Articles | Volume 17, issue 21
https://doi.org/10.5194/acp-17-13187-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-13187-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
08 Nov 2017
Research article |
| 08 Nov 2017
Kinetic modeling studies of SOA formation from α-pinene ozonolysis
Kathrin Gatzsche
CORRESPONDING AUTHOR
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
Yoshiteru Iinuma
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
now at: Okinawa Institute of Science and Technology Graduate University (OIST), Okinawa, Japan
Andreas Tilgner
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
Anke Mutzel
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
Torsten Berndt
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
Ralf Wolke
Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
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Rocío Baró, Laura Palacios-Peña, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
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Carlo Bozzetti, Imad El Haddad, Dalia Salameh, Kaspar Rudolf Daellenbach, Paola Fermo, Raquel Gonzalez, María Cruz Minguillón, Yoshiteru Iinuma, Laurent Poulain, Miriam Elser, Emanuel Müller, Jay Gates Slowik, Jean-Luc Jaffrezo, Urs Baltensperger, Nicolas Marchand, and André Stephan Henry Prévôt
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Sudhakar Dipu, Johannes Quaas, Ralf Wolke, Jens Stoll, Andreas Mühlbauer, Odran Sourdeval, Marc Salzmann, Bernd Heinold, and Ina Tegen
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Maria Rodigast, Anke Mutzel, and Hartmut Herrmann
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James W. Grayson, Yue Zhang, Anke Mutzel, Lindsay Renbaum-Wolff, Olaf Böge, Saeid Kamal, Hartmut Herrmann, Scot T. Martin, and Allan K. Bertram
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Yan Lv, Xiang Li, Ting Ting Xu, Tian Tao Cheng, Xin Yang, Jian Min Chen, Yoshiteru Iinuma, and Hartmut Herrmann
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Maria Rodigast, Anke Mutzel, Janine Schindelka, and Hartmut Herrmann
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Ying Chen, Ya-Fang Cheng, Stephan Nordmann, Wolfram Birmili, Hugo A. C. Denier van der Gon, Nan Ma, Ralf Wolke, Birgit Wehner, Jia Sun, Gerald Spindler, Qing Mu, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
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A. J. Rusumdar, R. Wolke, A. Tilgner, and H. Herrmann
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K. W. Fomba, D. van Pinxteren, K. Müller, Y. Iinuma, T. Lee, J. L. Collett Jr., and H. Herrmann
Atmos. Chem. Phys., 15, 8751–8765, https://doi.org/10.5194/acp-15-8751-2015, https://doi.org/10.5194/acp-15-8751-2015, 2015
M. Rodigast, A. Mutzel, Y. Iinuma, S. Haferkorn, and H. Herrmann
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L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
K. E. Yttri, J. Schnelle-Kreis, W. Maenhaut, G. Abbaszade, C. Alves, A. Bjerke, N. Bonnier, R. Bossi, M. Claeys, C. Dye, M. Evtyugina, D. García-Gacio, R. Hillamo, A. Hoffer, M. Hyder, Y. Iinuma, J.-L. Jaffrezo, A. Kasper-Giebl, G. Kiss, P. L. López-Mahia, C. Pio, C. Piot, C. Ramirez-Santa-Cruz, J. Sciare, K. Teinilä, R. Vermeylen, A. Vicente, and R. Zimmermann
Atmos. Meas. Tech., 8, 125–147, https://doi.org/10.5194/amt-8-125-2015, https://doi.org/10.5194/amt-8-125-2015, 2015
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128, https://doi.org/10.5194/acp-14-9105-2014, https://doi.org/10.5194/acp-14-9105-2014, 2014
T. Berndt, M. Sipilä, F. Stratmann, T. Petäjä, J. Vanhanen, J. Mikkilä, J. Patokoski, R. Taipale, R. L. Mauldin III, and M. Kulmala
Atmos. Chem. Phys., 14, 751–764, https://doi.org/10.5194/acp-14-751-2014, https://doi.org/10.5194/acp-14-751-2014, 2014
A. Kahnt, Y. Iinuma, A. Mutzel, O. Böge, M. Claeys, and H. Herrmann
Atmos. Chem. Phys., 14, 719–736, https://doi.org/10.5194/acp-14-719-2014, https://doi.org/10.5194/acp-14-719-2014, 2014
S. Barthel, I. Tegen, R. Wolke, and M. van Pinxteren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-377-2014, https://doi.org/10.5194/acpd-14-377-2014, 2014
Revised manuscript not accepted
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Weakened aerosol-radiation interaction exacerbating ozone pollution in eastern China since China’s clean air actions
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Reaction of SO3 with H2SO4 and Its Implication for Aerosol Particle Formation in the Gas Phase and at the Air-Water Interface
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
Anthropogenic amplification of biogenic secondary organic aerosol production
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling
Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts
Assessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of China
Impact of Landes forest fires on air quality in France during the 2022 summer
Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach
Comprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional model
Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019
Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
Modelling wintertime sea-spray aerosols under Arctic haze conditions
Impact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China
Simulation of organic aerosol, its precursors, and related oxidants in the Landes pine forest in southwestern France: accounting for domain-specific land use and physical conditions
Modelling the European wind-blown dust emissions and their impact on particulate matter (PM) concentrations
Impacts of estimated plume rise on PM2.5 exceedance prediction during extreme wildfire events: a comparison of three schemes (Briggs, Freitas, and Sofiev)
Strong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon Basin
Sources of organic aerosols in eastern China: a modeling study with high-resolution intermediate-volatility and semivolatile organic compound emissions
Composited analyses of the chemical and physical characteristics of co-polluted days by ozone and PM2.5 over 2013–2020 in the Beijing–Tianjin–Hebei region
Observation-based constraints on modeled aerosol surface area: implications for heterogeneous chemistry
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
EGUsphere, https://doi.org/10.5194/egusphere-2023-2393, https://doi.org/10.5194/egusphere-2023-2393, 2023
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The present study quantifies the response of aerosol-radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the mainly focus on the contribution to changed O3 concentrations over eastern China both in summer and winter by using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb) averaged over eastern China.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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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 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. 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.
