Articles | Volume 18, issue 13
Technical note 12 Jul 2018
Technical note | 12 Jul 2018
Technical note: Updated parameterization of the reactive uptake of glyoxal and methylglyoxal by atmospheric aerosols and cloud droplets
Leah A. Curry et al.
No articles found.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536,Short summary
Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018,Short summary
The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808,Short summary
Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519,Short summary
Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Joseph L. Woo, Neha Sareen, Allison N. Schwier, and V. Faye McNeill
Atmos. Meas. Tech., 12, 3395–3402,Short summary
We present a proof-of-concept method of concentrating aerosols in a continuous stream using an applied electric field. Potential enrichment was estimated using a trajectory model, predicting values of up to 65 % for 75–200 nm aerosol, using voltages of up to 30 kV. Experimental results using similar geometry yielded up to 15 % observed enrichment for the same conditions. These results imply that aerosol enrichment using an applied electric field can be achieved in continuous-flow applications.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651,Short summary
This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Predicting gas–particle partitioning coefficients of atmospheric molecules with machine learningDevelopment of a new emission reallocation method for industrial sources in ChinaProjections of shipping emissions and the related impact on air pollution and human health in the Nordic regionA predictive model for salt nanoparticle formation using heterodimer stability calculationsUsing GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied campheneSeasonal distribution and drivers of surface fine particulate matter and organic aerosol over the Indo-Gangetic PlainIntensified modulation of winter aerosol pollution in China by El Niño with short durationForest-fire aerosol–weather feedbacks over western North America using a high-resolution, online coupled air-quality modelEstimation of secondary organic aerosol viscosity from explicit modeling of gas-phase oxidation of isoprene and α-pineneQuantitative assessment of changes in surface particulate matter concentrations and precursor emissions over China during the COVID-19 pandemic and their implications for Chinese economic activitySecondary aerosol formation from dimethyl sulfide – improved mechanistic understanding based on smog chamber experiments and modellingNon-linear response of PM2.5 to changes in NOx and NH3 emissions in the Po basin (Italy): consequences for air quality plansInsights into seasonal variation of wet deposition over southeast Asia via precipitation adjustment from the findings of MICS-Asia IIIModeling the impact of COVID-19 on air quality in southern California: implications for future control policiesResponses of Arctic black carbon and surface temperature to multi-region emission reductions: a Hemispheric Transport of Air Pollution Phase 2 (HTAP2) ensemble modeling studyNonlinear responses of particulate nitrate to NOx emission controls in the megalopolises of ChinaA Comprehensive Observational Based Multiphase Chemical Model Analysis of the Sulfur Dioxide Oxidations in both Summer and WinterAnalysis of secondary organic aerosol simulation bias in the Community Earth System Model (CESM2.1)Future evolution of aerosols and implications for climate change in the Euro-Mediterranean region using the CNRM-ALADIN63 regional climate modelSource apportionment of fine organic carbon at an urban site of Beijing using a chemical mass balance modelModeled changes in source contributions of particulate matter during the COVID-19 pandemic in the Yangtze River Delta, ChinaAerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basinAerosol radiative forcings induced by substantial changes in anthropogenic emissions in China from 2008 to 2016A study of the effect of aerosols on surface ozone through meteorology feedbacks over ChinaEvaluation and intercomparison of wildfire smoke forecasts from multiple modeling systems for the 2019 Williams Flats fireInsight into PM2.5 Sources by Applying Positive Matrix Factorization (PMF) at an Urban and Rural Site of BeijingSensitivities to biological aerosol particle properties and ageing processes: potential implications for aerosol–cloud interactions and optical propertiesFuture changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: the importance of physicochemical dependencyImproving regional air quality predictions in the Indo-Gangetic Plain – case study of an intensive pollution episode in November 2017Recommendations on benchmarks for numerical air quality model applications in China – Part 1: PM2.5 and chemical