Articles | Volume 20, issue 15
https://doi.org/10.5194/acp-20-9311-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-9311-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Aug 2020
Research article |
| 07 Aug 2020
| 07 Aug 2020
Development and application of the WRFDA-Chem three-dimensional variational (3DVAR) system: aiming to improve air quality forecasting and diagnose model deficiencies
Wei Sun
National Center for Atmospheric Research, Boulder, CO 80301, USA
National Space Science Center, Chinese Academy of Sciences, Beijing,
100190, China
National Center for Atmospheric Research, Boulder, CO 80301, USA
Institute of Urban Meteorology, China Meteorology Administration,
Beijing, 100089, China
Pusheng Zhao
Institute of Urban Meteorology, China Meteorology Administration,
Beijing, 100089, China
Min Chen
Institute of Urban Meteorology, China Meteorology Administration,
Beijing, 100089, China
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Byoung-Joo Jung, Benjamin Ménétrier, Chris Snyder, Zhiquan Liu, Jonathan J. Guerrette, Junmei Ban, Ivette Hernández Baños, Yonggang G. Yu, and William C. Skamarock
Geosci. Model Dev., 17, 3879–3895, https://doi.org/10.5194/gmd-17-3879-2024, https://doi.org/10.5194/gmd-17-3879-2024, 2024
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We describe the multivariate static background error covariance (B) for the JEDI-MPAS 3D-Var data assimilation system. With tuned B parameters, the multivariate B gives physically balanced analysis increment fields in the single-observation test framework. In the month-long cycling experiment with a global 60 km mesh, 3D-Var with static B performs stably. Due to its simple workflow and minimal computational requirements, JEDI-MPAS 3D-Var can be useful for the research community.
Jonathan J. Guerrette, Zhiquan Liu, Chris Snyder, Byoung-Joo Jung, Craig S. Schwartz, Junmei Ban, Steven Vahl, Yali Wu, Ivette Hernández Baños, Yonggang G. Yu, Soyoung Ha, Yannick Trémolet, Thomas Auligné, Clementine Gas, Benjamin Ménétrier, Anna Shlyaeva, Mark Miesch, Stephen Herbener, Emily Liu, Daniel Holdaway, and Benjamin T. Johnson
Geosci. Model Dev., 16, 7123–7142, https://doi.org/10.5194/gmd-16-7123-2023, https://doi.org/10.5194/gmd-16-7123-2023, 2023
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We demonstrate an ensemble of variational data assimilations (EDA) with the Model for Prediction Across Scales and the Joint Effort for Data assimilation Integration (JEDI) software framework. When compared to 20-member ensemble forecasts from operational initial conditions, those from 80-member EDA-generated initial conditions improve flow-dependent error covariances and subsequent 10 d forecasts. These experiments are repeatable for any atmospheric model with a JEDI interface.
Zhiquan Liu, Chris Snyder, Jonathan J. Guerrette, Byoung-Joo Jung, Junmei Ban, Steven Vahl, Yali Wu, Yannick Trémolet, Thomas Auligné, Benjamin Ménétrier, Anna Shlyaeva, Stephen Herbener, Emily Liu, Daniel Holdaway, and Benjamin T. Johnson
Geosci. Model Dev., 15, 7859–7878, https://doi.org/10.5194/gmd-15-7859-2022, https://doi.org/10.5194/gmd-15-7859-2022, 2022
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JEDI-MPAS 1.0.0, a new data assimilation (DA) system for the MPAS model, was publicly released for community use. This article describes JEDI-MPAS's implementation of the ensemble–variational DA technique and demonstrates its robustness and credible performance by incrementally adding three types of microwave radiances (clear-sky AMSU-A, all-sky AMSU-A, clear-sky MHS) to a non-radiance DA experiment. We intend to periodically release new and improved versions of JEDI-MPAS in upcoming years.
Xinghong Cheng, Zilong Hao, Zengliang Zang, Zhiquan Liu, Xiangde Xu, Shuisheng Wang, Yuelin Liu, Yiwen Hu, and Xiaodan Ma
Atmos. Chem. Phys., 21, 13747–13761, https://doi.org/10.5194/acp-21-13747-2021, https://doi.org/10.5194/acp-21-13747-2021, 2021
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We develop a new inversion method of emission sources based on sensitivity analysis and the three-dimension variational technique. The novel explicit observation operator matrix between emission sources and the receptor’s concentrations is established. Then this method is applied to a typical heavy haze episode in North China, and spatiotemporal variations of SO2, NO2, and O3 concentrations simulated using a posterior emission sources are compared with results using an a priori inventory.
