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ACP | Articles | Volume 19, issue 13
Atmos. Chem. Phys., 19, 8619–8650, 2019
https://doi.org/10.5194/acp-19-8619-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-8619-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 19, 8619–8650, 2019
https://doi.org/10.5194/acp-19-8619-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-8619-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article 08 Jul 2019
Research article | 08 Jul 2019
The 2015 and 2016 wintertime air pollution in China: SO2 emission changes derived from a WRF-Chem/EnKF coupled data assimilation system
Dan Chen et al.
Related authors
Wei Sun, Zhiquan Liu, Dan Chen, Pusheng Zhao, and Min Chen
Atmos. Chem. Phys., 20, 9311–9329, https://doi.org/10.5194/acp-20-9311-2020, https://doi.org/10.5194/acp-20-9311-2020, 2020
Short summary
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.
Yang Yang, Min Chen, Xiujuan Zhao, Dan Chen, Shuiyong Fan, and Shaukat Ali
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1056, https://doi.org/10.5194/acp-2019-1056, 2020
Revised manuscript under review for ACP
Short summary
Short summary
To facilitate the future inclusion of aerosol-radiation interactions in the regional operational Numerical Weather Prediction (NWP) system – RMAPS-ST (adapted from Weather Research and Forecasting, WRF) at the Institute of Urban Meteorology (IUM), China Meteorological Administration (CMA), the impacts of aerosol-radiation interactions on the forecast of surface radiation and meteorological parameters during a heavy pollution event (December 6th–10th, 2015) over northern China were investigated.
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
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
Wei Sun, Zhiquan Liu, Dan Chen, Pusheng Zhao, and Min Chen
Atmos. Chem. Phys., 20, 9311–9329, https://doi.org/10.5194/acp-20-9311-2020, https://doi.org/10.5194/acp-20-9311-2020, 2020
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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.
Yang Yang, Min Chen, Xiujuan Zhao, Dan Chen, Shuiyong Fan, and Shaukat Ali
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1056, https://doi.org/10.5194/acp-2019-1056, 2020
Revised manuscript under review for ACP
Short summary
Short summary
To facilitate the future inclusion of aerosol-radiation interactions in the regional operational Numerical Weather Prediction (NWP) system – RMAPS-ST (adapted from Weather Research and Forecasting, WRF) at the Institute of Urban Meteorology (IUM), China Meteorological Administration (CMA), the impacts of aerosol-radiation interactions on the forecast of surface radiation and meteorological parameters during a heavy pollution event (December 6th–10th, 2015) over northern China were investigated.
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
Short summary
Short summary
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, 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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
An inversion of NOx and non-methane volatile organic compound (NMVOC) emissions using satellite observations during the KORUS-AQ campaign and implications for surface ozone over East Asia
Influences of hydroxyl radicals (OH) on top-down estimates of the global and regional methane budgets
Evaluation of nitrogen oxides (NOx) sources and sinks and ozone production in Colombia and surrounding areas
The impact of biomass burning on upper tropospheric carbon monoxide: a study using MOCAGE global model and IAGOS airborne data
Temporal and spatial analysis of ozone concentrations in Europe based on timescale decomposition and a multi-clustering approach
Why is the Indo-Gangetic Plain the region with the largest NH3 column in the globe during pre-monsoon and monsoon seasons?