Rui Wang, Yang Cheng, Yue Hu, Shasha Chen, Xiaokai Guo, Fengmin Song, Hao Li, and Tianlei Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2009, https://doi.org/10.5194/egusphere-2023-2009, 2023
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We employed QC calculations, BOMD simulations and ACDC kinetic model to characterize the SO3-H2SO4 interaction in the gas phase and at the air-water interface and to study the effect of H2S2O7 on H2SO4-NH3-based clusters. The present work will expand our understanding of new pathway for the loss of SO3 in acidic polluted areas, and help to reveal some missing sources of metropolis industrial regions NPF and to understand the atmospheric organic-sulfur cycle more comprehensively.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
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., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
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The 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. An analysis of the 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.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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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 chemical transport models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
EGUsphere, https://doi.org/10.5194/egusphere-2023-1919, https://doi.org/10.5194/egusphere-2023-1919, 2023
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The presented study deals with the attribution of particulate matter (PM) concentrations to anthropogenic emissions over Central Europe using regional scale models. It calculates the present-day contributions of different emissions sectors to urban concentrations of PM and their secondary components. Moreover, the study investigates the effect of chemical non-linearities by using multiple methods of source attribution and calculation of secondary organic aerosol.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
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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, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
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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, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
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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, https://doi.org/10.5194/acp-23-8623-2023, https://doi.org/10.5194/acp-23-8623-2023, 2023
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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, https://doi.org/10.5194/acp-23-8021-2023, https://doi.org/10.5194/acp-23-8021-2023, 2023
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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, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
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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, https://doi.org/10.5194/acp-23-7091-2023, https://doi.org/10.5194/acp-23-7091-2023, 2023
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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, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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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, https://doi.org/10.5194/acp-23-6647-2023, https://doi.org/10.5194/acp-23-6647-2023, 2023
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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, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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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, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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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, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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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, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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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.
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, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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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.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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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, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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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, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
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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, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
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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, https://doi.org/10.5194/acp-23-3679-2023, https://doi.org/10.5194/acp-23-3679-2023, 2023
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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.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys., 23, 3629–3654, https://doi.org/10.5194/acp-23-3629-2023, https://doi.org/10.5194/acp-23-3629-2023, 2023
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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.
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, https://doi.org/10.5194/acp-23-3083-2023, https://doi.org/10.5194/acp-23-3083-2023, 2023
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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.
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, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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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, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
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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, https://doi.org/10.5194/acp-23-23-2023, https://doi.org/10.5194/acp-23-23-2023, 2023
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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, https://doi.org/10.5194/acp-22-15449-2022, https://doi.org/10.5194/acp-22-15449-2022, 2022
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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.
Cited articles
Abramson, E., Imre, D., Beranek, J., Wilson, J., and Zelenyuk, A.: Experimental determination of chemical diffusion within secondary organic aerosol particles, Phys. Chem. Chem. Phys., 15, 2983–2991, https://doi.org/10.1039/c2cp44013j, 2013.
Andreae, M. O. and Crutzen, P. J.: Atmospheric Aerosols: Biogeochemical Sources and Role in Atmospheric Chemistry, Science, 276, 1052–1058, https://doi.org/10.1126/science.276.5315.1052, 1997.
Antonovskii, V. L. and Terent'ev, V. A.: Effect of the Structure of Hydroperoxides and Some Aldehydes on the Kinetics of the Noncatalytic Formation of α-Hydroxy Peroxides, Zhurnal Organicheskoi Khimii, 3, 1011–1015, 1967.
Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions-Part 1: aldehydes and ketones, Atmos. Environ., 38, 4371–4382, https://doi.org/10.1016/j.atmosenv.2004.03.035, 2004.
Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions-Part 3: Carboxylic and dicarboxylic acids, Atmos. Environ., 40, 6676–6686, https://doi.org/10.1016/j.atmosenv.2006.03.013, 2006.
