen, Liisa Pirjola, and Leena Järvi
EGUsphere, https://doi.org/10.5194/egusphere-2022-978, https://doi.org/10.5194/egusphere-2022-978, 2023
Short summary
Short summary
In this study we concluded that with low wind speeds, solar radiation has a larger decreasing effect (53 %) on pollutant concentrations than aerosol processes (18 %). Additionally, our results showed that with solar radiation included, pollutant concentrations were closer to observations (-13 %) than with only aerosol processes (+97 %). This has implications when planning simulations under calm conditions such as our case and deciding whether or not simulations need to include these processes.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 22, 15887–15907, https://doi.org/10.5194/acp-22-15887-2022, https://doi.org/10.5194/acp-22-15887-2022, 2022
Short summary
Short summary
Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, their global atmospheric distribution in the cirrus regime is still very uncertain. We present a global climatology of INPs under cirrus conditions derived from model simulations, considering the mineral dust, soot, crystalline ammonium sulfate, and glassy organics INP types. The comparison of respective INP concentrations indicates the large importance of ammonium sulfate particles.
Yue Peng, Hong Wang, Xiaoye Zhang, Zhaodong Liu, Wenjie Zhang, Siting Li, Chen Han, and Huizheng Che
EGUsphere, https://doi.org/10.5194/egusphere-2022-780, https://doi.org/10.5194/egusphere-2022-780, 2022
Short summary
Short summary
This study demonstrates a strong link between local circulation, aerosols-radiation interaction (ARI), and haze pollution. Under the weak weather-scale systems, the typical local circulation driven by mountainous topography is the main cause of pollutant distribution in the Beijing-Tianjin-Hebei region, and the ARI mechanism amplifies this influence of local circulation on pollutants, making haze pollution aggravated by the superposition of both.
Mykhailo Savenets, Larysa Pysarenko, Svitlana Krakovska, Alexander Mahura, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 15777–15791, https://doi.org/10.5194/acp-22-15777-2022, https://doi.org/10.5194/acp-22-15777-2022, 2022
Short summary
Short summary
The paper explores the spatio-temporal variability of black carbon during a wildfire in August 2010, with a focus on Ukraine. As a research tool, the seamless Enviro-HIRLAM modelling system is used for investigating the atmospheric transport of aerosol particles emitted by wildfires from remote and local sources. The results of this study improve our understanding of the physical and chemical processes and the interactions of aerosols in the atmosphere.
Huilin Huang, Yun Qian, Ye Liu, Cenlin He, Jianyu Zheng, Zhibo Zhang, and Antonis Gkikas
Atmos. Chem. Phys., 22, 15469–15488, https://doi.org/10.5194/acp-22-15469-2022, https://doi.org/10.5194/acp-22-15469-2022, 2022
Short summary
Short summary
Using a clustering method developed in the field of artificial neural networks, we identify four typical dust transport patterns across the Sierra Nevada, associated with the mesoscale and regional-scale wind circulations. Our results highlight the connection between dust transport and dominant weather patterns, which can be used to understand dust transport in a changing climate.
Anbao Zhu, Haiming Xu, Jiechun Deng, Jing Ma, and Shaofeng Hua
Atmos. Chem. Phys., 22, 15425–15447, https://doi.org/10.5194/acp-22-15425-2022, https://doi.org/10.5194/acp-22-15425-2022, 2022
Short summary
Short summary
This study demonstrates the instant and delayed effects of biomass burning (BB) aerosols on precipitation over the Indochina Peninsula (ICP). The convection suppression due to the BB aerosol-induced stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to an overall reduced precipitation in March, while the delayed effect promotes precipitation from early April to mid April due to the anomalous atmospheric circulations.
Wenjie Zhang, Hong Wang, Xiaoye Zhang, Liping Huang, Yue Peng, Zhaodong Liu, Xiao Zhang, and Huizheng Che
Atmos. Chem. Phys., 22, 15207–15221, https://doi.org/10.5194/acp-22-15207-2022, https://doi.org/10.5194/acp-22-15207-2022, 2022
Short summary
Short summary
Aerosol–cloud interaction (ACI) is first implemented in the atmospheric chemistry system GRAPES_Meso5.1/CUACE. ACI can improve the simulated cloud, temperature, and precipitation under haze pollution conditions in Jing-Jin-Ji in China. This paper demonstrates the critical role of ACI in current numerical weather prediction over the severely polluted region.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091, https://doi.org/10.5194/acp-22-15071-2022, https://doi.org/10.5194/acp-22-15071-2022, 2022
Short summary
Short summary
We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Stephanie Woodward, Alistair A. Sellar, Yongming Tang, Marc Stringer, Andrew Yool, Eddy Robertson, and Andy Wiltshire
Atmos. Chem. Phys., 22, 14503–14528, https://doi.org/10.5194/acp-22-14503-2022, https://doi.org/10.5194/acp-22-14503-2022, 2022
Short summary
Short summary
We describe the dust scheme in the UKESM1 Earth system model and show generally good agreement with observations. Comparing with the closely related HadGEM3-GC3.1 model, we show that dust differences are not only due to inter-model differences but also to the dust size distribution. Under climate change, HadGEM3-GC3.1 dust hardly changes, but UKESM1 dust decreases because that model includes the vegetation response which, in our models, has a bigger impact on dust than climate change itself.