Improving the prediction of an atmospheric chemistry transport model using gradient-boosted regression trees
Attributing ozone and its precursors to land transport emissions in Europe and Germany
Nonstationary modeling of NO2, NO and NOx in Paris using the Street-in-Grid model: coupling local and regional scales with a two-way dynamic approach
Constraining remote oxidation capacity with ATom observations
H migration in peroxy radicals under atmospheric conditions
Variability and past long-term changes of brominated very short-lived substances at the tropical tropopause
Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study
Inverse modeling of SO2 and NOx emissions over China using multisensor satellite data – Part 2: Downscaling techniques for air quality analysis and forecasts
Worsening urban ozone pollution in China from 2013 to 2017 – Part 1: The complex and varying roles of meteorology
Worsening urban ozone pollution in China from 2013 to 2017 – Part 2: The effects of emission changes and implications for multi-pollutant control
Developing a novel hybrid model for the estimation of surface 8 h ozone (O3) across the remote Tibetan Plateau during 2005–2018
Attribution of ground-level ozone to anthropogenic and natural sources of NOx and reactive carbon in a global chemical transport model
Spatial–temporal variations and process analysis of O3 pollution in Hangzhou during the G20 summit
Model simulations of atmospheric methane (1997–2016) and their evaluation using NOAA and AGAGE surface and IAGOS-CARIBIC aircraft observations
The role of plume-scale processes in long-term impacts of aircraft emissions
Evaluation of the CAMS global atmospheric trace gas reanalysis 2003–2016 using aircraft campaign observations
2013–2019 increases of surface ozone pollution in China: anthropogenic and meteorological influences
The impact of ship emissions on air quality and human health in the Gothenburg area – Part II: Scenarios for 2040
Quantification and evaluation of atmospheric ammonia emissions with different methods: a case study for the Yangtze River Delta region, China
Global sensitivity analysis of chemistry–climate model budgets of tropospheric ozone and OH: exploring model diversity
Comprehensive isoprene and terpene gas-phase chemistry improves simulated surface ozone in the southeastern US
Evaluating China's anthropogenic CO2 emissions inventories: a northern China case study using continuous surface observations from 2005 to 2009
Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 – Part 1: Model evaluation and air mass characterization for stratosphere–troposphere transport
Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 – Part 2: Examination of emission impacts based on the higher-order decoupled direct method
The long-term trend and production sensitivity change in the US ozone pollution from observations and model simulations
Comparison of tropospheric NO2 columns from MAX-DOAS retrievals and regional air quality model simulations
Street-scale air quality modelling for Beijing during a winter 2016 measurement campaign
CRI-HOM: A novel chemical mechanism for simulating Highly Oxygenated Organic Molecules (HOMs) in global chemistry-aerosol-climate models
Magnitude, trends, and impacts of ambient long-term ozone exposure in the United States from 2000 to 2015
On the limit to the accuracy of regional-scale air quality models
Effect of changing NOx lifetime on the seasonality and long-term trends of satellite-observed tropospheric NO2 columns over China
A machine learning examination of hydroxyl radical differences among model simulations for CCMI-1
Peroxy radical chemistry and the volatility basis set
The impact of weather pattern and related transport processes on aviation's contribution to ozone and methane concentrations from NOx emissions
Evaluation of a multi-model, multi-constituent assimilation framework for tropospheric chemical reanalysis
Investigation of the global methane budget over 1980–2017 using GFDL-AM4.1
Tropospheric ozone radiative forcing uncertainty due to pre-industrial fire and biogenic emissions
Attribution of Chemistry-Climate Model Initiative (CCMI) ozone radiative flux bias from satellites
Evaluation and uncertainty investigation of the NO2, CO and NH3 modeling over China under the framework of MICS-Asia III
Evaluating China's fossil-fuel CO2 emissions from a comprehensive dataset of nine inventories
Impact of halogen chemistry on summertime air quality in coastal and continental Europe: application of the CMAQ model and implications for regulation
An increase in methane emissions from tropical Africa between 2010 and 2016 inferred from satellite data
Characterizing sources of high surface ozone events in the southwestern U.S. with intensive field measurements and two global models
Source attribution of European surface O3 using a tagged O3 mechanism
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546, https://doi.org/10.5194/acp-20-9525-2020, https://doi.org/10.5194/acp-20-9525-2020, 2020
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The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458, https://doi.org/10.5194/acp-20-9441-2020, https://doi.org/10.5194/acp-20-9441-2020, 2020
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Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Martin Cussac, Virginie Marécal, Valérie Thouret, Béatrice Josse, and Bastien Sauvage
Atmos. Chem. Phys., 20, 9393–9417, https://doi.org/10.5194/acp-20-9393-2020, https://doi.org/10.5194/acp-20-9393-2020, 2020
