Articles | Volume 22, issue 14
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Quantifying the effects of mixing state on aerosol optical properties
Jeffrey H. Curtis
Department of Mechanical Science and Engineering, University of Illinois Urbana-Champaign, Urbana, IL 61801, USA
Meteorological Research Institute, Japan Meteorological Agency, Tsukuba, Ibaraki, 305-0052, Japan
National Institute of Polar Research, 10-3 Midori-cho, Tachikawa, Tokyo, 190-8518, Japan
Research Institute for Humanity and Nature, 457-4 Motoyama, Kamigamo, Kita-ku, Kyoto, 603-8047, Japan
now at: Arid Land Research Center, Tottori University, 1390 Hamasaka, Tottori, 680-0001, Japan
Computational and Information Systems Laboratory, National Center for Atmospheric Research, Boulder, CO 80307, USA
Climate and Global Dynamics Laboratory, National Center for Atmospheric Research, Boulder, CO 80307, USA
Advanced Study Program, National Center for Atmospheric Research, Boulder, CO 80307, USA
No articles found.
Lingcheng Li, Yilin Fang, Zhonghua Zheng, Mingjie Shi, Marcos Longo, Charles D. Koven, Jennifer A. Holm, Rosie A. Fisher, Nate G. McDowell, Jeffrey Chambers, and L. Ruby Leung
Geosci. Model Dev., 16, 4017–4040,Short summary
Accurately modeling plant coexistence in vegetation demographic models like ELM-FATES is challenging. This study proposes a repeatable method that uses machine-learning-based surrogate models to optimize plant trait parameters in ELM-FATES. Our approach significantly improves plant coexistence modeling, thus reducing errors. It has important implications for modeling ecosystem dynamics in response to climate change.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev. Discuss.,
Revised manuscript accepted for GMDShort summary
The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations, and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model-satellite discrepancies, we find that future field campaigns in an East African region (30° E – 45° E, 5° S – 5° N) could substantially improve the predictive skill of air quality models.
Sudipta Ghosh, Sagnik Dey, Sushant Das, Nicole Riemer, Graziano Giuliani, Dilip Ganguly, Chandra Venkataraman, Filippo Giorgi, Sachchida Nand Tripathi, Srikanthan Ramachandran, Thazhathakal Ayyappen Rajesh, Harish Gadhavi, and Atul Kumar Srivastava
Geosci. Model Dev., 16, 1–15,Short summary
Accurate representation of aerosols in climate models is critical for minimizing the uncertainty in climate projections. Here, we implement region-specific emission fluxes and a more accurate scheme for carbonaceous aerosol ageing processes in a regional climate model (RegCM4) and show that it improves model performance significantly against in situ, reanalysis, and satellite data over the Indian subcontinent. We recommend improving the model performance before using them for climate studies.
Matthew L. Dawson, Christian Guzman, Jeffrey H. Curtis, Mario Acosta, Shupeng Zhu, Donald Dabdub, Andrew Conley, Matthew West, Nicole Riemer, and Oriol Jorba
Geosci. Model Dev., 15, 3663–3689,Short summary
Progress in identifying complex, mixed-phase physicochemical processes has resulted in an advanced understanding of the evolution of atmospheric systems but has also introduced a level of complexity that few atmospheric models were designed to handle. We present a flexible treatment for multiphase chemical processes for models of diverse scale, from box up to global models. This enables users to build a customized multiphase mechanism that is accessible to a much wider community.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741,Short summary
Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Mizuo Kajino, Makoto Deushi, Tsuyoshi Thomas Sekiyama, Naga Oshima, Keiya Yumimoto, Taichu Yasumichi Tanaka, Joseph Ching, Akihiro Hashimoto, Tetsuya Yamamoto, Masaaki Ikegami, Akane Kamada, Makoto Miyashita, Yayoi Inomata, Shin-ichiro Shima, Pradeep Khatri, Atsushi Shimizu, Hitoshi Irie, Kouji Adachi, Yuji Zaizen, Yasuhito Igarashi, Hiromasa Ueda, Takashi Maki, and Masao Mikami
Geosci. Model Dev., 14, 2235–2264,Short summary
This study compares performance of aerosol representation methods of the Japan Meteorological Agency's regional-scale nonhydrostatic meteorology–chemistry model (NHM-Chem). It indicates separate treatment of sea salt and dust in coarse mode and that of light-absorptive and non-absorptive particles in fine mode could provide accurate assessments on aerosol feedback processes.
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,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.
Mizuo Kajino, Makoto Deushi, Tsuyoshi Thomas Sekiyama, Naga Oshima, Keiya Yumimoto, Taichu Yasumichi Tanaka, Joseph Ching, Akihiro Hashimoto, Tetsuya Yamamoto, Masaaki Ikegami, Akane Kamada, Makoto Miyashita, Yayoi Inomata, Shin-ichiro Shima, Kouji Adachi, Yuji Zaizen, Yasuhito Igarashi, Hiromasa Ueda, Takashi Maki, and Masao Mikami
Geosci. Model Dev. Discuss.,
Revised manuscript not accepted
Jeffrey H. Curtis, Nicole Riemer, and Matthew West
Geosci. Model Dev., 10, 4057–4079,Short summary
Traditional aerosol representations rely on simplifying assumptions about the aerosol composition in order to reduce computational cost. This introduces errors in estimates of aerosol impacts on climate. In contrast, the WRF-PartMC-MOSAIC-SCM model, presented here, uses a particle-resolved aerosol representation. It is made feasible by the development of efficient numerical methods, and allows for the capture of complex aerosol mixing states with altitude.