Yang Yang, Liangying Zeng, Hailong Wang, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 22, 14489–14502, https://doi.org/10.5194/acp-22-14489-2022, https://doi.org/10.5194/acp-22-14489-2022, 2022
Short summary
Short summary
Using an aerosol–climate model, dust pollution in China affected by different spatial and temporal types of El Niño are examined. Both eastern and central Pacific El Niño and short-duration El Niño increase winter dust concentrations over northern China, while long-duration El Niño decreases concentrations. Only long-duration El Niño events can significantly affect dust over China in the following spring. This study has profound implications for air pollution control and dust storm prediction.
Robin Stevens, Andrei Ryjkov, Mahtab Majdzadeh, and Ashu Dastoor
Atmos. Chem. Phys., 22, 13527–13549, https://doi.org/10.5194/acp-22-13527-2022, https://doi.org/10.5194/acp-22-13527-2022, 2022
Short summary
Short summary
Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
Fan Wang, Gregory R. Carmichael, Jing Wang, Bin Chen, Bo Huang, Yuguo Li, Yuanjian Yang, and Meng Gao
Atmos. Chem. Phys., 22, 13341–13353, https://doi.org/10.5194/acp-22-13341-2022, https://doi.org/10.5194/acp-22-13341-2022, 2022
Short summary
Short summary
Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. We find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.
Qianqian Song, Zhibo Zhang, Hongbin Yu, Jasper F. Kok, Claudia Di Biagio, Samuel Albani, Jianyu Zheng, and Jiachen Ding
Atmos. Chem. Phys., 22, 13115–13135, https://doi.org/10.5194/acp-22-13115-2022, https://doi.org/10.5194/acp-22-13115-2022, 2022
Short summary
Short summary
This study developed a dataset that enables us to efficiently calculate dust direct radiative effect (DRE, i.e., cooling or warming our planet) for any given dust size distribution in addition to three sets of dust mineral components and two dust shapes. We demonstrate and validate the method of using this dataset to calculate dust DRE. Moreover, using this dataset we found that dust mineral composition is a more important factor in determining dust DRE than dust size and shape.
Eleni Drakaki, Vassilis Amiridis, Alexandra Tsekeri, Antonis Gkikas, Emmanouil Proestakis, Sotirios Mallios, Stavros Solomos, Christos Spyrou, Eleni Marinou, Claire L. Ryder, Demetri Bouris, and Petros Katsafados
Atmos. Chem. Phys., 22, 12727–12748, https://doi.org/10.5194/acp-22-12727-2022, https://doi.org/10.5194/acp-22-12727-2022, 2022
Short summary
Short summary
State-of-the-art atmospheric dust models have limitations in accounting for a realistic dust size distribution (emission, transport). We modify the parameterization of the mineral dust cycle by including particles with diameter >20 μm, as indicated by observations over deserts. Moreover, we investigate the effects of reduced settling velocities of dust particles. Model results are evaluated using airborne and spaceborne dust measurements above Cabo Verde.
Chenguang Tian, Xu Yue, Jun Zhu, Hong Liao, Yang Yang, Yadong Lei, Xinyi Zhou, Hao Zhou, Yimian Ma, and Yang Cao
Atmos. Chem. Phys., 22, 12353–12366, https://doi.org/10.5194/acp-22-12353-2022, https://doi.org/10.5194/acp-22-12353-2022, 2022
Short summary
Short summary
We quantify the impacts of fire aerosols on climate through direct, indirect, and albedo effects. In atmosphere-only simulations, we find global fire aerosols cause surface cooling and rainfall inhibition over many land regions. These fast atmospheric perturbations further lead to a reduction in regional leaf area index and lightning activities. By considering the feedback of fire aerosols on humidity, lightning, and leaf area index, we predict a slight reduction in fire emissions.
Yanxing Wu, Run Liu, Yanzi Li, Junjie Dong, Zhijiong Huang, Junyu Zheng, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 11945–11955, https://doi.org/10.5194/acp-22-11945-2022, https://doi.org/10.5194/acp-22-11945-2022, 2022
Short summary
Short summary
Multiple linear regression (MLR) analyses often interpret the correlation coefficient (r2) as the contribution of an independent variable to the dependent variable. Since a good correlation does not imply a causal relationship, we propose that r2 should be interpreted as the maximum possible contribution. Moreover, MLR results are sensitive to the length of time analyzed; long-term analysis gives a more accurate assessment because of its additional constraints.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
Short summary
Short summary
This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Petri Räisänen, Joonas Merikanto, Risto Makkonen, Mikko Savolahti, Alf Kirkevåg, Maria Sand, Øyvind Seland, and Antti-Ilari Partanen
Atmos. Chem. Phys., 22, 11579–11602, https://doi.org/10.5194/acp-22-11579-2022, https://doi.org/10.5194/acp-22-11579-2022, 2022
Short summary
Short summary
A climate model is used to evaluate how the radiative forcing (RF) associated with black carbon (BC) emissions depends on the latitude, longitude, and seasonality of emissions. It is found that both the direct RF (BC absorption of solar radiation in air) and snow RF (BC absorption in snow/ice) depend strongly on the emission region and season. The results suggest that, for a given mass of BC emitted, climatic impacts are likely to be largest for high-latitude emissions due to the large snow RF.