Ying Wei, Xueshun Chen, Huansheng Chen, Yele Sun, Wenyi Yang, Huiyun Du, Qizhong Wu, Dan Chen, Xiujuan Zhao, Jie Li, and Zifa Wang
Geosci. Model Dev., 14, 4411–4428, https://doi.org/10.5194/gmd-14-4411-2021, https://doi.org/10.5194/gmd-14-4411-2021, 2021
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The sub-grid particle formation (SGPF) in plumes plays an important role in air pollution and climate. We coupled an SGPF scheme to a chemical transport model with an aerosol microphysics module and applied it to investigate the SGPF impact over China. The scheme clearly improved the model performance in simulating aerosol components and particle number at typical sites influenced by point sources. The results indicate the significant effects of SGPF on aerosol particles in industrial areas.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Sihang Wang, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 21, 10375–10391, https://doi.org/10.5194/acp-21-10375-2021, https://doi.org/10.5194/acp-21-10375-2021, 2021
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might result in more appropriate parameterization approaches in chemical and climate models.
Yang Yang, Min Chen, Xiujuan Zhao, Dan Chen, Shuiyong Fan, Jianping Guo, and Shaukat Ali
Atmos. Chem. Phys., 20, 12527–12547, https://doi.org/10.5194/acp-20-12527-2020, https://doi.org/10.5194/acp-20-12527-2020, 2020
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This study analyzed the impacts of aerosol–radiation interaction on radiation and meteorological forecasts using the offline coupling of WRF and high-frequency updated AOD simulated by WRF-Chem. The results revealed that aerosol–radiation interaction had a positive influence on the improvement of predictive accuracy, including 2 m temperature (~ 73.9 %) and horizontal wind speed (~ 7.8 %), showing potential prospects for its application in regional numerical weather prediction in northern China.
Soyoung Ha, Zhiquan Liu, Wei Sun, Yonghee Lee, and Limseok Chang
Atmos. Chem. Phys., 20, 6015–6036, https://doi.org/10.5194/acp-20-6015-2020, https://doi.org/10.5194/acp-20-6015-2020, 2020
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This study examines the effect of aerosol optical depth (AOD) retrieved from the Korean Geostationary Ocean Color Imager (GOCI) sensors on surface PM2.5 forecasts using the online coupled WRF-Chem forecasting model and the GSI 3D-Var analysis system. During the KORUS-AQ campaign period, the assimilation of GOCI AOD retrieved at the 550 nm wavelength greatly improved air quality forecasting up to 24 h when assimilated with surface PM2.5 observations, particularly for heavy pollution events.
Bin Yao, Chao Liu, Yan Yin, Zhiquan Liu, Chunxiang Shi, Hironobu Iwabuchi, and Fuzhong Weng
Atmos. Meas. Tech., 13, 1033–1049, https://doi.org/10.5194/amt-13-1033-2020, https://doi.org/10.5194/amt-13-1033-2020, 2020
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Due to the complex spatiotemporal and physical properties of clouds, their quantitative depictions in different atmospheric reanalysis datasets are still highly uncertain. A radiance-based evaluation approach is developed to evaluate the quality of cloud properties by directly comparing them with satellite radiance observations. ERA5 and CRA are found to have great capability in representing the cloudy atmosphere over East Asia, and MERRA-2 tends to slightly overestimate clouds over the region.
Ye Kuang, Yao He, Wanyun Xu, Pusheng Zhao, Yafang Cheng, Gang Zhao, Jiangchuan Tao, Nan Ma, Hang Su, Yanyan Zhang, Jiayin Sun, Peng Cheng, Wenda Yang, Shaobin Zhang, Cheng Wu, Yele Sun, and Chunsheng Zhao
Atmos. Chem. Phys., 20, 865–880, https://doi.org/10.5194/acp-20-865-2020, https://doi.org/10.5194/acp-20-865-2020, 2020
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A new method was developed to calculate hygroscopicity parameter κ of organic aerosols (κOA) based on aerosol light-scattering measurements and bulk aerosol chemical-composition measurements. Derived high-time-resolution κOA varied in a wide range (near 0 to 0.25), and the organic aerosol oxidation degree significantly impacts variations in κOA. Distinct diurnal variation in κOA is found, and its relationship with oxygenated organic aerosol is discussed.