Berndt, T., Böge, O., and Stratmann, F.: Gas-phase ozonolysis of α-pinene: gaseous products and particle formation, Atmos. Environ., 37, 3933–3945, https://doi.org/10.1016/S1352-2310(03)00501-6, 2003.
Berndt, T., Richters, S., Jokinen, T., Hyttinen, N., Kurtén, T., Otkjær, R. V., Kjaergaard, H. G., Stratmann, F., Herrmann, H., Sipilä, M., Kulmala, M., and Ehn, M.: Hydroxyl radical-induced formation of highly oxidized organic compounds, Nat. Commun., 7, 13677, https://doi.org/10.1038/ncomms13677, 2016.
Cappa, C. D. and Wilson, K. R.: Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior, Atmos. Chem. Phys., 11, 1895–1911, https://doi.org/10.5194/acp-11-1895-2011, 2011.
Carey, F. and Sundberg, R.: Advanced Organic Chemistry, Part A. Structure and Mechanisms, 5th Edn., Springer US, https://doi.org/10.1007/978-0-387-44899-2, 2007.
Carslaw, H. S. and Jaeger, J. C.: Conduction of Heat in Solids, 2nd Edn., Clarendon Press, Oxford, 1959.
Casale, M. T., Richman, A. R., Elrod, M. J., Garland, R. M., Beaver, M. R., and Tolbert, M. A.: Kinetics of acid-catalyzed aldol condensation reactions of aliphatic aldehydes, Atmos. Environ., 41, 6212–6224, https://doi.org/10.1016/j.atmosenv.2007.04.002, 2007.
Champion, D., Hervet, H., Blond, G., Meste, M. L., and Simatos, D.: Translational Diffusion in Sucrose Solutions in the Vicinity of Their Glass Transition Temperature, J. Phys. Chem. B, 101, 10674–10679, https://doi.org/10.1021/jp971899i, 1997.
Chen, J. and Griffin, R. J.: Modeling secondary organic aerosol formation from oxidation of α-pinene, β-pinene, and d-limonene, Atmos. Environ., 39, 7731–7744, https://doi.org/10.1016/j.atmosenv.2005.05.049, 2005.
Compernolle, S., Ceulemans, K., and Müller, J.-F.: EVAPORATION: a new vapour pressure estimation method for organic molecules including non-additivity and intramolecular interactions, Atmos. Chem. Phys., 11, 9431–9450, https://doi.org/10.5194/acp-11-9431-2011, 2011.
Crank, J.: The Mathematics of Diffusion, 2nd Edn., Oxford University Press Inc., New York, https://doi.org/10.1088/0031-9112/26/11/044, 1975.
Cussler, E. L.: Diffusion: mass transfer in fluid systems, 3rd Edn., Cambridge University Press, https://doi.org/10.1017/cbo9780511805134, 2009.
Danckwarts, P. V.: Absorption and simultaneous diffusion and chemical reaction into particles of various shapes and into falling drops, T. Faraday Soc., 1014–1023, https://doi.org/10.1039/tf9514701014, 1951.
DePalma, J. W., Horan, A. J., Hall IV, W. A., and Johnston, M. V.: Thermodynamics of oligomer formation: implications for secondary organic aerosol formation and reactivity, Phys. Chem. Chem. Phys., 15, 6935–6944, https://doi.org/10.1039/C3CP44586K, 2013.
Docherty, K. S., Wu, W., Lim, Y. B., and Ziemann, P. J.: Contributions of Organic Peroxides to Secondary Aerosol Formed from Reactions of Monoterpenes with O3, Environ. Sci. Technol., 39, 4049–4059, https://doi.org/10.1021/es050228s, 2005.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012.
Donahue, N. M., Ortega, I. K., Chuang, W., Riipinen, I., Riccobono, F., Schobesberger, S., Dommen, J., Baltensperger, U., Kulmala, M., Worsnop, D. R., and Vehkamaki, H.: How do organic vapors contribute to new-particle formation?, Faraday Discuss., 165, 91–104, https://doi.org/10.1039/C3FD00046J, 2013.
Eckert, F. and Klamt, A.: Fast solvent screening via quantum chemistry: COSMO-RS approach, AIChE Journal, 48, 369–385, https://doi.org/10.1002/aic.690480220, 2002.
Ehn, M., Kleist, E., Junninen, H., Petäjä, T., Lönn, G., Schobesberger, S., Dal Maso, M., Trimborn, A., Kulmala, M., Worsnop, D. R., Wahner, A., Wildt, J., and Mentel, T. F.: Gas phase formation of extremely oxidized pinene reaction products in chamber and ambient air, Atmos. Chem. Phys., 12, 5113–5127, https://doi.org/10.5194/acp-12-5113-2012, 2012.
Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurtén, T., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., Canagaratna, M., Maso, M. D., Berndt, T., Petäjä, T., Wahner, A., Kerminen, V.-M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.: A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Einstein, A.: Investigations on the Theory of Brownian Motion, Dover, New York, 1956.