Joseph Ching, Jerome Fast, Matthew West, and Nicole Riemer
Atmos. Chem. Phys., 17, 7445–7458,Short summary
The composition of individual aerosols affects their cloud condensation nuclei (CCN) properties, but is challenging to represent in models. This study quantifies the error in CCN calculations when per-particle information is neglected by using a metric for the composition diversity within a population. With more particle-level measurements from field campaigns, the approach is useful for quantifying uncertainties in composition-dependent quantities regarding aerosol–cloud–climate interactions.
Megan D. Willis, Robert M. Healy, Nicole Riemer, Matthew West, Jon M. Wang, Cheol-Heon Jeong, John C. Wenger, Greg J. Evans, Jonathan P. D. Abbatt, and Alex K. Y. Lee
Atmos. Chem. Phys., 16, 4693–4706,
L. Fierce, N. Riemer, and T. C. Bond
Atmos. Chem. Phys., 15, 3173–3191,Short summary
The timescale for particles containing black carbon to age from hydrophobic to hygroscopic strongly influences black carbon's atmospheric lifetime and climate impact. This paper identifies the minimal set of independent variables needed to explain variance in this aging timescale. This work distills the complex interactions captured by a particle-resolved aerosol model to a few input variables and is a first step toward developing physically based parameterizations of aerosol aging.
R. M. Healy, N. Riemer, J. C. Wenger, M. Murphy, M. West, L. Poulain, A. Wiedensohler, I. P. O'Connor, E. McGillicuddy, J. R. Sodeau, and G. J. Evans
Atmos. Chem. Phys., 14, 6289–6299,
J. C. Kaiser, J. Hendricks, M. Righi, N. Riemer, R. A. Zaveri, S. Metzger, and V. Aquila
Geosci. Model Dev., 7, 1137–1157,
J. Tian, N. Riemer, M. West, L. Pfaffenberger, H. Schlager, and A. Petzold
Atmos. Chem. Phys., 14, 5327–5347,
N. Riemer and M. West
Atmos. Chem. Phys., 13, 11423–11439,
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2Anthropogenic amplification of biogenic secondary organic aerosol productionA dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modelingModeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impactsAssessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of ChinaImpact of Landes forest fires on air quality in France during the 2022 summerGlobal nitrogen and sulfur deposition mapping using a measurement–model fusion approachComprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional modelImplications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilationSimulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulatorModelling wintertime sea-spray aerosols under Arctic haze conditionsImpact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6Reactive Organic Carbon Air Emissions from Mobile Sources in the United StatesLinking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem modelA multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean SeaContribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global modelCoarse particulate matter air quality in East Asia: implications for fine particulate nitrateForeign emissions exacerbate PM2.5 pollution in China through nitrate chemistryAnalysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, ChinaSimulation of organic aerosol, its precursors, and related oxidants in the Landes pine forest in southwestern France: accounting for domain-specific land use and physical conditionsSubstantially positive contributions of new particle formation to Cloud Condensation Nuclei under low supersaturation in China based on numerical model improvementsModelling the European wind-blown dust emissions and their impact on particulate matter (PM) concentrationsEvolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern ChinaImpacts of estimated plume rise on PM2.5 exceedance prediction during extreme wildfire events: a comparison of three schemes (Briggs, Freitas, and Sofiev)Effects of Secondary Organic Aerosol Water on fine PM levels and composition over USStrong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon BasinSources of organic aerosols in eastern China: a modeling study with high-resolution intermediate-volatility and semivolatile organic compound emissionsComposited analyses of the chemical and physical characteristics of co-polluted days by ozone and PM2.5 over 2013–2020 in the Beijing–Tianjin–Hebei regionObservation-based constraints on modeled aerosol surface area: implications for heterogeneous chemistryOligomer formation from the gas-phase reactions of Criegee intermediates with hydroperoxide esters: mechanism and kineticsModelling SO2 conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012Global distribution of Asian, Middle Eastern, and North African dust simulated by CESM1/CARMAOpinion: Coordinated development of emission inventories for climate forcers and air pollutantsSeasonal modeling analysis of nitrate formation pathways in Yangtze River Delta region, ChinaModeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate modelNumerical simulation of the impact of COVID-19 lockdown on tropospheric composition and aerosol radiative forcing in EuropeEvaluation of the WRF and CHIMERE models for the simulation of PM2.5 in large East African urban conurbationsImpact of urban heat island on inorganic aerosol in the lower free troposphere: a case study in Hangzhou, ChinaStatistical and machine learning methods for evaluating trends in air quality under changing meteorological conditionsSimulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimatesSecondary organic aerosol formation via multiphase reaction of hydrocarbons in urban atmospheres using CAMx integrated with the UNIPAR modelContrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effectsEffect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulationsA new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosolsLimitations in representation of physical processes prevent successful simulation of PM2.5 during KORUS-AQEurodelta multi-model simulated and observed particulate matter trends in Europe in the period of 1990–2010Elucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formationFast climate responses to emission reductions in aerosol and ozone precursors in China during 2013–2017
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216,Short summary
Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007,Short summary
Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804,Short summary
We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
María Gonçalves Ageitos, Vincenzo Obiso, Ron L. Miller, Oriol Jorba, Martina Klose, Matt Dawson, Yves Balkanski, Jan Perlwitz, Sara Basart, Enza Di Tomaso, Jerónimo Escribano, Francesca Macchia, Gilbert Montané, Natalie M. Mahowald, Robert O. Green, David R. Thompson, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8623–8657,Short summary
Dust aerosols affect our climate differently depending on their mineral composition. We include dust mineralogy in an atmospheric model considering two existing soil maps, which still have large associated uncertainties. The soil data and the distribution of the minerals in different aerosol sizes are key to our model performance. We find significant regional variations in climate-relevant variables, which supports including mineralogy in our current models and the need for improved soil maps.