Shizhang Wang and Zhiquan Liu
Geosci. Model Dev., 12, 4031–4051, https://doi.org/10.5194/gmd-12-4031-2019, https://doi.org/10.5194/gmd-12-4031-2019, 2019
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A reflectivity operator was developed for directly assimilating radar reflectivity involving contributions from ice species with the variational data assimilation method. Its current version was implemented in WRFDA 3.9.1. This operator allows for not only the dry snow/graupel but also the wet species so that it can effectively obtain the rainwater, snow, and graupel analysis which improved the short-term precipitation forecasts compared to those of the experiment without DA.
Dan Chen, Zhiquan Liu, Junmei Ban, and Min Chen
Atmos. Chem. Phys., 19, 8619–8650, https://doi.org/10.5194/acp-19-8619-2019, https://doi.org/10.5194/acp-19-8619-2019, 2019
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We updated the WRF/Chem-EnKF DA system to quantitatively estimate SO2 emissions using hourly surface observations as constraints. The 2010 MEIC prior emissions were used to generate January 2015 and 2016 analyzed emissions, which revealed inhomogeneous SO2 emission changes for northern, western, and southern China. These changes were related to facts in reality, indicating that the updated DA system was capable of detecting emission deficiencies and optimizing emissions.
Jing Ding, Pusheng Zhao, Jie Su, Qun Dong, Xiang Du, and Yufen Zhang
Atmos. Chem. Phys., 19, 7939–7954, https://doi.org/10.5194/acp-19-7939-2019, https://doi.org/10.5194/acp-19-7939-2019, 2019
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Aerosol acidity plays a key role in secondary aerosol formation. To provide a more comprehensive reference for aerosol pH and a basis for controlling secondary aerosol generation, this study used the latest data covering four seasons and different particle sizes to obtain the characteristics of aerosol pH and explore the main factors affecting aerosol pH and gas–particle partitioning in the Beijing area.
Dan Chen, Zhiquan Liu, Junmei Ban, Pusheng Zhao, and Min Chen
Atmos. Chem. Phys., 19, 7409–7427, https://doi.org/10.5194/acp-19-7409-2019, https://doi.org/10.5194/acp-19-7409-2019, 2019
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To better characterize the anthropogenic emission-relevant aerosol species, the GSI-WRF/Chem data assimilation system was updated from GOCART to MOSAIC-4BIN scheme. Wintertime 2015–2017 (January) surface PM2.5 observations from more than 1600 sites were assimilated hourly. The observations and reanalysis data from the assimilation experiment were used to investigate year-to-year changes. Roles of emission and meteorology in driving the changes were also distinguished and quantitatively assessed.
Zhen Peng, Lili Lei, Zhiquan Liu, Jianning Sun, Aijun Ding, Junmei Ban, Dan Chen, Xingxia Kou, and Kekuan Chu
Atmos. Chem. Phys., 18, 17387–17404, https://doi.org/10.5194/acp-18-17387-2018, https://doi.org/10.5194/acp-18-17387-2018, 2018
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An EnKF system was developed to simultaneously assimilate multiple surface measurements, including PM10, PM2.5, SO2, NO2, O3, and CO, via the joint adjustment of ICs and source emissions. Large improvements were achieved in the first 24 h forecast for PM2.5, PM10, SO2, and CO during an extreme haze episode that occurred in early October 2014 over the North China Plain, but no improvements were achieved for NO2 and O3.
Pusheng Zhao, Jing Ding, Xiang Du, and Jie Su
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-794, https://doi.org/10.5194/acp-2018-794, 2018
Preprint withdrawn
Dan Chen, Zhiquan Liu, Chris Davis, and Yu Gu
Atmos. Chem. Phys., 17, 7917–7939, https://doi.org/10.5194/acp-17-7917-2017, https://doi.org/10.5194/acp-17-7917-2017, 2017
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Saharan dust influences Atlantic TC genesis, but the relationship and mechanisms are not fully understood. This study investigated the dust radiative effects on atmospheric thermodynamics and tropical cyclogenesis over the Atlantic Ocean using WRF-Chem coupled with an aerosol data assimilation system. Both statistics and a case study revealed that low-altitude (high-altitude) dust inhibits (favors) convection owing to changes in convective inhibition. Semi-direct effects were also noted.