Ervens, B., Feingold, G., Clegg, S. L., and Kreidenweis, S. M.: A modeling study of aqueous production of dicarboxylic acids: 2. Implications for cloud microphysics, J. Geophys. Res.-Atmos., 109, D15, https://doi.org/10.1029/2004JD004575, 2004.
Ervens, B., Feingold, G., and Kreidenweis, S. M.: Influence of water-soluble organic carbon on cloud drop number concentration, J. Geophys. Res.-Atmos., 110, D18, https://doi.org/10.1029/2004JD005634, 2005.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011.
Facchini, M. C., Mircea, M., Fuzzi, S., and Charlson, R. J.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 40, 257–259, https://doi.org/10.1038/45758, 1999.
Fuchs, N. and Sutugin, A.: HIGH-DISPERSED AEROSOLS, in: Topics in Current Aerosol Research, edited by: Hidy, G. and Brock, J., International Reviews in Aerosol Physics and Chemistry, Pergamon, https://doi.org/10.1016/B978-0-08-016674-2.50006-6, 1971.
Goldstein, A. H. and Galbally, I. E.: Known and Unexplored Organic Constituents in the Earth's Atmosphere, Environ. Sci. Technol., 41, 1514–1521, https://doi.org/10.1021/es072476p, 2007.
Grayson, J. W., Song, M., Sellier, M., and Bertram, A. K.: Validation of the poke-flow technique combined with simulations of fluid flow for determining viscosities in samples with small volumes and high viscosities, Atmos. Meas. Tech., 8, 2463–2472, https://doi.org/10.5194/amt-8-2463-2015, 2015.
Grayson, J. W., Zhang, Y., Mutzel, A., Renbaum-Wolff, L., Böge, O., Kamal, S., Herrmann, H., Martin, S. T., and Bertram, A. K.: Effect of varying experimental conditions on the viscosity of α-pinene derived secondary organic material, Atmos. Chem. Phys., 16, 6027–6040, https://doi.org/10.5194/acp-16-6027-2016, 2016.
Griffin, R. J., Dabdub, D., and Seinfeld, J. H.: Secondary organic aerosol 1. Atmospheric chemical mechanism for production of molecular constituents, J. Geophys. Res.-Atmos., 107, 1–26, https://doi.org/10.1029/2001jd000541, 2002.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, T. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Harrison, R. and Yin, J.: Particulate matter in the atmosphere: which particle properties are important for its effects on health?, Sci. Total Environ., 249, 85–101, https://doi.org/10.1016/s0048-9697(99)00513-6, 2000.
Haywood, J. and Boucher, O.: Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review, Rev. Geophys., 38, 513–543, https://doi.org/10.1029/1999RG000078, 2000.
Hitzenberger, R., Berner, A., Kasper-Giebl, A., Löflund, M., and Puxbaum, H.: Surface tension of Rax cloud water and its relation to the concentration of organic material, J. Geophys. Res.-Atmos., 107, AAC 5–1–AAC 5–6, https://doi.org/10.1029/2002JD002506, 2002.
Hoffmann, E., Tilgner, A., Schrödner, R., Bräuer, P., Wolke, R., and Herrmann, H.: An advanced modeling study on the impacts and atmospheric implications of multiphase dimethyl sulfide chemistry, P. Natl. Acad. Sci. USA, 113, 11776–11781, https://doi.org/10.1073/pnas.1606320113, 2016.
Holz, M., Heil, S. R., and Sacco, A.: Temperature-dependent self-diffusion coefficients of water and six selected molecular liquids for calibration in accurate 1H NMR PFG measurements, Phys. Chem. Chem. Phys., 2, 4740–4742, https://doi.org/10.1039/B005319H, 2000.
Hosny, N. A., Fitzgerald, C., Tong, C., Kalberer, M., Kuimova, M. K., and Pope, F. D.: Fluorescent lifetime imaging of atmospheric aerosols: a direct probe of aerosol viscosity, Faraday Discuss., 165, 343–356, https://doi.org/10.1039/c3fd00041a, 2013.
Hosny, N. A., Fitzgerald, C., Vyšniauskas, A., Athanasiadis, A., Berkemeier, T., Uygur, N., Pöschl, U., Shiraiwa, M., Kalberer, M., Pope, F. D., and Kuimova, M. K.: Direct imaging of changes in aerosol particle viscosity upon hydration and chemical aging, Chemical Science, 7, 1357–1367, https://doi.org/10.1039/c5sc02959g, 2016.
Iinuma, Y., Böge, O., Gnauk, T., and Herrmann, H.: Aerosol-chamber study of the α-pinene/O3 reaction: influence of particle acidity on aerosol yields and products, Atmos. Environ., 38, 761–773, https://doi.org/10.1016/j.atmosenv.2003.10.015, 2004.
Iinuma, Y., Böge, O., Kahnt, A., and Herrmann, H.: Laboratory chamber studies on the formation of organosulfates from reactive uptake of monoterpene oxides, Phys. Chem. Chem. Phys., 11, 7985–7997, https://doi.org/10.1039/B904025K, 2009.