Jianyan Lu, Sunling Gong, Jian Zhang, Jianmin Chen, Lei Zhang, and Chunhong Zhou
Atmos. Chem. Phys., 23, 8021–8037,Short summary
WRF/CUACE was used to assess the cloud chemistry contribution in China. Firstly, the CUACE cloud chemistry scheme was found to reproduce well the cloud processing and consumption of H2O2, O3, and SO2, as well as the increase of sulfate. Secondly, during cloud availability in December under a heavy pollution episode, sulfate production increased 60–95 % and SO2 was reduced by over 80 %. This study provides a way to analyze the phenomenon of overestimation of SO2 in many chemical transport models.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296,Short summary
This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 23, 7091–7102,Short summary
We update the 2010 global deposition budget for nitrogen (N) and sulfur (S) with new regional wet deposition measurements, improving the ensemble results of 11 global chemistry transport models from HTAP II. Our study demonstrates that a global measurement–model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO goal of global fusion products for accurately mapping harmful air pollution.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896,Short summary
New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys., 23, 6647–6662,Short summary
Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have a notable influence on simulated regional abundances of anthropogenic aerosol over the 1990–2019 period. This, in turn, affects estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies on anthropogenic aerosols using different emission inventories.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240,Short summary
A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782,Short summary
Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678,Short summary
Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486,Short summary
Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu H. Jathar, Li Li, Andrew A. May, and Allen L. Robinson
We update methods for calculating organic particle and vapor emissions from mobile sources in the U.S. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099,Short summary
Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
We developed and evaluated processes affecting within-day (diel) variability in fine particulate matter (PM2.5) concentrations in a chemical transport model (GEOS-Chem) over the US. We find that diel variability in PM2.5 is driven by 1) early morning accumulation into a shallow mixed layer, 2) decreases from mid-morning through afternoon with mixed-layer growth, 3) increases from mid-afternoon through evening as the mixed-layer collapses, and 4) decreases overnight as emissions decrease.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemistry transport models.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461,Short summary
New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281,Short summary
Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163,Short summary
Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104,Short summary
From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeño, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys., 23, 3679–3706,Short summary
This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (southwestern France). Several sensitivity cases involving biogenic emission factors, land cover data, anthropogenic emissions, and physical or meteorological parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy is discussed.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
New particle formation is one of the important sources of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools for understanding the evolution of atmospheric particles, however, their usefulness may be large discounted due to the existence of model biases. In this study, we first improve the model behavior through parametrization adjustments. Utilizing the improved model, we find substantial contributions of newly formed particles on climate.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys., 23, 3629–3654,Short summary
Wind-blown dust (WBD) emissions emitted from European soils are estimated for the 2007–2016 period, and their impact on the total particulate matter (PM) concentration is calculated. We found a considerable increase in PM concentrations due to such emissions, especially on selected days (rather than on a seasonal average). We also found that WBD emissions are strongest over western Europe, and the highest impacts on PM are calculated for this region.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. Analysis atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Yunyao Li, Daniel Tong, Siqi Ma, Saulo R. Freitas, Ravan Ahmadov, Mikhail Sofiev, Xiaoyang Zhang, Shobha Kondragunta, Ralph Kahn, Youhua Tang, Barry Baker, Patrick Campbell, Rick Saylor, Georg Grell, and Fangjun Li
Atmos. Chem. Phys., 23, 3083–3101,Short summary
Plume height is important in wildfire smoke dispersion and affects air quality and human health. We assess the impact of plume height on wildfire smoke dispersion and the exceedances of the National Ambient Air Quality Standards. A higher plume height predicts lower pollution near the source region, but higher pollution in downwind regions, due to the faster spread of the smoke once ejected, affects pollution exceedance forecasts and the early warning of extreme air pollution events.
Stylianos Kakavas, Spyros Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds, but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out year-long aerosol simulations over the continental US. We show that such organic water impacts can have an important impact on dry PM1 levels when RH levels and PM1 concentrations are high.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272,Short summary
The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344,Short summary
This paper aims to build up an approach to establish a high-resolution emission inventory of intermediate-volatility and semi-volatile organic compounds in city-scale and detailed source categories and incorporate it into the CMAQ model. We believe this approach can be widely applied to improve the simulation of secondary organic aerosol and its source contributions.