Zhen Peng, Zhiquan Liu, Dan Chen, and Junmei Ban
Atmos. Chem. Phys., 17, 4837–4855, https://doi.org/10.5194/acp-17-4837-2017, https://doi.org/10.5194/acp-17-4837-2017, 2017
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In order to improve the forecasting of atmospheric aerosols over China, the ensemble square root filter algorithm was extended to simultaneously optimize the chemical initial conditions and primary and precursor emissions. This system was applied to assimilate hourly surface PM2.5 measurements. The forecasts with the optimized initial conditions and emissions typically outperformed those from the control experiment without data assimilation.
Dan Chen, Zhiquan Liu, Jerome Fast, and Junmei Ban
Atmos. Chem. Phys., 16, 10707–10724, https://doi.org/10.5194/acp-16-10707-2016, https://doi.org/10.5194/acp-16-10707-2016, 2016
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Extreme haze events occurred frequently over China recently, and adequately predicting peak PM2.5 concentrations is still challenging. In this study, the sulfate–nitrate–ammonium relevant heterogeneous reactions were parameterized for the first time in the WRF-Chem model. We evaluated the performance of WRF-Chem and used the model to investigate the sensitivity of heterogeneous reactions on simulated peak sulfate, nitrate, and ammonium concentrations in the vicinity of Beijing during October 2014.
Zengliang Zang, Zilong Hao, Yi Li, Xiaobin Pan, Wei You, Zhijin Li, and Dan Chen
Geosci. Model Dev., 9, 2623–2638, https://doi.org/10.5194/gmd-9-2623-2016, https://doi.org/10.5194/gmd-9-2623-2016, 2016
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The aerosol data assimilation and forecasts can be improved by adopting balance constraints that spread observation information across variables, thus producing balanced initial distributions. Surface and aircraft aerosol observations were assimilated to demonstrate the impact of the balance constraints. The results showed that the forecasting experiment with balance constraints is more skillful and durable than the experiment without balance constraints.
D. Chen, Z. Liu, C. S. Schwartz, H.-C. Lin, J. D. Cetola, Y. Gu, and L. Xue
Geosci. Model Dev., 7, 2709–2715, https://doi.org/10.5194/gmd-7-2709-2014, https://doi.org/10.5194/gmd-7-2709-2014, 2014
M. Pagowski, Z. Liu, G. A. Grell, M. Hu, H.-C. Lin, and C. S. Schwartz
Geosci. Model Dev., 7, 1621–1627, https://doi.org/10.5194/gmd-7-1621-2014, https://doi.org/10.5194/gmd-7-1621-2014, 2014
Y. H. Mao, Q. B. Li, D. Chen, L. Zhang, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 14, 7195–7211, https://doi.org/10.5194/acp-14-7195-2014, https://doi.org/10.5194/acp-14-7195-2014, 2014
P. E. Saide, G. R. Carmichael, Z. Liu, C. S. Schwartz, H. C. Lin, A. M. da Silva, and E. Hyer
Atmos. Chem. Phys., 13, 10425–10444, https://doi.org/10.5194/acp-13-10425-2013, https://doi.org/10.5194/acp-13-10425-2013, 2013
D. N. Bernstein, J. D. Neelin, Q. B. Li, and D. Chen
Atmos. Chem. Phys., 13, 6373–6390, https://doi.org/10.5194/acp-13-6373-2013, https://doi.org/10.5194/acp-13-6373-2013, 2013
X. J. Zhao, P. S. Zhao, J. Xu, W. Meng,, W. W. Pu, F. Dong, D. He, and Q. F. Shi
Atmos. Chem. Phys., 13, 5685–5696, https://doi.org/10.5194/acp-13-5685-2013, https://doi.org/10.5194/acp-13-5685-2013, 2013
P. S. Zhao, F. Dong, D. He, X. J. Zhao, X. L. Zhang, W. Z. Zhang, Q. Yao, and H. Y. Liu
Atmos. Chem. Phys., 13, 4631–4644, https://doi.org/10.5194/acp-13-4631-2013, https://doi.org/10.5194/acp-13-4631-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
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
Technical note: Influence of different averaging metrics and temporal resolutions on aerosol pH calculated by thermodynamic modeling
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
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM
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
Observation-Constrained Kinetic Modelling of Isoprene SOA Formation in the Atmosphere
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
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
The Role of Naphthalene and Its Derivatives in the Formation of Secondary Organic Aerosols in the Yangtze River Delta Region, China
Significant impact of urban-tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry-transport modeling
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
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Dual roles of inorganic aqueous phase on SOA growth from benzene and phenol
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
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
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying pre-existing particles – Part 2: Modeling chemical drivers and 3-D NPF occurrence
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
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize 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 work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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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 main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter 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.