IPCC: Climate Change 2013: The Physical Science Basis, Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, https://doi.org/10.1017/CBO9781107415324, 1535 pp., 2013.
Jenkin, M. E., Saunders, S. M., and Pilling, M. J.: The tropospheric degradation of volatile organic compounds: a protocol for mechanism development, Atmos. Environ., 31, 81–104, https://doi.org/10.1016/s1352-2310(96)00105-7, 1997.
Jenkin, M. E., Shallcross, D. E., and Harvey, J. N.: Development and application of a possible mechanism for the generation of cis-pinic acid from the ozonolysis of α- and β-pinene, Atmos. Environ., 34, 2837–2850, https://doi.org/10.1016/s1352-2310(00)00087-x, 2000.
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, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Jokinen, T., Sipilä, M., Richters, S., Kerminen, V.-M., Paasonen, P., Stratmann, F., Worsnop, D., Kulmala, M., Ehn, M., Herrmann, H., and Berndt, T.: Rapid Autoxidation Forms Highly Oxidized RO2 Radicals in the Atmosphere, Angewandte Chemie International Edition, 53, 14596–14600, https://doi.org/10.1002/anie.201408566, 2014.
Jokinen, T., Berndt, T., Makkonen, R., Kerminen, V.-M., Junninen, H., Paasonen, P., Stratmann, F., Herrmann, H., Guenther, A. B., Worsnop, D. R., Kulmala, M., Ehn, M., and Sipilä, M.: Production of extremely low volatile organic compounds from biogenic emissions: Measured yields and atmospheric implications, P. Natl. Acad. Sci. USA, 112, 7123–7128, https://doi.org/10.1073/pnas.1423977112, 2015.
Kahnt, A., Iinuma, Y., Böge, O., Mutzel, A., and Herrmann, H.: Denuder sampling techniques for the determination of gas-phase carbonyl compounds: A comparison and characterisation of in situ and ex situ derivatisation methods, J. Chromatogr. B, 879, 1402–1411, https://doi.org/10.1016/j.jchromb.2011.02.028, 2011.
Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.: Integrating phase and composition of secondary organic aerosol from the ozonolysis of α-pinene, P. Natl. Acad. Sci. USA, 111, 7552–7557, https://doi.org/10.1073/pnas.1322558111, 2014.
Köhler, H.: The nucleus in and the growth of hygroscopic droplets, T. Faraday Soc., 32, 1152–1161, https://doi.org/10.1039/TF9363201152, 1936.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/c1cp22617g, 2011.
Kuimova, M. K.: Molecular Rotors Image Intracellular Viscosity, CHIMIA International Journal for Chemistry, 66, 159–165, https://doi.org/10.2533/chimia.2012.159, 2012.
Kulmala, M., Toivonen, A., Mäkelä, J., and Laaksonen, A.: Analysis of the growth of nucleation mode particles observed in Boreal forest, Tellus B, 50, 449–462, https://doi.org/10.3402/tellusb.v50i5.16229, 1998.
Kurtén, T., Tiusanen, K., Roldin, P., Rissanen, M., Luy, J., Boy, M., Ehn, M., and Donahue, N.: α-Pinene Autoxidation Products May Not Have Extremely Low Saturation Vapor Pressures Despite High O:C Ratios, J. Phys. Chem. A, 120, 2569–2582, https://doi.org/10.1021/acs.jpca.6b02196, 2016.
Lewis, W. K. and Whitman, W. G.: Principles of Gas Absorption, Industrial & Engineering Chemistry, 16, 1215–1220, https://doi.org/10.1021/ie50180a002, 1924.
Lienhard, D. M., Huisman, A. J., Bones, D. L., Te, Y.-F., Luo, B. P., Krieger, U. K., and Reid, J. P.: Retrieving the translational diffusion coefficient of water from experiments on single levitated aerosol droplets, Phys. Chem. Chem. Phys., 16, 16677–16683, https://doi.org/10.1039/C4CP01939C, 2014.
Lienhard, D. M., Huisman, A. J., Krieger, U. K., Rudich, Y., Marcolli, C., Luo, B. P., Bones, D. L., Reid, J. P., Lambe, A. T., Canagaratna, M. R., Davidovits, P., Onasch, T. B., Worsnop, D. R., Steimer, S. S., Koop, T., and Peter, T.: Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?, Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, 2015.
Mai, H., Shiraiwa, M., Flagan, R. C., and Seinfeld, J. H.: Under What Conditions Can Equilibrium Gas-Particle Partitioning Be Expected to Hold in the Atmosphere?, Environ. Sci. Technol., 49, 11485–11491, https://doi.org/10.1021/acs.est.5b02587, 2015.
Marshall, F. H., Miles, R. E. H., Song, Y.-C., Ohm, P. B., Power, R. M., Reid, J. P., and Dutcher, C. S.: Diffusion and reactivity in ultraviscous aerosol and the correlation with particle viscosity, Chem. Sci., 7, 1298–1308, https://doi.org/10.1039/C5SC03223G, 2016.