Xipeng Jin, Xuhui Cai, Mingyuan Yu, Yu Song, Xuesong Wang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 22, 11409–11427, https://doi.org/10.5194/acp-22-11409-2022, https://doi.org/10.5194/acp-22-11409-2022, 2022
Short summary
Short summary
Meteorological discontinuities in the vertical direction define the lowest atmosphere as the boundary layer, while in the horizontal direction it identifies the contrast zone as the internal boundary. Both of them determine the polluted air mass dimension over the North China Plain. This study reveals the boundary layer structures under three categories of internal boundaries, modified by thermal, dynamical, and blending effects. It provides a new insight to understand regional pollution.
Lichao Yang, Wansuo Duan, Zifa Wang, and Wenyi Yang
Atmos. Chem. Phys., 22, 11429–11453, https://doi.org/10.5194/acp-22-11429-2022, https://doi.org/10.5194/acp-22-11429-2022, 2022
Short summary
Short summary
The initial meteorological state has a great impact on PM2.5 forecasts. Assimilating additional observations is an effective way to improve the accuracy of the initial meteorological state. Here we used an advanced optimization approach to identify where we should preferentially place the meteorological observations associated with PM2.5 forecasts in the Beijing–Tianjin–Hebei region of China. We provide evidence that the target observation strategy is effective for improving PM2.5 forecasts.
Cited articles
Abrams, D. S. and Prausnitz, J. M.: Statistical thermodynamics of liquid
mixtures: A new expression for the excess Gibbs energy of partly or
completely miscible systems, AIChE Journal, 21, 116–128,
https://doi.org/10.1002/aic.690210115, 1975. a
Bellouin, N., Quaas, J., Gryspeerdt, E., Kinne, S., Stier, P., Watson-Parris,
D., Boucher, O., Carslaw, K. S., Christensen, M., Daniau, A.-L., Dufresne,
J.-L., Feingold, G., Fiedler, S., Forster, P., Gettelman, A., Haywood, J. M.,
Lohmann, U., Malavelle, F., Mauritsen, T., McCoy, D. T., Myhre, G.,
Mülmenstädt, J., Neubauer, D., Possner, A., Rugenstein, M., Sato, Y.,
Schulz, M., Schwartz, S. E., Sourdeval, O., Storelvmo, T., Toll, V., Winker,
D., and Stevens, B.: Bounding Global Aerosol Radiative Forcing of Climate
Change, Rev. Geophys., 58, e2019RG000660,
https://doi.org/10.1029/2019RG000660, 2020. a
Binyaminov, H., Abdullah, F., Zargarzadeh, L., and Elliott, J. A. W.:
Thermodynamic Investigation of Droplet–Droplet and Bubble–Droplet
Equilibrium in an Immiscible Medium, J. Phys. Chem. B,
125, 8636–8651, https://doi.org/10.1021/acs.jpcb.1c02877, 2021. a
Booth, A. M., Topping, D. O., McFiggans, G., and Percival, C. J.: Surface
tension of mixed inorganic and dicarboxylic acid aqueous solutions at 298.15 K and their importance for cloud activation predictions, Phys. Chem. Chem.
Phys., 11, 8021–8028, https://doi.org/10.1039/B906849J, 2009. a, b, c
Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster,
P., Kerminen, V. M., Kondo, Y., Liao, H., Lohmann, U., Rasch, P., Satheesh,
S. K., Sherwood, S., Stevens, B., and Zhang, X. Y.: Clouds and aerosols,
Climate Change 2013: The Physical Science Basis, Contribution of Working
Group I to the Fifth Assessment Report of the Intergovernmental Panel on
Climate Change, 571–657, https://doi.org/10.1017/CBO9781107415324.016, 2013. a
Burnett, R., Chen, H., Szyszkowicz, M., Fann, N., Hubbell, B., Pope, C. A.,
Apte, J. S., Brauer, M., Cohen, A., Weichenthal, S., Coggins, J., Di, Q.,
Brunekreef, B., Frostad, J., Lim, S. S., Kan, H., Walker, K. D., Thurston,
G. D., Hayes, R. B., Lim, C. C., Turner, M. C., Jerrett, M., Krewski, D.,
Gapstur, S. M., Diver, W. R., Ostro, B., Goldberg, D., Crouse, D. L., Martin,
R. V., Peters, P., Pinault, L., Tjepkema, M., van Donkelaar, A., Villeneuve,
P. J., Miller, A. B., Yin, P., Zhou, M., Wang, L., Janssen, N. A. H., Marra,
M., Atkinson, R. W., Tsang, H., Quoc Thach, T., Cannon, J. B., Allen, R. T.,
Hart, J. E., Laden, F., Cesaroni, G., Forastiere, F., Weinmayr, G., Jaensch,
A., Nagel, G., Concin, H., and Spadaro, J. V.: Global estimates of mortality
associated with long-term exposure to outdoor fine particulate matter,
P. Natl. Acad. Sci. USA, 115, 9592–9597,
https://doi.org/10.1073/pnas.1803222115, 2018. a
Butler, J. A. V. and Kendall, J. P.: The thermodynamics of the surfaces of
solutions, P. Roy. Soc. Lond. A, 135, 348–375,
https://doi.org/10.1098/rspa.1932.0040, 1932. a
Bzdek, B. R., Power, R. M., Simpson, S. H., Reid, J. P., and Royall, C. P.:
Precise, contactless measurements of the surface tension of picolitre
aerosol droplets, Chem. Sci., 7, 274–285, https://doi.org/10.1039/C5SC03184B, 2016. a, b, c
Bzdek, B. R., Reid, J. P., Malila, J., and Prisle, N. L.: The surface tension
of surfactant-containing, finite volume droplets, P. Natl.