Huibin Dai, Hong Liao, Ke Li, Xu Yue, Yang Yang, Jia Zhu, Jianbing Jin, Baojie Li, and Xingwen Jiang
Atmos. Chem. Phys., 23, 23–39,Short summary
We apply the 3-D global chemical transport model (GEOS-Chem) to simulate co-polluted days by O3 and PM2.5 (O3–PM2.5PDs) in Beijing–Tianjin–Hebei in 2013–2020 and investigate the chemical and physical characteristics of O3–PM2.5PDs by composited analyses of such days that are captured by both the observations and the model. We report for the first time the unique features in vertical distributions of aerosols during O3–PM2.5PDs and the physical and chemical characteristics of O3–PM2.5PDs.
Rachel A. Bergin, Monica Harkey, Alicia Hoffman, Richard H. Moore, Bruce Anderson, Andreas Beyersdorf, Luke Ziemba, Lee Thornhill, Edward Winstead, Tracey Holloway, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 15449–15468,Short summary
Correctly predicting aerosol surface area concentrations is important for determining the rate of heterogeneous reactions in chemical transport models. Here, we compare aircraft measurements of aerosol surface area with a regional model. In polluted air masses, we show that the model underpredicts aerosol surface area by a factor of 2. Despite this disagreement, the representation of heterogeneous chemistry still dominates the overall uncertainty in the loss rate of molecules such as N2O5.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 14529–14546,Short summary
Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Mathieu Lachatre, Sylvain Mailler, Laurent Menut, Arineh Cholakian, Pasquale Sellitto, Guillaume Siour, Henda Guermazi, Giuseppe Salerno, and Salvatore Giammanco
Atmos. Chem. Phys., 22, 13861–13879,Short summary
In this study, we have evaluated the predominance of various pathways of volcanic SO2 conversion to sulfates in the upper troposphere. We show that the main conversion pathway was gaseous oxidation by OH, although the liquid pathways were expected to be predominant. These results are interesting with respect to a better understanding of sulfate formation in the middle and upper troposphere and are an important component to help evaluate particulate matter radiative forcing.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676,Short summary
Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Steven J. Smith, Erin E. McDuffie, and Molly Charles
Atmos. Chem. Phys., 22, 13201–13218,Short summary
Emissions into the atmosphere of greenhouse gases (GHGs) and air pollutants, quantified in emission inventories, impact human health, ecosystems, and the climate. We review how air pollutant and GHG inventory activities have historically been structured and their different uses and requirements. We discuss the benefits of increasing coordination between air pollutant and GHG inventory development efforts, but also caution that there are differences in appropriate methodologies and applications.
Jinjin Sun, Momei Qin, Xiaodong Xie, Wenxing Fu, Yang Qin, Li Sheng, Lin Li, Jingyi Li, Ishaq Dimeji Sulaymon, Lei Jiang, Lin Huang, Xingna Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 12629–12646,Short summary
NO3- has become the dominant and the least reduced chemical component of fine particulate matter in China. NO3- formation is mostly in the NH3-rich regime in the Yangtze River Delta (YRD). OH + NO2 contributes 60 %–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes 10 %–36 %. The N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute 50 %–62 % and 38 %–50 % to YRD NO3- concentrations, respectively.
Thomas Drugé, Pierre Nabat, Marc Mallet, Martine Michou, Samuel Rémy, and Oleg Dubovik
Atmos. Chem. Phys., 22, 12167–12205,Short summary
This study presents the implementation of brown carbon in the atmospheric component of the CNRM global climate model and particularly in its aerosol scheme TACTIC. Several simulations were carried out with this climate model, over the period 2000–2014, to evaluate the model by comparison with different reference datasets (PARASOL-GRASP, OMI-OMAERUVd, MACv2, FMI_SAT, AERONET) and to analyze the brown carbon radiative and climatic effects.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917,Short summary
In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701,Short summary
A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Hanqing Kang, Bin Zhu, Gerrit de Leeuw, Bu Yu, Ronald J. van der A, and Wen Lu
Atmos. Chem. Phys., 22, 10623–10634,Short summary
This study quantified the contribution of each urban-induced meteorological effect (temperature, humidity, and circulation) to aerosol concentration. We found that the urban heat island (UHI) circulation dominates the UHI effects on aerosol. The UHI circulation transports aerosol and its precursor gases from the warmer lower boundary layer to the colder lower free troposphere and promotes the secondary formation of ammonium nitrate aerosol in the cold atmosphere.
Minghao Qiu, Corwin Zigler, and Noelle E. Selin
Atmos. Chem. Phys., 22, 10551–10566,Short summary
Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but little is known about their performance. Using cases in the US and China, we show that widely used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policymakers and researchers.
Junri Zhao, Weichun Ma, Kelsey R. Bilsback, Jeffrey R. Pierce, Shengqian Zhou, Ying Chen, Guipeng Yang, and Yan Zhang
Atmos. Chem. Phys., 22, 9583–9600,Short summary
Marine dimethylsulfide (DMS) emissions play important roles in atmospheric sulfur cycle and climate effects. In this study, DMS emissions were estimated by using the machine learning method and drove the global 3D chemical transport model to simulate their climate effects. To our knowledge, this is the first study in the Asian region that quantifies the combined impacts of DMS on sulfate, particle number concentration, and radiative forcings.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098,Short summary
The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys., 22, 8989–9009,Short summary
Using a global aerosol model, we find that the source contributions to radiative effects of black carbon (BC) in the Arctic are quite different from those to mass concentrations and deposition flux of BC in the Arctic. This is because microphysical properties (e.g., mixing state), altitudes, and seasonal variations of BC in the atmosphere differ among emissions sources. These differences need to be considered for accurate simulations of Arctic BC and its source contributions and climate impacts.