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Biomass burning emissions are a major source of carbon monoxide in the atmosphere. Here, the vertical transport that these emissions can undergo until the upper troposphere is investigated, as well as their contribution to carbon monoxide concentrations. It was found that boreal forest emissions were specific to the occurrence of pyroconvection directly above the fires, whereas biomass burning emissions from other regions of the globe relied more on the occurrence of deep convection.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tiantian Wang, Yu Song, Zhenying Xu, Mingxu Liu, Tingting Xu, Wenling Liao, Lifei Yin, Xuhui Cai, Ling Kang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 20, 8727–8736, https://doi.org/10.5194/acp-20-8727-2020, https://doi.org/10.5194/acp-20-8727-2020, 2020
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Satellite measurements have revealed that the Indo-Gangetic Plain (IGP) has the global maximum ammonia concentrations, with a peak from June to August. Here, we studied the reasons for this phenomenon through computer simulations. Low sulfur dioxide and nitrogen oxides emissions and high air temperature over the IGP weaken the swallowing of gaseous ammonia by acidic gases. Additionally, the barrier effects of the Himalayas, like a windshield, are also conducive to the accumulation of ammonia.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873, https://doi.org/10.5194/acp-20-7843-2020, https://doi.org/10.5194/acp-20-7843-2020, 2020
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We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
Lya Lugon, Karine Sartelet, Youngseob Kim, Jérémy Vigneron, and Olivier Chrétien
Atmos. Chem. Phys., 20, 7717–7740, https://doi.org/10.5194/acp-20-7717-2020, https://doi.org/10.5194/acp-20-7717-2020, 2020
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This study presents a new version of the multi-scale model Street-in-Grid (SinG) that interconnects regional and local scales in air-quality modeling in urban areas. The new version of SinG performs the finest coupling between transport and chemistry, leading to a numerically stable partitioning between NO and NO2. Multi-scale, local-scale and regional-scale simulations of NO, NO2 and NOx over Paris are compared to observations, and SinG shows good performance for both local and regional scales.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Luc Vereecken and Barbara Nozière
Atmos. Chem. Phys., 20, 7429–7458, https://doi.org/10.5194/acp-20-7429-2020, https://doi.org/10.5194/acp-20-7429-2020, 2020
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Alkyl peroxy radicals, RO2, are important intermediates in the oxidation of organic material in the atmosphere. It was shown earlier that hydrogen atom migration within RO2 can be important and results in the formation of additional oxidants and large highly oxygenated molecules that lead to more and larger aerosols. In this work we propose a method for predicting the chemical rate for these H migrations in RO2, helping atmospheric models to correctly include these reactions.
Susann Tegtmeier, Elliot Atlas, Birgit Quack, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 20, 7103–7123, https://doi.org/10.5194/acp-20-7103-2020, https://doi.org/10.5194/acp-20-7103-2020, 2020
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We investigate emissions of brominated gases from the ocean and their contribution to stratospheric ozone depletion. Once in the atmosphere, these gases usually break down in less than 6 months. Their impact on the ozone layer depends on the prevailing atmospheric circulation, since transport to the stratosphere requires uplift. We combine aircraft and ship observations with atmospheric modelling to analyse how, where, and when these gases are transported from the ocean into the stratosphere.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
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Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
Yi Wang, Jun Wang, Meng Zhou, Daven K. Henze, Cui Ge, and Wei Wang
Atmos. Chem. Phys., 20, 6651–6670, https://doi.org/10.5194/acp-20-6651-2020, https://doi.org/10.5194/acp-20-6651-2020, 2020
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We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS satellite observations (in Part 1) for regional air quality modeling at a spatial resolution that is finer than satellite observations. The VIIRS (city lights), TROPOMI, and OMI satellite data as well as surface data are used to evaluate the model. The method of using the top-down emissions from the past month for the air quality forecast in the present month is also shown to have practical merit.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6305–6321, https://doi.org/10.5194/acp-20-6305-2020, https://doi.org/10.5194/acp-20-6305-2020, 2020
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This study revealed the effects of changes in meteorology and anthropogenic emissions on the summer ozone variations from 2013 to 2017 across China by conducting numerical experiments. We highlighted the important but varying roles of meteorology in ozone variations attributed to the synergistic or counteracting effects from individual meteorological factors. Developing future ozone pollution mitigation policies should consider the counteracting impact of meteorological changes.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6323–6337, https://doi.org/10.5194/acp-20-6323-2020, https://doi.org/10.5194/acp-20-6323-2020, 2020
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Surface ozone levels in urban areas of China were increasing despite the implementation of stringent emission control measures since 2013. Our modeling results show that the decrease in NOx, SO2, and PM emissions and increase in VOC emissions contributed to the urban ozone increases due to the nonlinear ozone chemistry and complex aerosol affects. VOC reduction measures should be implemented in the current and future policies to achieve the goal of improving the overall air quality.