speciesGlobal modeling studies of composition and decadal trends of the Asian Tropopause Aerosol LayerComparison of chemical lateral boundary conditions for air quality predictions over the contiguous United States during pollutant intrusion eventsClimate-driven chemistry and aerosol feedbacks in CMIP6 Earth system modelsSize-resolved aerosol pH over Europe during summerInsights into the aging of biomass burning aerosol from satellite observations and 3D atmospheric modeling: evolution of the aerosol optical properties in Siberian wildfire plumesGlobal modeling of heterogeneous hydroxymethanesulfonate chemistryHow alkaline compounds control atmospheric aerosol aciditySignificant wintertime PM2.5 mitigation in the Yangtze River Delta, China, from 2016 to 2019: observational constraints on anthropogenic emission controlsHistorical and future changes in air pollutants from CMIP6 modelsEvaluating trends and seasonality in modeled PM2.5 concentrations using empirical mode decompositionLong-term observational constraints of organic aerosol dependence on inorganic species in the southeast USModel bias in simulating major chemical components of PM2.5 in ChinaAerosol pH and chemical regimes of sulfate formation in aerosol water during winter haze in the North China PlainPollutant emission reductions deliver decreased PM2.5-caused mortality across China during 2015–2017Effects of global ship emissions on European air pollution levelsTreatment of non-ideality in the SPACCIM multiphase model – Part 2: Impacts on the multiphase chemical processing in deliquesced aerosol particlesInverse modeling of fire emissions constrained by smoke plume transport using HYSPLIT dispersion model and geostationary satellite observationsComprehensive analyses of source sensitivities and apportionments of PM2.5 and ozone over Japan via multiple numerical techniquesNumerical analysis of agricultural emissions impacts on PM2.5 in China using a high-resolution ammonia emission inventoryClimate and air quality impacts due to mitigation of non-methane near-term climate forcers
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246,Short summary
The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Yun Fat Lam, Chi Chiu Cheung, Xuguo Zhang, Joshua S. Fu, and Jimmy Chi Hung Fung
Atmos. Chem. Phys., 21, 12895–12908,Short summary
In recent years, air pollution forecasting has become an important municipal service of the government. In this study, a new spatial allocation method based on satellite remote sensing and GIS techniques was developed to address the spatial deficiency of industrial source emissions in China, providing a substantial improvement on NO2 and PM2.5 forecast for the Pearl River Delta/Greater Bay Area.
Camilla Geels, Morten Winther, Camilla Andersson, Jukka-Pekka Jalkanen, Jørgen Brandt, Lise M. Frohn, Ulas Im, Wing Leung, and Jesper H. Christensen
Atmos. Chem. Phys., 21, 12495–12519,Short summary
In this study, we set up new shipping emissions scenarios and use two chemistry transport models and a health assessment model to assess the development of air quality and related health impacts in the Nordic region. Shipping alone is associated with about 850 premature deaths during present-day conditions, decreasing to approximately 550–600 cases in the 2050 scenarios.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys., 21, 11637–11654,Short summary
We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487,Short summary
This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
Caterina Mogno, Paul I. Palmer, Christoph Knote, Fei Yao, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 10881–10909,Short summary
We use a 3-D atmospheric chemistry model to investigate how seasonal emissions sources and meteorological conditions affect the surface distribution of fine particulate matter (PM2.5) and organic aerosol (OA) over the Indo-Gangetic Plain. We find that all seasonal mean values of PM2.5 still exceed safe air quality levels, with human emissions contributing to PM2.5 all year round, open fires during post- and pre-monsoon, and biogenic emissions during monsoon. OA contributes up to 30 % to PM2.5.
Liangying Zeng, Yang Yang, Hailong Wang, Jing Wang, Jing Li, Lili Ren, Huimin Li, Yang Zhou, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 21, 10745–10761,Short summary
Using an aerosol–climate model, the impacts of El Niño with different durations on aerosols in China are examined. The modulation on aerosol concentrations and haze days by short-duration El Niño events is 2–3 times more than that by long-duration El Niño events in China. The frequency of short-duration El Niño has been increasing significantly in recent decades, suggesting that El Niño events have exerted increasingly intense modulation on aerosol pollution in China over the past few decades.