Sagar P. Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys., 22, 8659–8682,Short summary
Rainfall affects the distribution of surface- and groundwater resources, which are constantly declining over the Middle East and North Africa (MENA) due to overexploitation. Here, we explored the effects of dust on rainfall using WRF-Chem model simulations. Although dust is considered a nuisance from an air quality perspective, our results highlight the positive fundamental role of dust particles in modulating rainfall formation and distribution, which has implications for cloud seeding.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 22, 8343–8368,Short summary
Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958,Short summary
The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257,Short summary
Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Yuemeng Ji, Qiuju Shi, Xiaohui Ma, Lei Gao, Jiaxin Wang, Yixin Li, Yanpeng Gao, Guiying Li, Renyi Zhang, and Taicheng An
Atmos. Chem. Phys., 22, 7259–7271,Short summary
The formation mechanisms of secondary organic aerosol and brown carbon from small α-carbonyls are still unclear. Thus, the mechanisms and kinetics of aqueous-phase reactions of glyoxal were investigated using quantum chemical and kinetic rate calculations. Several essential isomeric processes were identified, including protonation to yield diol/tetrol and carbenium ions as well as nucleophilic addition of carbenium ions to diol/tetrol and free methylamine/ammonia.
Jiyuan Gao, Yang Yang, Hailong Wang, Pinya Wang, Huimin Li, Mengyun Li, Lili Ren, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 22, 7131–7142,Short summary
China has been implementing a sequence of policies for clean air since the year 2013. The aerosol decline produced a 0.09 ± 0.10°C warming during 2013–2017 estimated in this study, and the increase in ozone in the lower troposphere during this time period accelerated the warming, leading to a total 0.16 ± 0.15°C temperature increase in eastern China. Residential emission reductions led to a cooling effect because of a substantial decrease in light-absorbing aerosols.
Appel, K. W., Napelenok, S. L., Foley, K. M., Pye, H. O. T., Hogrefe, C., Luecken, D. J., Bash, J. O., Roselle, S. J., Pleim, J. E., Foroutan, H., Hutzell, W. T., Pouliot, G. A., Sarwar, G., Fahey, K. M., Gantt, B., Gilliam, R. C., Heath, N. K., Kang, D., Mathur, R., Schwede, D. B., Spero, T. L., Wong, D. C., and Young, J. O.: Description and evaluation of the Community Multiscale Air Quality (CMAQ) modeling system version 5.1, Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, 2017. a
Asmi, A., Wiedensohler, A., Laj, P., Fjaeraa, A.-M., Sellegri, K., Birmili, W., Weingartner, E., Baltensperger, U., Zdimal, V., Zikova, N., Putaud, J.-P., Marinoni, A., Tunved, P., Hansson, H.-C., Fiebig, M., Kivekäs, N., Lihavainen, H., Asmi, E., Ulevicius, V., Aalto, P. P., Swietlicki, E., Kristensson, A., Mihalopoulos, N., Kalivitis, N., Kalapov, I., Kiss, G., de Leeuw, G., Henzing, B., Harrison, R. M., Beddows, D., O'Dowd, C., Jennings, S. G., Flentje, H., Weinhold, K., Meinhardt, F., Ries, L., and Kulmala, M.: Number size distributions and seasonality of submicron particles in Europe 2008–2009, Atmos. Chem. Phys., 11, 5505–5538, https://doi.org/10.5194/acp-11-5505-2011, 2011. a
Burgos, M. A., Andrews, E., Titos, G., Benedetti, A., Bian, H., Buchard, V., Curci, G., Kipling, Z., Kirkevåg, A., Kokkola, H., Laakso, A., Letertre-Danczak, J., Lund, M. T., Matsui, H., Myhre, G., Randles, C., Schulz, M., van Noije, T., Zhang, K., Alados-Arboledas, L., Baltensperger, U., Jefferson, A., Sherman, J., Sun, J., Weingartner, E., and Zieger, P.: A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity, Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, 2020. a
Bzdek, B. R., Pennington, M. R., and Johnston, M. V.: Single particle chemical analysis of ambient ultrafine aerosol: A review, J. Aerosol Sci., 52, 109–120, 2012. a
Cappa, C. D., Onasch, T. B., Massoli, P., Worsnop, D. R., Bates, T. S., Cross, E. S., Davidovits, P., Hakala, J., Hayden, K. L., Jobson, B. T., Kolesar, K. R., Lack, D. A., Lerner, B. M., Li, S. M., Mellon, D., Nuaaman, I., Olfert, J. S., Petäjä, T., Quinn, P. K., Song, C., Subramanian, R., Williams, E. J., and Zaveri, R. A.: Radiative absorption enhancements due to the mixing state of atmospheric black carbon, Science, 337, 1078–1081, 2012. a