Rui Li, Yilong Zhao, Wenhui Zhou, Ya Meng, Ziyu Zhang, and Hongbo Fu
Atmos. Chem. Phys., 20, 6159–6175, https://doi.org/10.5194/acp-20-6159-2020, https://doi.org/10.5194/acp-20-6159-2020, 2020
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The Tibetan Plateau lacks ground-level O3 observation due to its unique geographical environment. It is imperative to employ modelling methods to simulate the O3 level. The present study proposed a novel technique for estimating the surface O3 level in remote regions. The result captured long-term O3 concentration on the Tibetan Plateau, which was beneficial for assessing the effects of O3 on climate change and ecosystem safety, especially in a vulnerable area of the ecological environment.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-436, https://doi.org/10.5194/acp-2020-436, 2020
Revised manuscript accepted for ACP
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Ground-level ozone is not directly emitted, but rather formed chemically in the atmosphere. Some ground-level ozone is transported from the stratosphere, but most is produced from reactive precursors which are emitted by both natural and man-made sources. We present the results of a novel source apportionment method for ground-level ozone. Our results are consistent with previous work, while also providing new insights. In particular we highlight the role of methane and international shipping.
Zhi-Zhen Ni, Kun Luo, Yang Gao, Xiang Gao, Fei Jiang, Cheng Huang, Jian-Ren Fan, Joshua S. Fu, and Chang-Hong Chen
Atmos. Chem. Phys., 20, 5963–5976, https://doi.org/10.5194/acp-20-5963-2020, https://doi.org/10.5194/acp-20-5963-2020, 2020
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The Weather Research Forecast with Chemistry (WRF-Chem) model was used to simulate spatial and temporal O3 evolution in the Yangtze River Delta (YRD) region. Various atmospheric processes were analyzed to determine the influential factors of ozone formation through the integrated process rate method. This paper provides insight into urban O3 formation and dispersion during tropical cyclone events and supports the Model Intercomparison Study Asia Phase III (MICS-Asia Phase III).
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Yuting Wang, Yong-Feng Ma, Henk Eskes, Antje Inness, Johannes Flemming, and Guy P. Brasseur
Atmos. Chem. Phys., 20, 4493–4521, https://doi.org/10.5194/acp-20-4493-2020, https://doi.org/10.5194/acp-20-4493-2020, 2020
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The paper presents an evaluation of the CAMS global reanalysis of reactive gases performed for the period 2003–2016. The evaluation is performed by comparing concentrations of chemical species gathered during airborne field campaigns with calculated values. The reanalysis successfully reproduces the observed concentrations of ozone and carbon monoxide but generally underestimates the abundance of hydrocarbons. Large discrepancies exist for fast-reacting radicals such as OH and HO2.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-298, https://doi.org/10.5194/acp-2020-298, 2020
Revised manuscript accepted for ACP
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Surface summer ozone has been increasing in China over 2013–2019, despite new governmental efforts targeting ozone pollution. We find the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for North China Plain shows that PM2.5 continued to decrease through 2019 while emissions of volatile organic compounds (VOCs) stayed flat. This can explain the anthropogenic increase in ozone because PM2.5 scavenges the radical precursors of ozone.
Martin O. P. Ramacher, Lin Tang, Jana Moldanová, Volker Matthias, Matthias Karl, Erik Fridell, and Lasse Johansson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-319, https://doi.org/10.5194/acp-2020-319, 2020
Revised manuscript accepted for ACP
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The effects of shipping emissions on air quality and health in the harbor city Gothenburg were simulated for different scenarios for the year 2040 with coupled regional and city-scale chemistry transport models, to evaluate the impact of regional emission regulations and on-shore electricity for ships at berth. The results show that contributions of shipping to exposure and associated health impacts from particulate matter and NO2 are significantly decreasing compared to 2012, in all scenarios.
Yu Zhao, Mengchen Yuan, Xin Huang, Feng Chen, and Jie Zhang
Atmos. Chem. Phys., 20, 4275–4294, https://doi.org/10.5194/acp-20-4275-2020, https://doi.org/10.5194/acp-20-4275-2020, 2020
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We estimated the ammonia emissions based on the constant emission factors and those characterizing the agricultural processes for the Yangtze River Delta, China. The discrepancies between the two estimates and their causes were analyzed. Based on ground and satellite observations, the two estimates were evaluated with air quality modeling. This work indicates ways to improve the emission estimation and helps better understand the necessity of multi-pollutant control strategy.