Paul A. Makar, Ayodeji Akingunola, Jack Chen, Balbir Pabla, Wanmin Gong, Craig Stroud, Christopher Sioris, Kerry Anderson, Philip Cheung, Junhua Zhang, and Jason Milbrandt
Atmos. Chem. Phys., 21, 10557–10587,Short summary
We have examined the effects of airborne particles on absorption and scattering of incoming sunlight by the particles themselves via cloud formation. We used an advanced, combined high-resolution weather forecast and chemical transport computer model, for western North America, and simulations with and without the connections between particles and weather enabled. Feedbacks improved weather and air pollution forecasts and changed cloud behaviour and forest-fire pollutant amount and height.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213,Short summary
We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Hyun Cheol Kim, Soontae Kim, Mark Cohen, Changhan Bae, Dasom Lee, Rick Saylor, Minah Bae, Eunhye Kim, Byeong-Uk Kim, Jin-Ho Yoon, and Ariel Stein
Atmos. Chem. Phys., 21, 10065–10080,Short summary
Global outbreaks of COVID-19 offer rare opportunities of natural experiments in emission control and corresponding responses of tropospheric chemistry. This study's novel approach investigates (1) isolating the pandemic's impact from natural and anthropogenic variations, (2) emission adjustment to reproduce real-time emissions, and (3) brute-force modeling to investigate Chinese economic activities. Results provide characteristics of the region's chemistry and emissions.
Robin Wollesen de Jonge, Jonas Elm, Bernadette Rosati, Sigurd Christiansen, Noora Hyttinen, Dana Lüdemann, Merete Bilde, and Pontus Roldin
Atmos. Chem. Phys., 21, 9955–9976,Short summary
This study presents a detailed analysis of the OH-initiated oxidation of dimethyl sulfide (DMS) based on experiments performed in the Aarhus University Research on Aerosol (AURA) smog chamber and the gas- and particle-phase chemistry kinetic multilayer model (ADCHAM). We capture the formation, growth and chemical composition of aerosols in the chamber setup by an improved multiphase oxidation mechanism and utilize our results to reproduce the important role of DMS in the marine boundary layer.
Philippe Thunis, Alain Clappier, Matthias Beekmann, Jean Philippe Putaud, Cornelis Cuvelier, Jessie Madrazo, and Alexander de Meij
Atmos. Chem. Phys., 21, 9309–9327,Short summary
Modelling simulations are used to identify the most efficient emission reduction strategies to reduce PM2.5 concentration levels in northern Italy. Results show contrasting chemical regimes and important non-linearities during wintertime, with the striking result that PM2.5 levels may increase when NOx reductions are applied in NOx-rich areas – a process that may have contributed to the absence of significant PM2.5 decrease during the COVID-19 lockdowns in many European cities.
Syuichi Itahashi, Baozhu Ge, Keiichi Sato, Zhe Wang, Junichi Kurokawa, Jiani Tan, Kan Huang, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 21, 8709–8734,Short summary
This study presents the detailed analysis of acid deposition over southeast Asia based on the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Simulated wet deposition is evaluated with observation data from the Acid Deposition Monitoring Network in East Asia (EANET). The difficulties of models to capture observations are related to the model performance on precipitation. The precipitation-adjusted approach was applied, and the distribution of wet deposition was successfully revised.
Zhe Jiang, Hongrong Shi, Bin Zhao, Yu Gu, Yifang Zhu, Kazuyuki Miyazaki, Xin Lu, Yuqiang Zhang, Kevin W. Bowman, Takashi Sekiya, and Kuo-Nan Liou
Atmos. Chem. Phys., 21, 8693–8708,Short summary
We use the COVID-19 pandemic as a unique natural experiment to obtain a more robust understanding of the effectiveness of emission reductions toward air quality improvement by combining chemical transport simulations and observations. Our findings imply a shift from current control policies in California: a strengthened control on primary PM2.5 emissions and a well-balanced control on NOx and volatile organic compounds are needed to effectively and sustainably alleviate PM2.5 and O3 pollution.
Na Zhao, Xinyi Dong, Kan Huang, Joshua S. Fu, Marianne Tronstad Lund, Kengo Sudo, Daven Henze, Tom Kucsera, Yun Fat Lam, Mian Chin, and Simone Tilmes
Atmos. Chem. Phys., 21, 8637–8654,Short summary
Black carbon acts as a strong climate forcer, especially in vulnerable pristine regions such as the Arctic. This work utilizes ensemble modeling results from the task force Hemispheric Transport of Air Pollution Phase 2 to investigate the responses of Arctic black carbon and surface temperature to various source emission reductions. East Asia contributed the most to Arctic black carbon. The response of Arctic temperature to black carbon was substantially more sensitive than the global average.