Mendoza, C. I., Santamaría-Holek, I., and Pérez-Madrid, A.: Effective temperatures and the breakdown of the Stokes-Einstein relation for particle suspensions, J. Chem. Phys., 143, 104506, https://doi.org/10.1063/1.4930550, 2015.
Mentel, T. F., Springer, M., Ehn, M., Kleist, E., Pullinen, I., Kurtén, T., Rissanen, M., Wahner, A., and Wildt, J.: Formation of highly oxidized multifunctional compounds: autoxidation of peroxy radicals formed in the ozonolysis of alkenes – deduced from structure-product relationships, Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, 2015.
Mutzel, A., Poulain, L., Berndt, T., Iinuma, Y., Rodigast, M., Böge, O., Richters, S., Spindler, G., Sipilä, M., Jokinen, T., Kulmala, M., and Herrmann, H.: Highly Oxidized Multifunctional Organic Compounds Observed in Tropospheric Particles: A Field and Laboratory Study, Environ. Sci. Technol., 49, 7754–7761, https://doi.org/10.1021/acs.est.5b00885, 2015.
Mutzel, A., Rodigast, M., Iinuma, Y., Böge, O., and Herrmann, H.: Monoterpene SOA – Contribution of first-generation oxidation products to formation and chemical composition, Atmos. Environ., 130, 136–144, https://doi.org/10.1016/j.atmosenv.2015.10.080, 2016.
Ng, N., Kroll, J., Keywood, M., Bahreini, R., Varutbangkul, V., Flagan, R., Seinfeld, J., Lee, A., and Goldstein, A.: Contribution of First- versus Second-Generation Products to Secondary Organic Aerosols Formed in the Oxidation of Biogenic Hydrocarbons, Environ. Sci. Technol., 40, 2283–2297, https://doi.org/10.1021/es052269u, 2006.
O'Meara, S., Booth, A. M., Barley, M. H., Topping, D., and McFiggans, G.: An assessment of vapour pressure estimation methods, Phys. Chem. Chem. Phys., 16, 19453–19469, https://doi.org/10.1039/C4CP00857J, 2014.
O'Meara, S., Topping, D. O., and McFiggans, G.: The rate of equilibration of viscous aerosol particles, Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, 2016.
Pajunoja, A., Malila, J., Hao, L., Joutsensaari, J., Lehtinen, K. E. J., and Virtanen, A.: Estimating the Viscosity Range of SOA Particles Based on Their Coalescence Time, Aerosol Sci. Technol., 48, i–iv, https://doi.org/10.1080/02786826.2013.870325, 2014.
Pankow, J. F.: An absorption model of the gas/aerosol partitioning involved in the formation of secondary organic aerosol, Atmos. Environ., 28, 189–193, https://doi.org/10.1016/1352-2310(94)90094-9, 1994.
Pankow, J. F. and Asher, W. E.: SIMPOL.1: a simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds, Atmos. Chem. Phys., 8, 2773–2796, https://doi.org/10.5194/acp-8-2773-2008, 2008.
Perraud, V., Bruns, E. A., Ezell, M. J., Johnson, S. N., Yu, Y., Alexander, M. L., Zelenyuk, A., Imre, D., Chang, W. L., Dabdub, D., Pankow, J. F., and Finlayson-Pitts, B. J.: Nonequilibrium atmospheric secondary organic aerosol formation and growth, P. Natl. Acad. Sci. USA, 109, 2836–2841, https://doi.org/10.1073/pnas.1119909109, 2012.
Pope, C. and Dockery, D.: Health Effects of Fine Particulate Air Pollution: Lines that Connect, J. Air Waste Manage., 56, 709–742, https://doi.org/10.1080/10473289.2006.10464485, 2006.
Power, R. M., Simpson, S. H., Reid, J. P., and Hudson, A. J.: The transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles, Chem. Sci., 4, 2597–2604, https://doi.org/10.1039/c3sc50682g, 2013.
Price, H. C., Mattsson, J., Zhang, Y., Bertram, A. K., Davies, J. F., Grayson, J. W., Martin, S. T., O'Sullivan, D., Reid, J. P., Rickards, A. M. J., and Murray, B. J.: Water diffusion in atmospherically relevant α-pinene secondary organic material, Chem. Sci., 6, 4876–4883, https://doi.org/10.1039/C5SC00685F, 2015.
Pruppacher, H. and Klett, J.: Microphysics of Clouds and Precipitation, 2nd Edn., Springer Netherlands, https://doi.org/10.1007/978-0-306-48100-0, 2010.
Pun, B. K., Wu, S.-Y., Seigneur, C., Seinfeld, J. H., Griffin, R. J., and Pandis, S. N.: Uncertainties in Modeling Secondary Organic Aerosols: Three-Dimensional Modeling Studies in Nashville/Western Tennessee, Environ. Sci. Technol., 37, 3647–3661, https://doi.org/10.1021/es0341541, 2003.