Cappa, C. D., Zhang, X., Russell, L. M., Collier, S., Lee, A. K. Y., Chen, C. L., Betha, R., Chen, S., Liu, J., Price, D. J., Sanchez, K. J., McMeeking, G. R., Williams, L. R., Onasch, T. B., Worsnop, D. R., Abbatt, J., and Zhang, Q.: Light absorption by ambient black and brown carbon and its dependence on black carbon coating state for two California, USA, cities in winter and summer, J. Geophys. Res.-Atmos., 124, 1550–1577, 2019. a, b
Charlson, R. J., Schwartz, S., Hales, J., Cess, R. D., Coakley, J. J., Hansen, J., and Hofmann, D.: Climate forcing by anthropogenic aerosols, Science, 255, 423–430, 1992. a
China, S., Mazzoleni, C., Gorkowski, K., Aiken, A. C., and Dubey, M. K.: Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles, Nat. Commun., 4, 1–7, 2013. a
China, S., Scarnato, B., Owen, R. C., Zhang, B., Ampadu, M. T., Kumar, S., Dzepina, K., Dziobak, M. P., Fialho, P., Perlinger, J. A., Hueber, J., Helmig, D., Mazzoleni, L. R., and Mazzoleni, C.: Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties, Geophys. Res. Lett., 42, 1243–1250, 2015. a
Corbin, J. C., Pieber, S. M., Czech, H., Zanatta, M., Jakobi, G., Massabò, D., Orasche, J., El Haddad, I., Mensah, A. A., Stengel, B., Drinovec, L., Mocnik, G., Zimmermann, R., Prévôt, A. S. H., and Gysel, M.: Brown and black carbon emitted by a marine engine operated on heavy fuel oil and distillate fuels: Optical properties, size distributions, and emission factors, J. Geophys. Res.-Atmos., 123, 6175–6195, 2018. a, b
Curci, G., Hogrefe, C., Bianconi, R., Im, U., Balzarini, A., Baró, R., Brunner, D., Forkel, R., Giordano, L., Hirtl, M., Honzak, L., Jiménez-Guerrero, P., Knote, C., Langer, M., Makar, P. A., Pirovano, G., Pérez, J. L., San José, R., Syrakov, D., Tuccella, P., Werhahn, J., Wolke, R., Žabkar, R., Zhang, J., and Galmarini, S.: Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: An AQMEII-2 perspective, Atmos. Environ., 115, 541–552, https://doi.org/10.1016/j.atmosenv.2014.09.009, 2015. a
Curtis, D. B., Meland, B., Aycibin, M., Arnold, N. P., Grassian, V. H., Young, M. A., and Kleiber, P. D.: A laboratory investigation of light scattering from representative components of mineral dust aerosol at a wavelength of 550 nm, J. Geophys. Res.-Atmos., 113, D08210, https://doi.org/10.1029/2007JD009387, 2008. a
Esteve, A. R., Highwood, E. J., Morgan, W. T., Allen, G., Coe, H., Grainger, R. G., Brown, P., and Szpek, K.: A study on the sensitivities of simulated aerosol optical properties to composition and size distribution using airborne measurements, Atmos. Environ., 89, 517–524, https://doi.org/10.1016/j.atmosenv.2014.02.063, 2014. a, b
Fast, J. D., Gustafson Jr., W. I., Easter, R. C., Zaveri, R. A., Barnard, J. C., Chapman, E. G., Grell, G. A., and Peckham, S. E.: Evolution of ozone, particulates, and aerosol direct radiative forcing in the vicinity of Houston using a fully coupled meteorology-chemistry-aerosol model, J. Geophys. Res.-Atmos., 111, D21305, https://doi.org/10.1029/2005JD006721, 2006. a
Fierce, L., Onasch, T. B., Cappa, C. D., Mazzoleni, C., China, S., Bhandari, J., Davidovits, P., Al Fischer, D., Helgestad, T., Lambe, A. T., Sedlacek, A. J., Smith, G. D., and Wolff, L.: Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition, P. Natl. Acad. Sci. USA, 117, 5196–5203, https://doi.org/10.1073/pnas.1919723117, 2020. a, b, c
Forster, P., Storelvmo, T., Armour, K., Collins, W., Dufresne, J.-L., Frame, D., Lunt, D., Mauritsen, T., Palmer, M., Watanabe, M., Wild, M., and Zhang, H.: The Earth's Energy Budget, Climate Feedbacks, and Climate Sensitivity, 923–1054, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2021. a
Healy, R. M., Riemer, N., Wenger, J. C., Murphy, M., West, M., Poulain, L., Wiedensohler, A., O'Connor, I. P., McGillicuddy, E., Sodeau, J. R., and Evans, G. J.: Single particle diversity and mixing state measurements, Atmos. Chem. Phys., 14, 6289–6299, https://doi.org/10.5194/acp-14-6289-2014, 2014. a, b, c
Hu, K., Liu, D., Tian, P., Wu, Y., Deng, Z., Wu, Y., Zhao, D., Li, R., Sheng, J., Huang, M., Ding, D., Li, W., Wang, Y., and Wu, Y.: Measurements of the diversity of shape and mixing state for ambient black carbon particles, Geophys. Res. Lett., 48, e2021GL094522, https://doi.org/10.1029/2021gl094522, 2021. a, b