Mengmeng Li, Zihan Zhang, Tijian Wang, Min Xie, Shu Li, Bingliang Zhuang, and Yong Han
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Nitrate production is related to the abundance of both NOx and atmospheric oxidants. We establish the nonlinear responses between nitrate and NOx in China. Reduction of NOx results in linearly lower nitrate in summer-autumn, whereas an increase of winter nitrate until an inflexion point appears at 40–50 reduction. Such nonlinear nitrate-NOx responses can be explained by the excess oxidants under lower NOx emissions. This paper helps understand the nonlinear aerosol and photochemistry feedback.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Secondary sulfate aerosol is an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Yaman Liu, Xinyi Dong, Minghuai Wang, Louisa K. Emmons, Yawen Liu, Yuan Liang, Xiao Li, and Manish Shrivastava
Atmos. Chem. Phys., 21, 8003–8021,Short summary
Secondary organic aerosol (SOA) is considered one of the most important uncertainties in climate modeling. We evaluate SOA performance in the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 with chemistry (CAM6-Chem) through a long-term simulation (1988–2019) with observations in the United States, which indicates monoterpene-formed SOA contributes most to the overestimation of SOA at the surface and underestimation in the upper air.
Thomas Drugé, Pierre Nabat, Marc Mallet, and Samuel Somot
Atmos. Chem. Phys., 21, 7639–7669,Short summary
This study presents the surface mass concentration and AOD evolution of various aerosols over the Euro-Mediterranean region between the end of the 20th century and the mid-21st century. This study also describes the part of the expected climate change over the Euro-Mediterranean region that can be explained by the evolution of these different aerosols.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341,Short summary
Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Jinlong Ma, Juanyong Shen, Peng Wang, Shengqiang Zhu, Yu Wang, Pengfei Wang, Gehui Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 21, 7343–7355,Short summary
Due to the reduced anthropogenic emissions during the COVID-19 lockdown, mainly from the transportation and industrial sectors, PM2.5 decreased significantly in the whole Yangtze River Delta (YRD) and its major cities. However, the contributions and relative importance of different source sectors and regions changed differently, indicating that control strategies should be adjusted accordingly for further pollution control.
Janaína P. Nascimento, Megan M. Bela, Bruno B. Meller, Alessandro L. Banducci, Luciana V. Rizzo, Angel Liduvino Vara-Vela, Henrique M. J. Barbosa, Helber Gomes, Sameh A. A. Rafee, Marco A. Franco, Samara Carbone, Glauber G. Cirino, Rodrigo A. F. Souza, Stuart A. McKeen, and Paulo Artaxo
Atmos. Chem. Phys., 21, 6755–6779,
Mingxu Liu and Hitoshi Matsui
Atmos. Chem. Phys., 21, 5965–5982,Short summary
By integrating an advanced global climate model with the latest anthropogenic emission inventory, we quantify the aerosol perturbations to regional radiative budgets due to the changes in anthropogenic emissions in China from 2008–2016. We find that aerosol–radiation interactions lead to a relatively small net radiative forcing at the top of the atmosphere but contribute largely to surface brightening in China over the past few decades.
Yawei Qu, Apostolos Voulgarakis, Tijian Wang, Matthew Kasoar, Chris Wells, Cheng Yuan, Sunil Varma, and Laura Mansfield
Atmos. Chem. Phys., 21, 5705–5718,Short summary
The meteorological effect of aerosols on tropospheric ozone is investigated using global atmospheric modelling. We found that aerosol-induced meteorological effects act to reduce modelled ozone concentrations over China, which brings the simulation closer to observed levels. Our work sheds light on understudied processes affecting the levels of tropospheric gaseous pollutants and provides a basis for evaluating such processes using a combination of observations and model sensitivity experiments.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David Giles, and Pablo E. Saide
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of twelve real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles, for improving smoke forecasts.
Deepchandra Srivastava, Jingsha Xu, Tuan V. Vu, Di Liu, Linjie Li, Pingqing Fu, Siqi Hou, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study presents the source apportionment of PM2.5 performed by PMF at an urban and a rural site in Beijing. These factors are interpreted to be traffic emissions, biomass burning, road dust, soil dust, coal combustion, oil combustion and secondary inorganics. The PMF failed to resolve some sources identified by CMB and AMS, and appears to overestimate the dust sources. A comparison with earlier PMF studies from the Beijing area highlights inconsistent findings using this method.