Rampp, M., Buttersack, C., and Lüdemann, H.-D.: c,T-Dependence of the viscosity and the self-diffusion coefficients in some aqueous carbohydrate solutions, Carbohyd. Res., 328, 561–572, https://doi.org/10.1016/s0008-6215(00)00141-5, 2000.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity of α-pinene secondary organic material and implications for particle growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, https://doi.org/10.1073/pnas.1219548110, 2013a.
Renbaum-Wolff, L., Grayson, J. W., and Bertram, A. K.: Technical Note: New methodology for measuring viscosities in small volumes characteristic of environmental chamber particle samples, Atmos. Chem. Phys., 13, 791–802, https://doi.org/10.5194/acp-13-791-2013, 2013b.
Riipinen, I., Yli-Juuti, T., Pierce, J. R., Petaja, T., Worsnop, D. R., Kulmala, M., and Donahue, N. M.: The contribution of organics to atmospheric nanoparticle growth, Nat. Geosci., 5, 453–458, https://doi.org/10.1038/ngeo1499, 2012.
Roldin, P., Eriksson, A. C., Nordin, E. Z., Hermansson, E., Mogensen, D., Rusanen, A., Boy, M., Swietlicki, E., Svenningsson, B., Zelenyuk, A., and Pagels, J.: Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM, Atmos. Chem. Phys., 14, 7953–7993, https://doi.org/10.5194/acp-14-7953-2014, 2014.
Rusumdar, A. J., Wolke, R., Tilgner, A., and Herrmann, H.: Treatment of non-ideality in the SPACCIM multiphase model – Part 1: Model development, Geosci. Model Dev., 9, 247–281, https://doi.org/10.5194/gmd-9-247-2016, 2016.
Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D. R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop, D. R., and Virtanen, A.: Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517–7529, https://doi.org/10.5194/acpd-12-4447-2012, 2012.
Schwartz, S. E.: Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds, Springer Berlin Heidelberg, Berlin, Heidelberg, 415–471, https://doi.org/10.1007/978-3-642-70627-1_16, 1986.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: from Air Pollution to Climate Change, 2nd Edn., John Wiley, New York, https://doi.org/10.1029/2007JD009735, 2006.
Shiraiwa, M., Pfrang, C., and Pöschl, U.: Kinetic multi-layer model of aerosol surface and bulk chemistry (KM-SUB): the influence of interfacial transport and bulk diffusion on the oxidation of oleic acid by ozone, Atmos. Chem. Phys., 10, 3673–3691, https://doi.org/10.5194/acp-10-3673-2010, 2010.
Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108, 11003–11008, https://doi.org/10.1073/pnas.1103045108, 2011.
Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water, Atmos. Chem. Phys., 12, 2777–2794, https://doi.org/10.5194/acp-12-2777-2012, 2012.
Shiraiwa, M., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend, A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA, 110, 11746–11750, https://doi.org/10.1073/pnas.1307501110, 2013a.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, https://doi.org/10.1039/C3CP51595H, 2013b.
Simmel, M. and Wurzler, S.: Condensation and activation in sectional cloud microphysical models, Atmos. Res., 80, 218–236, https://doi.org/10.1016/j.atmosres.2005.08.002, 2006.
Simmel, M., Diehl, K., and Wurzler, S.: Numerical simulation of the microphysics of an orographic cloud: Comparison with measurements and sensitivity studies, Atmos. Environ., 39, 4365–4373, https://doi.org/10.1016/j.atmosenv.2005.02.017, 2005.
Surratt, J. D., Murphy, S. M., Kroll, J. H., Ng, N. L., Hildebrandt, L., Sorooshian, A., Szmigielski, R., Vermeylen, R., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Chemical Composition of Secondary Organic Aerosol Formed from the Photooxidation of Isoprene, J. Phys. Chem. A, 110, 9665–9690, https://doi.org/10.1021/jp061734m, 2006.
Tarjus, G. and Kivelson, D.: Breakdown of the Stokes-Einstein relation in supercooled liquids, J. Chem. Phys., 103, 3071–3073, https://doi.org/10.1063/1.470495, 1995.
Tilgner, A., Bräuer, P., Wolke, R., and Herrmann, H.: Modelling multiphase chemistry in deliquescent aerosols and clouds using CAPRAM3.0i, J. Atmos. Chem., 70, 221–256, https://doi.org/10.1007/s10874-013-9267-4, 2013.
Tobias, H. and Ziemann, P.: Thermal Desorption Mass Spectrometric Analysis of Organic Aerosol Formed from Reactions of 1-Tetradecene and O3 in the Presence of Alcohols and Carboxylic Acids, Environ. Sci. Technol., 34, 2105–2115, https://doi.org/10.1021/es9907156, 2000.
Vaden, T. D., Imre, D., Beránek, J., Shrivastava, M., and Zelenyuk, A.: Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195, https://doi.org/10.1073/pnas.1013391108, 2011.
Vignes, A.: Diffusion in Binary Solutions. Variation of Diffusion Coefficient with Composition, Industrial & Engineering Chemistry Fundamentals, 5, 189–199, https://doi.org/10.1021/i160018a007, 1966.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P., Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic secondary organic aerosol particles, Nature, 467, 824–827, https://doi.org/10.1038/nature09455, 2010.