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., 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, S., 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, 2009. a
Kodros, J. K., Hanna, S. J., Bertram, A. K., Leaitch, W. R., Schulz, H., Herber, A. B., Zanatta, M., Burkart, J., Willis, M. D., Abbatt, J. P. D., and Pierce, J. R.: Size-resolved mixing state of black carbon in the Canadian high Arctic and implications for simulated direct radiative effect, Atmos. Chem. Phys., 18, 11345–11361, https://doi.org/10.5194/acp-18-11345-2018, 2018. a, b
Koike, M., Moteki, N., Khatri, P., Takamura, T., Takegawa, N., Kondo, Y., Hashioka, H., Matsui, H., Shimizu, A., and Sugimoto, N.: Case study of absorption aerosol optical depth closure of black carbon over the East China Sea, J. Geophys. Res.-Atmos., 119, 122–136, 2014. a
Lanz, V. A., Prévôt, A. S. H., Alfarra, M. R., Weimer, S., Mohr, C., DeCarlo, P. F., Gianini, M. F. D., Hueglin, C., Schneider, J., Favez, O., D'Anna, B., George, C., and Baltensperger, U.: Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview, Atmos. Chem. Phys., 10, 10453–10471, https://doi.org/10.5194/acp-10-10453-2010, 2010. a
Liu, D., Whitehead, J., Alfarra, M. R., Reyes-Villegas, E., Spracklen, D. V., Reddington, C. L., Kong, S., Williams, P. I., Ting, Y. C., Haslett, S., Taylor, J. W., Flynn, M. J., Morgan, W. T., McFiggans, G., Coe, H., and Allan, J. D.: Black-carbon absorption enhancement in the atmosphere determined by particle mixing state, Nat. Geosci., 10, 184–188, https://doi.org/10.1038/ngeo2901, 2017. a
Liu, X., Easter, R. C., Ghan, S. J., Zaveri, R., Rasch, P., Shi, X., Lamarque, J.-F., Gettelman, A., Morrison, H., Vitt, F., Conley, A., Park, S., Neale, R., Hannay, C., Ekman, A. M. L., Hess, P., Mahowald, N., Collins, W., Iacono, M. J., Bretherton, C. S., Flanner, M. G., and Mitchell, D.: Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5, Geosci. Model Dev., 5, 709–739, https://doi.org/10.5194/gmd-5-709-2012, 2012. a
Luo, J., Zhang, Q., Luo, J., Liu, J., Huo, Y., and Zhang, Y.: Optical modeling of black carbon with different coating materials: The effect of coating configurations, J. Geophys. Res.-Atmos., 124, 13230–13253, 2019. a
Matsui, H.: Development of a global aerosol model using a two-dimensional sectional method: 1. Model design, J. Adv. Model. Earth Sy., 9, 1921–1947, 2017. a
Matsui, H. and Mahowald, N.: Development of a global aerosol model using a two-dimensional sectional method: 2. Evaluation and sensitivity simulations, J. Adv. Model. Earth Sy., 9, 1887–1920, 2017. a
Matsui, H., Koike, M., Kondo, Y., Moteki, N., Fast, J. D., and Zaveri, R. A.: Development and validation of a black carbon mixing state resolved three-dimensional model: Aging processes and radiative impact, J. Geophys. Res.-Atmos., 118, 2304–2326, 2013. a
Matsui, H., Hamilton, D. S., and Mahowald, N. M.: Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity, Nat. Commun., 9, 1–11, 2018. a
McKay, M. D., Beckman, R. J., and Conover, W. J.: A comparison of three methods for selecting values of input variables in the analysis of output from a computer code, Technometrics, 42, 55–61, 2000. a
Michel Flores, J., Bar-Or, R. Z., Bluvshtein, N., Abo-Riziq, A., Kostinski, A., Borrmann, S., Koren, I., Koren, I., and Rudich, Y.: Absorbing aerosols at high relative humidity: linking hygroscopic growth to optical properties, Atmos. Chem. Phys., 12, 5511–5521, https://doi.org/10.5194/acp-12-5511-2012, 2012. a
Mitchell Jr., J. M.: The effect of atmospheric aerosols on climate with special reference to temperature near the earth's surface, J. Appl. Meteorol. Clim., 10, 703–714, 1971. a
Oikawa, E., Nakajima, T., Inoue, T., and Winker, D.: A study of the shortwave direct aerosol forcing using ESSP/CALIPSO observation and GCM simulation, J. Geophys. Res.-Atmos., 118, 3687–3708, 2013. a
Riemer, N., West, M., Zaveri, R., and Easter, R.: Estimating black carbon aging time-scales with a particle-resolved aerosol model, J. Aerosol Sci., 41, 143–158, 2010. a
Rissler, J., Nordin, E. Z., Eriksson, A. C., Nilsson, P. T., Frosch, M., Sporre, M. K., Wierzbicka, A., Svenningsson, B., Löndahl, J., Messing, M. E., Sjogren, S., Hemmingsen, J. G., Loft, S., Pagels, J. H., and Swietlicki, E.: Effective density and mixing state of aerosol particles in a near-traffic urban environment, Environ. Sci. Technol., 48, 6300–6308, https://doi.org/10.1021/es5000353, 2014. a