Oliver Wild, Apostolos Voulgarakis, Fiona O'Connor, Jean-François Lamarque, Edmund M. Ryan, and Lindsay Lee
Atmos. Chem. Phys., 20, 4047–4058, https://doi.org/10.5194/acp-20-4047-2020, https://doi.org/10.5194/acp-20-4047-2020, 2020
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Global models of tropospheric chemistry and transport show a persistent diversity in results that has not been fully explained. We demonstrate the first use of global sensitivity analysis consistently across three independent models to explore these differences and reveal both clear similarities and surprising differences which have important implications for our assessment of future atmospheric composition change.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris Nielsen, Michael B. McElroy, and Rachel Chang
Atmos. Chem. Phys., 20, 3569–3588, https://doi.org/10.5194/acp-20-3569-2020, https://doi.org/10.5194/acp-20-3569-2020, 2020
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China has pledged to reduce carbon dioxide emissions per unit GDP by 60–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. Disagreement among available inventories of Chinese emissions makes it difficult for China to track progress toward its goals and evaluate the efficacy of regional control measures. This study uses a unique set of historical atmospheric observations for the key period from 2005 to 2009 to independently evaluate three different CO2 emission estimates.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, and Yang Zhang
Atmos. Chem. Phys., 20, 3373–3396, https://doi.org/10.5194/acp-20-3373-2020, https://doi.org/10.5194/acp-20-3373-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 1, modeled ozone is evaluated with observations at surface, by ozonesonde and airplane, and by satellite across the Northern Hemisphere. In addition, a newly developed air mass characterization method to estimate stratospheric intrusion is presented.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Atmos. Chem. Phys., 20, 3397–3413, https://doi.org/10.5194/acp-20-3397-2020, https://doi.org/10.5194/acp-20-3397-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 2, the higher-order decoupled direct method (HDDM) is applied to investigate the emission impacts from east Asia and the US during April 2010. Furthermore, changes in trans-Pacific transport caused by the recent emissions are examined.
Hao He, Xin-Zhong Liang, Chao Sun, Zhining Tao, and Daniel Q. Tong
Atmos. Chem. Phys., 20, 3191–3208, https://doi.org/10.5194/acp-20-3191-2020, https://doi.org/10.5194/acp-20-3191-2020, 2020
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We studied the trend of US ozone pollution from 1990 to 2015 using EPA observations and computer simulations. Observations indicated a decrease in peak ozone at noon due to regulations and a slight increase in ozone in early morning and late afternoon possibly. Our modeling system confirmed these findings and provided detailed information about ozone photochemistry. These results revealed the success of previous control measures and provide scientific evidence for the future regulations.
Anne-Marlene Blechschmidt, Joaquim Arteta, Adriana Coman, Lyana Curier, Henk Eskes, Gilles Foret, Clio Gielen, Francois Hendrick, Virginie Marécal, Frédérik Meleux, Jonathan Parmentier, Enno Peters, Gaia Pinardi, Ankie J. M. Piters, Matthieu Plu, Andreas Richter, Arjo Segers, Mikhail Sofiev, Álvaro M. Valdebenito, Michel Van Roozendael, Julius Vira, Tim Vlemmix, and John P. Burrows
Atmos. Chem. Phys., 20, 2795–2823, https://doi.org/10.5194/acp-20-2795-2020, https://doi.org/10.5194/acp-20-2795-2020, 2020
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MAX-DOAS tropospheric NO2 vertical column retrievals from a set of European measurement stations are compared to regional air quality models which contribute to the operational Copernicus Atmosphere Monitoring Service (CAMS). Correlations are on the order of 35 %–75 %; large differences occur for individual pollution plumes. The results demonstrate that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
James Weber, Alexander Archibald, Paul Griffiths, Scott Archer-Nicholls, Torsten Berndt, Michael Jenkin, Hamish Gordon, and Christoph Knote
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-154, https://doi.org/10.5194/acp-2020-154, 2020
Revised manuscript accepted for ACP
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Highly oxygenated organic molecules(HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM-precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosol. The greater importance of HOMs in the PI is also illustrated.
Karl M. Seltzer, Drew T. Shindell, Prasad Kasibhatla, and Christopher S. Malley
Atmos. Chem. Phys., 20, 1757–1775, https://doi.org/10.5194/acp-20-1757-2020, https://doi.org/10.5194/acp-20-1757-2020, 2020
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Long-term exposure to ambient ozone is associated with a variety of impacts, including adverse human-health effects and reduced commercial crop yields. We apply machine learning to empirically model long-term O3 exposure over the continental United States from 2000 to 2015 and generate a measurement-based assessment of impacts on human health and crop yields. Notably, our results illustrate how different conclusions regarding historical impacts can be drawn through the use of varying metrics.