Acad. Sci. USA, 117, 8335–8343, https://doi.org/10.1073/pnas.1915660117, 2020. a, b
Cai, X. and Griffin, R. J.: Theoretical Modeling of the Size-Dependent
Influence of Surface Tension on the Absorptive Partitioning of Semi-Volatile
Organic Compounds, J. Atmos. Chem., 50, 139–158,
https://doi.org/10.1007/s10874-005-2364-2, 2005. a
Chan, A. W. H., Kautzman, K. E., Chhabra, P. S., Surratt, J. D., Chan, M. N., Crounse, J. D., Kürten, A., Wennberg, P. O., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs), Atmos. Chem. Phys., 9, 3049–3060, https://doi.org/10.5194/acp-9-3049-2009, 2009. a
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.:
Liquid–Liquid Phase Separation in Mixed Organic/Inorganic Aerosol
Particles, J. Phys. Chem. A, 113, 10966–10978,
https://doi.org/10.1021/jp905054d, 2009. a
Cohen, A. J., Brauer, M., Burnett, R., Anderson, H. R., Frostad, J., Estep, K.,
Balakrishnan, K., Brunekreef, B., Dandona, L., Dandona, R., Feigin, V.,
Freedman, G., Hubbell, B., Jobling, A., Kan, H., Knibbs, L., Liu, Y., Martin,
R., Morawska, L., Pope, C. A., Shin, H., Straif, K., Shaddick, G., Thomas,
M., van Dingenen, R., van Donkelaar, A., Vos, T., Murray, C. J. L., and
Forouzanfar, M. H.: Estimates and 25-year trends of the global burden of
disease attributable to ambient air pollution: an analysis of data from the
Global Burden of Diseases Study 2015, The Lancet, 389, 1907–1918,
https://doi.org/10.1016/S0140-6736(17)30505-6, 2017. a
Defay, R., Prigogine, I., and Bellemans, A.: Surface tension and adsorption, Longmans, London, ark:/13960/s2ffcbbxv31, 1966. a
Dutcher, C. S., Wexler, A. S., and Clegg, S. L.: Surface Tensions of Inorganic
Multicomponent Aqueous Electrolyte Solutions and Melts, J.
Phys. Chem. A, 114, 12216–12230, https://doi.org/10.1021/jp105191z, 2010. a
Ernst, R. C., Watkins, C. H., and Ruwe, H.: The Physical Properties of the
Ternary System Ethyl Alcohol–Glycerin–Water, J. Phys.
Chem., 40, 627–635, 1935. a
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011. a
Facchini, M. C., Mircea, M., Fuzzi, S., and Charlson, R. J.: Cloud albedo
enhancement by surface-active organic solutes in growing droplets, Nature,
401, 257–259, https://doi.org/10.1038/45758, 1999. a
Facchini, M. C., Decesari, S., Mircea, M., Fuzzi, S., and Loglio, G.: Surface
tension of atmospheric wet aerosol and cloud/fog droplets in relation to
their organic carbon content and chemical composition, Atmos.