Schell, B., Ackermann, I. J., Hass, H., Binkowski, F. S., and Ebel, A.: Modeling the formation of secondary organic aerosol within a comprehensive air quality model system, J. Geophys. Res.-Atmos., 106, 28275–28293, 2001. a
Stokes, R. and Robinson, R.: Interactions in aqueous nonelectrolyte solutions. I. Solute-solvent equilibria, J. Phys. Chem., 70, 2126–2131, 1966. a
Szopa, S., Naik, V., Adhikary, B., Artaxo, P., Berntsen, T., Collins, W., Fuzzi, S., Gallardo, L., Kiendler-Scharr, A., Klimont, Z., Liao, H., Unger, N., and Zanis, P.: Short-Lived Climate Forcers, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 817–922, 2021. a
Thornhill, G. D., Collins, W. J., Kramer, R. J., Olivié, D., Skeie, R. B., O'Connor, F. M., Abraham, N. L., Checa-Garcia, R., Bauer, S. E., Deushi, M., Emmons, L. K., Forster, P. M., Horowitz, L. W., Johnson, B., Keeble, J., Lamarque, J.-F., Michou, M., Mills, M. J., Mulcahy, J. P., Myhre, G., Nabat, P., Naik, V., Oshima, N., Schulz, M., Smith, C. J., Takemura, T., Tilmes, S., Wu, T., Zeng, G., and Zhang, J.: Effective radiative forcing from emissions of reactive gases and aerosols – a multi-model comparison, Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, 2021. a
Titos, G., Cazorla, A., Zieger, P., Andrews, E., Lyamani, H., Granados-Muñoz, M. J., Olmo, F. J., and Alados-Arboledas, L.: Effect of hygroscopic growth on the aerosol light-scattering coefficient: A review of measurements, techniques and error sources, Atmos. Environ., 141, 494–507, https://doi.org/10.1016/j.atmosenv.2016.07.021, 2016. a, b
Wang, J., Cubison, M. J., Aiken, A. C., Jimenez, J. L., and Collins, D. R.: The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols, Atmos. Chem. Phys., 10, 7267–7283, https://doi.org/10.5194/acp-10-7267-2010, 2010. a
Winker, D. M., Pelon, J., Coakley, J. A., Ackerman, S. A., Charlson, R. J., Colarco, P. R., Flamant, P., Fu, Q., Hoff, R. M., Kittaka, C., Kubar, T. L., le Treut, H., Mccormick, M. P., Mégie, G., Poole, L., Powell, K., Trepte, C., Vaughan, M. A., and Wielicki, B. A.: The CALIPSO mission: A global 3D view of aerosols and clouds, B. Am. Meteorol. Soc., 91, 1211–1230, 2010. a
Ye, Q., Gu, P., Li, H. Z., Robinson, E. S., Lipsky, E., Kaltsonoudis, C., Lee, A. K., Apte, J. S., Robinson, A. L., Sullivan, R. C., Presto, A. A., and Donahue, N. M.: Spatial variability of sources and mixing state of atmospheric particles in a metropolitan area, Environ. Sci. Technol., 52, 6807–6815, 2018. a
Yu, C., Liu, D., Broda, K., Joshi, R., Olfert, J., Sun, Y., Fu, P., Coe, H., and Allan, J. D.: Characterising mass-resolved mixing state of black carbon in Beijing using a morphology-independent measurement method, Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, 2020. a, b
Yu, H., Kaufman, Y. J., Chin, M., Feingold, G., Remer, L. A., Anderson, T. L., Balkanski, Y., Bellouin, N., Boucher, O., Christopher, S., DeCola, P., Kahn, R., Koch, D., Loeb, N., Reddy, M. S., Schulz, M., Takemura, T., and Zhou, M.: A review of measurement-based assessments of the aerosol direct radiative effect and forcing, Atmos. Chem. Phys., 6, 613–666, https://doi.org/10.5194/acp-6-613-2006, 2006. a
Zaveri, R. A. and Peters, L. K.: A new lumped structure photochemical mechanism for large-scale applications, J. Geophys. Res.-Atmos., 104, 30387–30415, 1999. a
Zaveri, R. A., Barnard, J. C., Easter, R. C., Riemer, N., and West, M.: Particle-resolved simulation of aerosol size, composition, mixing state, and the associated optical and cloud condensation nuclei activation properties in an evolving urban plume, J. Geophys. Res.-Atmos., 115, 1–19, https://doi.org/10.1029/2009JD013616, 2010. a, b, c
Zdanovskii, A.: New methods for calculating solubilities of electrolytes in multicomponent systems, Zh. Fiz. Khim, 22, 1475–1485, 1948. 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, L13801, https://doi.org/10.1029/2007gl029979, 2007. a
Zheng, Z., Curtis, J. H., Yao, Y., Gasparik, J. T., Anantharaj, V. G., Zhao, L., West, M., and Riemer, N.: Estimating submicron aerosol mixing state at the global scale with machine learning and Earth system modeling, Earth Space Sci., 8, e2020EA001500, https://doi.org/10.1029/2020EA001500, 2021. a, b
Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Investigating the impacts of aerosol mixing state on aerosol optical properties has a long...