Virtanen, A., Kannosto, J., Kuuluvainen, H., Arffman, A., Joutsensaari, J., Saukko, E., Hao, L., Yli-Pirilä, P., Tiitta, P., Holopainen, J. K., Keskinen, J., Worsnop, D. R., Smith, J. N., and Laaksonen, A.: Bounce behavior of freshly nucleated biogenic secondary organic aerosol particles, Atmos. Chem. Phys., 11, 8759–8766, https://doi.org/10.5194/acp-11-8759-2011, 2011.
Wesselingh, J. and Bollen, A.: Distillation Multicomponent Diffusivities from the Free Volume Theory, Chemical Engineering Research and Design, 75, 590–602, https://doi.org/10.1205/026387697524119, 1997.
Winterhalter, R., Neeb, P., Grossmann, D., Kolloff, A., Horie, O., and Moortgat, G.: Products and Mechanism of the Gas Phase Reaction of Ozone with β-Pinene, J. Atmos. Chem., 35, 165–197, https://doi.org/10.1023/A:1006257800929, 2000.
Wolke, R. and Knoth, O.: Numerical Solution of Differential and Differential-Algebraic Equations, 4–9 September 2000, Halle, Germany Time-integration of multiphase chemistry in size-resolved cloud models, Appl. Numer. Math., 42, 473–487, https://doi.org/10.1016/S0168-9274(01)00169-6, 2002.
Wolke, R., Sehili, A., Simmel, M., Knoth, O., Tilgner, A., and Herrmann, H.: SPACCIM: A parcel model with detailed microphysics and complex multiphase chemistry, Atmos. Environ., 39, 4375–4388, https://doi.org/10.1016/j.atmosenv.2005.02.038, 2005.
Wolke, R., Schröder, W., Schrödner, R., and Renner, E.: Influence of grid resolution and meteorological forcing on simulated European air quality: A sensitivity study with the modeling system COSMO-MUSCAT, Atmos. Environ., 53, 110–130, https://doi.org/10.1016/j.atmosenv.2012.02.085, 2012.
Zaveri, R. A., Easter, R. C., Shilling, J. E., and Seinfeld, J. H.: Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction, Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, 2014.
Zelenyuk, A., Imre, D., Beránek, J., Abramson, E., Wilson, J., and Shrivastava, M.: Synergy between Secondary Organic Aerosols and Long-Range Transport of Polycyclic Aromatic Hydrocarbons, Environ. Sci. Technol., 46, 12459–12466, https://doi.org/10.1021/es302743z, 2012.
Zhang, X., Cappa, C. D., Jathar, S. H., McVay, R. C., Ensberg, J. J., Kleeman, M. J., and Seinfeld, J. H.: Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol, P. Natl. Acad. Sci. USA, 111, 5802–5807, https://doi.org/10.1073/pnas.1404727111, 2014.
Zhang, Y., Sanchez, M. S., Douet, C., Wang, Y., Bateman, A. P., Gong, Z., Kuwata, M., Renbaum-Wolff, L., Sato, B. B., Liu, P. F., Bertram, A. K., Geiger, F. M., and Martin, S. T.: Changing shapes and implied viscosities of suspended submicron particles, Atmos. Chem. Phys., 15, 7819–7829, https://doi.org/10.5194/acp-15-7819-2015, 2015.
Zhao, J., Ortega, J., Chen, M., McMurry, P. H., and Smith, J. N.: Dependence of particle nucleation and growth on high-molecular-weight gas-phase products during ozonolysis of α-pinene, Atmos. Chem. Phys., 13, 7631–7644, https://doi.org/10.5194/acp-13-7631-2013, 2013.
Zhou, S., Shiraiwa, M., McWhinney, R. D., Pöschl, U., and Abbatt, J. P. D.: Kinetic limitations in gas-particle reactions arising from slow diffusion in secondary organic aerosol, Faraday Discuss., 165, 391–406, https://doi.org/10.1039/C3FD00030C, 2013.
Zhu, L., Cai, T., Huang, J., Stringfellow, T. C., Wall, M., and Yu, L.: Water Self-Diffusion in Glassy and Liquid Maltose Measured by Raman Microscopy and NMR, J. Phys. Chem. B, 155, 5849–5899, https://doi.org/10.1021/jp202663r, 2011.
Ziemann, P. J. and Atkinson, R.: Kinetics, products, and mechanisms of secondary organic aerosol formation, Chem. Soc. Rev., 41, 6582–6605, https://doi.org/10.1039/C2CS35122F, 2012.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.: Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys., 13, 3514–3526, https://doi.org/10.1039/c0cp01273d, 2011.
Short summary
Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and, thus, an advanced treatment of SOA processes in models is necessary. Therefore, this investigation aims at sensitivity studies of a kinetic description of SOA formation. The results reveal that the particle-phase state and the reactivity of the organic solutes are key parameters in the SOA formation. Overall, the results show that an advanced kinetic treatment enables improved model predictions.
Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and,...
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