Environ., 34, 4853–4857,
https://doi.org/10.1016/S1352-2310(00)00237-5, 2000. a
Forestieri, S. D., Staudt, S. M., Kuborn, T. M., Faber, K., Ruehl, C. R., Bertram, T. H., and Cappa, C. D.: Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics, Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, 2018. a, b
Fredenslund, A., Jones, R. L., and Prausnitz, J. M.: Group-contribution
estimation of activity coefficients in nonideal liquid mixtures, AIChE
Journal, 21, 1086–1099, https://doi.org/10.1002/aic.690210607, 1975. a
Gérard, V., Nozière, B., Baduel, C., Fine, L., Frossard, A. A., and Cohen,
R. C.: Anionic, Cationic, and Nonionic Surfactants in Atmospheric Aerosols
from the Baltic Coast at Askö, Sweden: Implications for Cloud Droplet
Activation, Environ. Sci. Technol., 50, 2974–2982,
https://doi.org/10.1021/acs.est.5b05809, 2016. a
Gérard, V., Noziere, B., Fine, L., Ferronato, C., Singh, D. K., Frossard,
A. A., Cohen, R. C., Asmi, E., Lihavainen, H., Kivekäs, N., Aurela, M.,
Brus, D., Frka, S., and Cvitešić Kušan, A.: Concentrations and Adsorption
Isotherms for Amphiphilic Surfactants in PM1 Aerosols from Different Regions
of Europe, Environ. Sci. Technol., 53, 12379–12388,
https://doi.org/10.1021/acs.est.9b03386, 2019. a
Gervasi, N. R., Topping, D. O., and Zuend, A.: A predictive group-contribution model for the viscosity of aqueous organic aerosol, Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, 2020. a, b
Gibbs, J. W.: On the Equilibrium of Heterogeneous Substances, Am. J. Sci., s3-16, 441–458, https://doi.org/10.2475/ajs.s3-16.96.441, 1874. a, b
Goldsack, D. E. and White, B. R.: An iterative technique for calculating
surface tensions of -on-electrolyte solutions, Can. J. Chem.,
61, 1725–1729, https://doi.org/10.1139/v83-295, 1983. a, b, c
Guggenheim, E. A.: The thermodynamics of interfaces in systems of several
components, T. Faraday Soc., 35, 397–412,
https://doi.org/10.1039/TF9403500397, 1940. a
Guggenheim, E. A.: Mixtures; the theory of the equilibrium properties of some simple classes of mixtures, solutions and alloys, The International series of monographs on physics, Clarendon Press, Oxford, ark:/13960/s20q1n7jcr8, 1952. a
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009. a
Hansen, A. M. K., Hong, J., Raatikainen, T., Kristensen, K., Ylisirniö, A., Virtanen, A., Petäjä, T., Glasius, M., and Prisle, N. L.: Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate, Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, 2015. a
Hyvärinen, A.-P., Lihavainen, H., Gaman, A., Vairila, L., Ojala, H., Kulmala, M., and Viisanen, Y.: Surface Tensions and Densities
of Oxalic, Malonic, Succinic, Maleic, Malic, and cis-Pinonic Acids, J. Chem. Eng. Data, 51, 255–260,
https://doi.org/10.1021/je050366x, 2006. a
Huang, Y., Mahrt, F., Xu, S., Shiraiwa, M., Zuend, A., and Bertram, A. K.:
Coexistence of three liquid phases in individual atmospheric aerosol
particles, P. Natl. Acad. Sci. USA, 118,
e2102512118, https://doi.org/10.1073/pnas.2102512118, 2021. a
Jenkin, M. E., Saunders, S. M., and Pilling, M. J.: The tropospheric
degradation of volatile organic compounds: a protocol for mechanism
development, Atmos. Environ., 31, 81–104,
https://doi.org/10.1016/S1352-2310(96)00105-7, 1997. a
Jenkin, M. E., Wyche, K. P., Evans, C. J., Carr, T., Monks, P. S., Alfarra, M. R., Barley, M. H., McFiggans, G. B., Young, J. C., and Rickard, A. R.: Development and chamber evaluation of the MCM v3.2 degradation scheme for β-caryophyllene, Atmos. Chem. Phys., 12, 5275–5308, https://doi.org/10.5194/acp-12-5275-2012, 2012. a
Jenkin, M. E., Young, J. C., and Rickard, A. R.: The MCM v3.3.1 degradation scheme for isoprene, Atmos. Chem. Phys., 15, 11433–11459, https://doi.org/10.5194/acp-15-11433-2015, 2015. a
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang,
Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken,
A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L.,
Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun,
Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara,
P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J.,
null null, Dunlea, J., Huffman, J. A., Onasch, T. B., Alfarra, M. R.,
Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann,
S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R.,
Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang,
Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C.,
Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb,
C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols
in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353,
2009. a
Jura, G. and Harkins, W. D.: Surfaces of Solids. XIV. A Unitary Thermodynamic
Theory of the Adsorption of Vapors on Solids and of Insoluble Films on Liquid
Subphases, J. Am. Chem. Soc., 68, 1941–1952,
https://doi.org/10.1021/ja01214a022, 1946. a, b, c
Kleinheins, J., Shardt, N., El Haber, M., Ferronato, C., Nozière, B., Peter,
T., and Marcolli, C.: Surface tension models for binary aqueous solutions: a
review and intercomparison, Phys. Chem. Chem. Phys., 25, 11055–11074,
https://doi.org/10.1039/D3CP00322A, 2023. a
Köhler, H.: The nucleus in and the growth of hygroscopic droplets,
T. Faraday Soc., 32, 1152–1161,
https://doi.org/10.1039/TF9363201152, 1936. a
Kroflič, A., Frka, S., Simmel, M., Wex, H., and Grgić, I.: Size-Resolved
Surface-Active Substances of Atmospheric Aerosol: Reconsideration of the
Impact on Cloud Droplet Formation, Environ. Sci. Technol., 52,
9179–9187, https://doi.org/10.1021/acs.est.8b02381, 2018. a
Kuwata, M. and Martin, S. T.: Phase of atmospheric secondary organic material
affects its reactivity, P. Natl. Acad. Sci. USA, 109,
17354–17359, https://doi.org/10.1073/pnas.1209071109, 2012. a
Kwamena, N. O. A., Buajarern, J., and Reid, J. P.: Equilibrium Morphology of
Mixed Organic/Inorganic/Aqueous Aerosol Droplets: Investigating the Effect of
Relative Humidity and Surfactants, J. Phys. Chem. A, 114,
5787–5795, https://doi.org/10.1021/jp1003648, 2010. a
Laaksonen, A. and Kulmala, M.: An explicit cluster model for binary nuclei in
water–alcohol systems, J. Chem. Phys., 95, 6745–6748,
https://doi.org/10.1063/1.461513, 1991. a
Lane, J.: Surface Activity Coefficients, Adsorption from Solution, Academic Press, London, 115, 51–64, https://doi.org/10.1016/B978-0-12-530980-6.50008-5, 1983. a, b
Lang-Yona, N., Abo-Riziq, A., Erlick, C., Segre, E., Trainic, M., and Rudich,
Y.: Interaction of internally mixed aerosols with light, Phys. Chem.