Minghui Zhang, Amina Khaled, Pierre Amato, Anne-Marie Delort, and Barbara Ervens
Atmos. Chem. Phys., 21, 3699–3724,Short summary
Although primary biological aerosol particles (PBAPs, bioaerosols) represent a small fraction of total atmospheric aerosol burden, they might affect climate and public health. We summarize which PBAP properties are important to affect their inclusion in clouds and interaction with light and might also affect their residence time and transport in the atmosphere. Our study highlights that not only chemical and physical but also biological processes can modify these physicochemical properties.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425,Short summary
Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Behrooz Roozitalab, Gregory R. Carmichael, and Sarath K. Guttikunda
Atmos. Chem. Phys., 21, 2837–2860,Short summary
We used air quality modeling to study an extreme pollution episode in November 2017 in India. We found both local and regional emissions contribute to high pollution levels. The extreme pollution values were the result of agricultural fires in the northwest of India. Ozone should be considered in future air quality management strategies.
Ling Huang, Yonghui Zhu, Hehe Zhai, Shuhui Xue, Tianyi Zhu, Yun Shao, Ziyi Liu, Chris Emery, Greg Yarwood, Yangjun Wang, Joshua Fu, Kun Zhang, and Li Li
Atmos. Chem. Phys., 21, 2725–2743,Short summary
Numerical air quality models (AQMs) are being applied extensively to address diverse scientific and regulatory compliance associated with deteriorating air quality in China. For any AQM applications, model performance evaluation is a critical step that guarantees the robustness and reliability of the baseline modeling results and subsequent applications. We provided benchmarks for model performance evaluation of AQM applications in China to demonstrate model robustness.
Adriana Bossolasco, Fabrice Jegou, Pasquale Sellitto, Gwenaël Berthet, Corinna Kloss, and Bernard Legras
Atmos. Chem. Phys., 21, 2745–2764,Short summary
Using the Community Earth System Model, we simulate the surface aerosols lifted to the Asian tropopause (the ATAL layer), its composition and trend, covering a long-term period (2000–2015). We identify a
double-peakaerosol vertical profile that we attribute to
convectivecloud-borne aerosols. We find that natural aerosol (mineral dust) is the dominant aerosol type and has no long-term trend. ATAL's anthropogenic fraction, by contrast, shows a marked positive trend.
Youhua Tang, Huisheng Bian, Zhining Tao, Luke D. Oman, Daniel Tong, Pius Lee, Patrick C. Campbell, Barry Baker, Cheng-Hsuan Lu, Li Pan, Jun Wang, Jeffery McQueen, and Ivanka Stajner
Atmos. Chem. Phys., 21, 2527–2550,Short summary
Chemical lateral boundary condition (CLBC) impact is essential for regional air quality prediction during intrusion events. We present a model mapping Goddard Earth Observing System (GEOS) to Community Multi-scale Air Quality (CMAQ) CB05–AERO6 (Carbon Bond 5; version 6 of the aerosol module) species. Influence depends on distance from the inflow boundary and species and their regional characteristics. We use aerosol optical thickness to derive CLBCs, achieving reasonable prediction.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126,Short summary
We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811,Short summary
The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, and Meinrat O. Andreae
Atmos. Chem. Phys., 21, 357–392,Short summary
A lack of consistent observational constraints on the atmospheric evolution of the optical properties of biomass burning (BB) aerosol limits the accuracy of assessments of the aerosol radiative and climate effects. We show that useful insights into the evolution of the BB aerosol optical properties can be inferred from a combination of satellite observations and 3D modeling. We report major changes that occurred in the optical properties of Siberian BB aerosol during its long-range transport.
Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy
Atmos. Chem. Phys., 21, 457–481,Short summary
We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys. Discuss.,
Revised manuscript under review for ACPShort summary
Aerosol pH is well-buffered by alkaline compounds, notably NH3 and in some areas crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid that aerosols become highly acidic with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds and climate (aerosol hygroscopicity).
Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Khalid Mehmood, Weiping Liu, Tianfeng Chai, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14787–14800,Short summary
The Chinese government has made major strides in curbing anthropogenic emissions. In this study, we constrain a state-of-the-art CTM by a reliable data assimilation method with extensive chemical and meteorological observations. This comprehensive technical design provides a crucial advance in isolating the influences of emission changes and meteorological perturbations over the Yangtze River Delta (YRD) from 2016 to 2019, thus establishing the first map of the PM2.5 mitigation across the YRD.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579,Short summary
A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Huiying Luo, Marina Astitha, Christian Hogrefe, Rohit Mathur, and S. Trivikrama Rao
Atmos. Chem. Phys., 20, 13801–13815,Short summary
A new method is introduced to evaluate nonlinear, nonstationary modeled PM2.5 time series by decomposing decadal PM2.5 concentrations and its species onto various timescales. It does not require preselection of temporal scales and assumptions of linearity and stationarity. It provides a unique opportunity to assess the influence of each species on total PM2.5. The results reveal a phase shift in modeled EC/OC concentrations, indicating the need for improved model treatment of organic aerosols.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107,Short summary
This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284,Short summary
In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
Wei Tao, Hang Su, Guangjie Zheng, Jiandong Wang, Chao Wei, Lixia Liu, Nan Ma, Meng Li, Qiang Zhang, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 20, 11729–11746,Short summary
We simulated the thermodynamic and multiphase reactions in aerosol water during a wintertime haze event over the North China Plain. It was found that aerosol pH exhibited a strong spatiotemporal variability, and multiple oxidation pathways were predominant for particulate sulfate formation in different locations. Sensitivity tests further showed that ammonia, crustal particles, and dissolved transition metal ions were important factors for multiphase chemistry during haze episodes.
Ben Silver, Luke Conibear, Carly L. Reddington, Christoph Knote, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 20, 11683–11695,Short summary
China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
Jan Eiof Jonson, Michael Gauss, Michael Schulz, Jukka-Pekka Jalkanen, and Hilde Fagerli
Atmos. Chem. Phys., 20, 11399–11422,Short summary
We have calculated the effects of air pollution in Europe from shipping on levels of PM2.5 and ozone and depositions of oxidised nitrogen and sulfur from individual sea areas and from all global shipping. Model results are shown for Europe as a whole but also focusing on select, mainly coastal, countries. Calculations are made using 2017 emissions supplemented by calculations reducing sulfur emissions from ships by about 80 % following the implementation of the 2020 global sulfur cap.
Ahmad Jhony Rusumdar, Andreas Tilgner, Ralf Wolke, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 10351–10377,Short summary
In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are performed. The investigations aim at assessing the impact of a detailed treatment of non-ideality in multiphase models dealing with aqueous aerosol chemistry. The model studies demonstrate that the inclusion of non-ideality considerably affects the multiphase chemical processing of transition metal ions, oxidants, and related chemical subsystems such as organic chemistry in aqueous aerosols.
Hyun Cheol Kim, Tianfeng Chai, Ariel Stein, and Shobha Kondragunta
Atmos. Chem. Phys., 20, 10259–10277,Short summary
Smoke forecasts have been challenged by high uncertainty in fire emission estimates. We develop an inverse modeling system, the HYSPLIT-based Emissions Inverse Modeling System for wildfires, that estimates wildfire emissions from the transport and dispersion of smoke plumes as measured by satellite observations. Using NOAA HYSPLIT and GOES Aerosol/Smoke Product (GASP), the system resolves smoke source strength as a function of time and vertical level and outperforms current operational system.
Satoru Chatani, Hikari Shimadera, Syuichi Itahashi, and Kazuyo Yamaji
Atmos. Chem. Phys., 20, 10311–10329,Short summary
Source sensitivities and apportionments of PM2.5 and ozone concentrations over Japan for 2016 were evaluated using multiple numerical techniques including BFM, HDDM, and ISAM, embedded in regional chemical transport models. Influences of stringent emission controls recently implemented in Asian countries were reflected. Differences between sensitivities and apportionments greatly helped distinguish various direct and indirect effects of emission sources on PM2.5 and ozone concentrations.
Xiao Han, Lingyun Zhu, Mingxu Liu, Yu Song, and Meigen Zhang
Atmos. Chem. Phys., 20, 9979–9996,Short summary
China is one of the largest agricultural countries in the world. Some of the major PM2.5 particles that cause the atmospheric haze and impact the climate change were converted from agricultural NH3 emission. This paper applied the numerical modeling system, coupled with a high-resolution agricultural NH3 emissions inventory, to investigate the contribution of agricultural NH3 to PM2.5 mass burden in China and obtained some interesting results.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663,
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We have developed a new parameterization of the reactive uptake of glyoxal and methylglyoxal by atmospheric aerosols and cloud droplets. Our calculations take into account newly available information regarding the gas–particle partitioning of these species and their chemical processing in the aerosol phase. We expect application of these parameterizations will result in improved representation of aqueous secondary organic aerosol formation in atmospheric chemistry models.
We have developed a new parameterization of the reactive uptake of glyoxal and methylglyoxal by...