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.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
EGUsphere, https://doi.org/10.5194/egusphere-2024-479, https://doi.org/10.5194/egusphere-2024-479, 2024
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pH is a key property of ambient aerosols affecting many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence its calculation results from thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
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.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela Dominutti, Guillaume Salque Moreton, Grégory Gilles, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
EGUsphere, https://doi.org/10.5194/egusphere-2024-361, https://doi.org/10.5194/egusphere-2024-361, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focused on finding the appropriate model to evaluate the oxidative character of PM sources in 6 sites, using the PM sources and OP. 8 regression techniques were introduced to assess the OP of PM. This study enlightens the importance of selecting the model according to the input data characteristics and establishes some recommendations on the procedure.
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.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-97, https://doi.org/10.5194/egusphere-2024-97, 2024
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In this work, a multiphase condensed isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass can be reasonably reproduced using the new mechanism. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
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.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2552, https://doi.org/10.5194/egusphere-2023-2552, 2024
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We quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions during four historical period. Due to industrial development and the implementation of different economic policies, sources of anthropogenic aerosols show different variations, which has important implications for the pollution prevention/control measures and decision making for global collaboration.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2023-3042, https://doi.org/10.5194/egusphere-2023-3042, 2024
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The gas-phase chemistry and formation of secondary organic aerosols (SOA) from naphthalene and methylnaphthalene have not been explicitly addressed in models, leaving their contributions unquantified at regional scales. In this study, we incorporated their emissions and SOA parameterizations into an air quality model, revealing the significant potential of these compounds for forming SOA with minimal atmospheric emissions in highly polluted environment like China.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2023-2786, https://doi.org/10.5194/egusphere-2023-2786, 2023
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This study presents the development of a bottom-up inventory of urban-tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air-quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 % and of ozone by 1.0 % on average over the two months.
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.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
EGUsphere, https://doi.org/10.5194/egusphere-2023-2472, https://doi.org/10.5194/egusphere-2023-2472, 2023
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters, as well as model performance compared to AERONET and MODIS retrievals of total aerosol properties, was assessed. General recommendations for incorporating brown carbon into ESMs are also included.
Jiwon Choi, Myoseon Jang, and Spencer Blau
EGUsphere, https://doi.org/10.5194/egusphere-2023-2461, https://doi.org/10.5194/egusphere-2023-2461, 2023
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A persistent phenoxy radical (PPR) effectively forms via a heterogeneous reaction of phenol and phenol-related products in the presence of wet-inorganic aerosol. These PPR can catalytically consume ozone during a NOx cycle and negatively influence SOA formation. SOA formation from phenol or benzene is simulated using the UNIPAR model which predicted SOA formation via multiphase reactions of hydrocarbons and compared with chamber data obtained under varying NOx levels, humidity, and seed types.
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.
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.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
EGUsphere, https://doi.org/10.5194/egusphere-2023-540, https://doi.org/10.5194/egusphere-2023-540, 2023
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
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.
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Short summary
A new aerosol and gas pollutant assimilation capability is developed within the WRFDA system with the 3D variational algorithm and MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) aerosol scheme. By assimilating surface PM2.5, PM10, SO2, NO2, O3, and CO, it improves 24 h air quality forecasting. Based on this system, model deficiencies are explored. Parameterization in the newly added inorganic aerosol heterogeneous reactions should be adjusted and verified by data assimilation.
A new aerosol and gas pollutant assimilation capability is developed within the WRFDA system...
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