Chem. Phys., 12, 21–31, https://doi.org/10.1039/B913176K, 2010. a
Lee, H. D., Estillore, A. D., Morris, H. S., Ray, K. K., Alejandro, A.,
Grassian, V. H., and Tivanski, A. V.: Direct Surface Tension Measurements of
Individual Sub-Micrometer Particles Using Atomic Force Microscopy,
J. Phys. Chem. A, 121, 8296–8305,
https://doi.org/10.1021/acs.jpca.7b04041, 2017. a
Lin, J. J., Kristensen, T. B., Calderón, S. M., Malila, J., and Prisle, N. L.:
Effects of surface tension time-evolution for CCN activation of a complex
organic surfactant, Environ. Sci.-Processes and Impacts, 22,
271–284, https://doi.org/10.1039/C9EM00426B, 2020. a
Malila, J. and Prisle, N. L.: A Monolayer Partitioning Scheme for Droplets of
Surfactant Solutions, J. Adv. Model. Earth Sy., 10,
3233–3251, https://doi.org/10.1029/2018MS001456, 2018. a, b, c
McGraw, R. and Wang, J.: Surfactants and cloud droplet activation: A systematic
extension of Köhler theory based on analysis of droplet stability,
J. Chem. Phys., 154, 024707, https://doi.org/10.1063/5.0031436, 2021. a
Moré, J. J., Garbow, B. S., and Hillstrom, K. E.: User Guide for MINPACK-1,
Argonne National Laboratory Report ANL-80-74,
http://www.netlib.org/minpack/ (last access: 16 May 2028), 1980. a
Moré, J. J., Sorensen, D. C., Hillstrom, K. E., and Garbow, B. S.: The MINPACK Project, in: Sources and Development of Mathematical Software, Prentice-Hall, Inc., Englewood Cliffs, New Jersey, United States, ark:/13960/t07x3kd4r, 1984. a
Ng, N. L., Kroll, J. H., Chan, A. W. H., Chhabra, P. S., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from m-xylene, toluene, and benzene, Atmos. Chem. Phys., 7, 3909–3922, https://doi.org/10.5194/acp-7-3909-2007, 2007. a
Nozière, B., Baduel, C., and Jaffrezo, J.-L.: The dynamic surface tension of
atmospheric aerosol surfactants reveals new aspects of cloud activation,
Nat. Commun., 5, 3335, https://doi.org/10.1038/ncomms4335, 2014. a
Ovadnevaite, J., Zuend, A., Laaksonen, A., Sanchez, K. J., Roberts, G.,
Ceburnis, D., Decesari, S., Rinaldi, M., Hodas, N., Facchini, M. C.,
Seinfeld, J. H., and O’ Dowd, C.: Surface tension prevails over solute
effect in organic-influenced cloud droplet activation, Nature, 546, 637–641,
https://doi.org/10.1038/nature22806, 2017. a, b, c, d, e, f, g, h, i, j, k, l, m, n, o, p, q
Ozdemir, O., Karakashev, S. I., Nguyen, A. V., and Miller, J. D.: Adsorption
and surface tension analysis of concentrated alkali halide brine solutions,
Miner. Eng., 22, 263–271,
https://doi.org/10.1016/j.mineng.2008.08.001, 2009. a
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007. a, b
Petters, S. S. and Petters, M. D.: Surfactant effect on cloud condensation
nuclei for two-component internally mixed aerosols, J. Geophys.
Res.-Atmos., 121, 1878–1895,
https://doi.org/10.1002/2015JD024090, 2016. a
Pinsky, M., Mazin, I. P., Korolev, A., and Khain, A.: Supersaturation and
diffusional droplet growth in liquid clouds: Polydisperse spectra, J.
Geophys. Res.-Atmos., 119, 12872–12887,
https://doi.org/10.1002/2014JD021885, 2014. a, b
Pokhrel, R. P., Gordon, J., Fiddler, M. N., and Bililign, S.: Impact of
combustion conditions on physical and morphological properties of biomass
burning aerosol, Aerosol Sci. Technol., 55, 80–91,
https://doi.org/10.1080/02786826.2020.1822512, 2021. a
Prisle, N. L., Raatikainen, T., Sorjamaa, R., Svenningsson, B., Laaksonen, A.,
and Bilde, M.: Surfactant partitioning in cloud droplet activation: a study
of C8, C10, C12 and C14 normal fatty acid sodium salts, Tellus B, 60,
416–431, https://doi.org/10.1111/j.1600-0889.2008.00352.x, 2008. a, b
Prisle, N. L., Raatikainen, T., Laaksonen, A., and Bilde, M.: Surfactants in cloud droplet activation: mixed organic-inorganic particles, Atmos. Chem. Phys., 10, 5663–5683, https://doi.org/10.5194/acp-10-5663-2010, 2010. a, b
Prisle, N. L., Dal Maso, M., and Kokkola, H.: A simple representation of surface active organic aerosol in cloud droplet formation, Atmos. Chem. Phys., 11, 4073–4083, https://doi.org/10.5194/acp-11-4073-2011, 2011. a, b
Rastak, N., Pajunoja, A., Acosta Navarro, J. C., Ma, J., Song, M., Partridge,
D. G., Kirkevåg, A., Leong, Y., Hu, W. W., Taylor, N. F., Lambe, A.,
Cerully, K., Bougiatioti, A., Liu, P., Krejci, R., Petäjä, T., Percival,
C., Davidovits, P., Worsnop, D. R., Ekman, A. M. L., Nenes, A., Martin, S.,
Jimenez, J. L., Collins, D. R., Topping, D., Bertram, A. K., Zuend, A.,
Virtanen, A., and Riipinen, I.: Microphysical explanation of the RH-dependent
water affinity of biogenic organic aerosol and its importance for climate,
Geophys. Res. Lett., 44, 5167–5177,
https://doi.org/10.1002/2017GL073056, 2017. a, b, c, d
Reid, J. P., Dennis-Smither, B. J., Kwamena, N.-O. A., Miles, R. E. H.,
Hanford, K. L., and Homer, C. J.: The morphology of aerosol particles
consisting of hydrophobic and hydrophilic phases: hydrocarbons, alcohols and
fatty acids as the hydrophobic component, Phys. Chem. Chem.
Phys., 13, 15559–15572, https://doi.org/10.1039/C1CP21510H, 2011. a
Riipinen, I., Koponen, I. K., Frank, G. P., Hyvärinen, A.-P., Vanhanen, J.,
Lihavainen, H., Lehtinen, K. E. J., Bilde, M., and Kulmala, M.: Adipic and
Malonic Acid Aqueous Solutions: Surface Tensions and Saturation Vapor
Pressures, J. Phys. Chem. A, 111, 12995–13002,
https://doi.org/10.1021/jp073731v, 2007. a, b
Romakkaniemi, S., Kokkola, H., Smith, J. N., Prisle, N. L., Schwier, A. N., McNeill, V. F., and Laaksonen, A.: Partitioning of semivolatile surface-active compounds between bulk, surface and gas phase, Geophys. Res. Lett., 38, L03807, https://doi.org/10.1029/2010GL046147, 2011. a
Ruehl, C. R. and Wilson, K. R.: Surface Organic Monolayers Control the
Hygroscopic Growth of Submicrometer Particles at High Relative Humidity, J. Phys. Chem. A, 118, 3952–3966, https://doi.org/10.1021/jp502844g,
2014. a
Schmedding, R., Ma, M., Zhang, Y., Farrell, S., Pye, H. O. T., Chen, Y., Wang,
C.-t., Rasool, Q. Z., Budisulistiorini, S. H., Ault, A. P., Surratt, J. D.,
and Vizuete, W.: alpha-Pinene-Derived organic coatings on acidic sulfate
aerosol impacts secondary organic aerosol formation from isoprene in a box
model, Atmos. Environ., 213, 456–462,
https://doi.org/10.1016/j.atmosenv.2019.06.005, 2019. a
Schmedding, R., Rasool, Q. Z., Zhang, Y., Pye, H. O. T., Zhang, H., Chen, Y., Surratt, J. D., Lopez-Hilfiker, F. D., Thornton, J. A., Goldstein, A. H., and Vizuete, W.: Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model, Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, 2020. a
Seinfeld, J. H., Bretherton, C., Carslaw, K. S., Coe, H., DeMott, P. J.,
Dunlea, E. J., Feingold, G., Ghan, S., Guenther, A. B., Kahn, R., Kraucunas,
I., Kreidenweis, S. M., Molina, M. J., Nenes, A., Penner, J. E., Prather,
K. A., Ramanathan, V., Ramaswamy, V., Rasch, P. J., Ravishankara, A. R.,
Rosenfeld, D., Stephens, G., and Wood, R.: Improving our fundamental
understanding of the role of aerosol−cloud interactions in the climate
system, P. Natl. Acad. Sci. USA, 113, 5781–5790,
https://doi.org/10.1073/pnas.1514043113, 2016. a
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle
particle partitioning of atmospheric aerosols: interplay of physical state,
non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15,
11441–11453, https://doi.org/10.1039/C3CP51595H, 2013. a
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12, 2691–2712, https://doi.org/10.5194/acp-12-2691-2012, 2012. a
Song, M., Marcolli, C., Krieger, U. K., Lienhard, D. M., and Peter, T.:
Morphologies of mixed organic/inorganic/aqueous aerosol droplets, Faraday
Discuss., 165, 289–316, https://doi.org/10.1039/C3FD00049D, 2013. a
Sorjamaa, R. and Laaksonen, A.: The effect of H2O adsorption on cloud drop activation of insoluble particles: a theoretical framework, Atmos. Chem. Phys., 7, 6175–6180, https://doi.org/10.5194/acp-7-6175-2007, 2007. a
Sorjamaa, R., Svenningsson, B., Raatikainen, T., Henning, S., Bilde, M., and Laaksonen, A.: The role of surfactants in Köhler theory reconsidered, Atmos. Chem. Phys., 4, 2107–2117, https://doi.org/10.5194/acp-4-2107-2004, 2004. a, b, c, d
Sprow, F. B. and Prausnitz, J. M.: Surface tensions of simple liquid mixtures,
T. Faraday Soc., 62, 1105–1111, https://doi.org/10.1039/TF9666201105, 1966. a
Surratt, J. D., Chan, A. W. H., Eddingsaas, N. C., Chan, M., Loza, C. L., Kwan,
A. J., Hersey, S. P., Flagan, R. C., Wennberg, P. O., and Seinfeld, J. H.:
Reactive intermediates revealed in secondary organic aerosol formation from
isoprene, P. Natl. Acad. Sci. USA, 107, 6640–6645,
https://doi.org/10.1073/pnas.0911114107, 2010. a
Szyszkowski, B. V.: Experimentelle Studien über kapillare Eigenschaften der wässerigen Lösungen von Fettsäuren, Zeitschrift für Physikalische Chemie 385–414, https://doi.org/10.1515/zpch-1908-6425, 1908. a, b, c
Topping, D., Barley, M., Bane, M. K., Higham, N., Aumont, B., Dingle, N., and McFiggans, G.: UManSysProp v1.0: an online and open-source facility for molecular property prediction and atmospheric aerosol calculations, Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, 2016. a
Topping, D. O., McFiggans, G. B., Kiss, G., Varga, Z., Facchini, M. C., Decesari, S., and Mircea, M.: Surface tensions of multi-component mixed inorganic/organic aqueous systems of atmospheric significance: measurements, model predictions and importance for cloud activation predictions, Atmos. Chem. Phys., 7, 2371–2398, https://doi.org/10.5194/acp-7-2371-2007, 2007. a, b
Vepsäläinen, S., Calderón, S. M., Malila, J., and Prisle, N. L.: Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 1: moderately surface active organics, Atmos. Chem. Phys., 22, 2669–2687, https://doi.org/10.5194/acp-22-2669-2022, 2022. a, b, c
Vepsäläinen, S., Calderón, S. M., and Prisle, N. L.: Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: strong surfactants, EGUsphere [preprint], https://doi.org/10.5194/egusphere-2022-1188, 2023. a, b
Wexler, A. S. and Dutcher, C. S.: Statistical Mechanics of Multilayer Sorption:
Surface Tension, J. Phys. Chem. Lett., 4, 1723–1726,
https://doi.org/10.1021/jz400725p, 2013. a, b
Yin, H., Dou, J., Klein, L., Krieger, U. K., Bain, A., Wallace, B. J., Preston, T. C., and Zuend, A.: Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation, Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, 2022. a
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich,
I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K.,
Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne,
J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y.,
Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K.,
Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys.
Res. Lett., 34, 13, https://doi.org/10.1029/2007GL029979, 2007. a
Zhou, S., Hwang, B. C. H., Lakey, P. S. J., Zuend, A., Abbatt, J. P. D., and
Shiraiwa, M.: Multiphase reactivity of polycyclic aromatic hydrocarbons is
driven by phase separation and diffusion limitations, P. Natl. Acad. Sci. USA, 116, 11658–11663,
https://doi.org/10.1073/pnas.1902517116, 2019. a
Zuend, A. and Seinfeld, J. H.: A practical method for the calculation of
liquid–liquid equilibria in multicomponent organic–water–electrolyte
systems using physicochemical constraints, Fluid Phase Equilibr., 337,
201–213, https://doi.org/10.1016/j.fluid.2012.09.034, 2013. a
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008. a
Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols, Atmos. Chem. Phys., 10, 7795–7820, https://doi.org/10.5194/acp-10-7795-2010, 2010. a, b
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011. a
Short summary
Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The enrichment of compounds in the surface of an aerosol particle may lead to depletion of that species in the interior bulk of the particle. We present a framework for modeling the equilibrium bulk–surface partitioning of mixed organic–inorganic particles, including cases of co-condensation of semivolatile organic compounds and species with extremely limited solubility in the bulk or surface of a particle.
Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The...
Altmetrics
Final-revised paper
Preprint