S. Trivikrama Rao, Huiying Luo, Marina Astitha, Christian Hogrefe, Valerie Garcia, and Rohit Mathur
Atmos. Chem. Phys., 20, 1627–1639, https://doi.org/10.5194/acp-20-1627-2020, https://doi.org/10.5194/acp-20-1627-2020, 2020
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Since numerical air quality models do not explicitly simulate stochastic variations in the atmosphere, there will always be differences between modeled and measured pollutant levels even when the model's physics, chemistry, numerical analysis, and its input data are perfect. This paper quantifies the inherent uncertainty in regional models due to the stochastic nature of the atmosphere. A knowledge of the expected error helps model developers in evaluating the real progress in improving models.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Meredith Schervish and Neil M. Donahue
Atmos. Chem. Phys., 20, 1183–1199, https://doi.org/10.5194/acp-20-1183-2020, https://doi.org/10.5194/acp-20-1183-2020, 2020
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Gas-phase autoxidation of organics can generate highly oxygenated organic molecules (HOMs) and thus increase secondary organic aerosol production and enable new-particle formation. Here we explicitly represent the generation of HOMs via peroxy radical chemistry and resolve the products based on volatility and O : C. Using experimentally constrained assumptions about autoxidation and dimerization reactions, we see suppression of HOM formation under low-temperature and high-NOx conditions.
Simon Rosanka, Christine Frömming, and Volker Grewe
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-46, https://doi.org/10.5194/acp-2020-46, 2020
Revised manuscript accepted for ACP
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Aviation attributed nitrogen oxide (NOx) emissions lead to an increase in ozone and a depletion of methane. In this study we investigate the impact of weather related transport processes on these induced composition changes. Subsidence in high pressure systems leads to earlier ozone maxima due to elevated temperatures. Background NOx and hydroperoxyl radicals limit the total ozone change during summer and winter, respectively. High water vapor concentrations lead to a high methane depletion.
Kazuyuki Miyazaki, Kevin W. Bowman, Keiya Yumimoto, Thomas Walker, and Kengo Sudo
Atmos. Chem. Phys., 20, 931–967, https://doi.org/10.5194/acp-20-931-2020, https://doi.org/10.5194/acp-20-931-2020, 2020
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We introduce a multi-model, multi-constituent chemical data assimilation framework that directly accounts for model error in transport and chemistry by integrating a portfolio of forward chemical transport models. The assimilation was able to reduce ensemble forward model spread and bias relative to independent measurements. Diagnostic information readily available from the framework has the potential to improve chemical predictions through relationships such as emergent constraints.
Jian He, Vaishali Naik, Larry W. Horowitz, Ed Dlugokencky, and Kirk Thoning
Atmos. Chem. Phys., 20, 805–827, https://doi.org/10.5194/acp-20-805-2020, https://doi.org/10.5194/acp-20-805-2020, 2020
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In this work, methane representation in AM4.1 is improved by optimizing CH4 emissions to match surface observations. We find increases in CH4 sources balanced by increases in sinks lead to CH4 stabilization during 1999–2006, and anthropogenic sources (e.g., agriculture, energy, and waste) are more likely major contributors to the renewed growth after 2006. Increases in CH4 emissions and decreases in OH levels during 2008–2015 prolong CH4 lifetime and amplify methane response to emission changes.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Stephen R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1065, https://doi.org/10.5194/acp-2019-1065, 2020
Revised manuscript accepted for ACP
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Tropospheric ozone is an important greenhouse gas which contributed to anthropogenic climate change, however the effect of human emissions is uncertain as pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to simulate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34% lower when improved pre-industrial emissions from fires and vegetation are used.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Joshua S. Fu, Xuemei Wang, Syuichi Itahashi, Kazuyo Yamaji, Tatsuya Nagashima, Hyo-Jung Lee, Cheol-Hee Kim, Chuan-Yao Lin, Lei Chen, Meigen Zhang, Zhining Tao, Jie Li, Mizuo Kajino, Hong Liao, Zhe Wang, Kengo Sudo, Yuesi Wang, Yuepeng Pan, Guiqian Tang, Meng Li, Qizhong Wu, Baozhu Ge, and Gregory R. Carmichael
Atmos. Chem. Phys., 20, 181–202, https://doi.org/10.5194/acp-20-181-2020, https://doi.org/10.5194/acp-20-181-2020, 2020
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Evaluation and uncertainty investigation of NO2, CO and NH3 modeling over China were conducted in this study using 14 chemical transport model results from MICS-Asia III. All models largely underestimated CO concentrations and showed very poor performance in reproducing the observed monthly variations of NH3 concentrations. Potential factors related to such deficiencies are investigated and discussed in this paper.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-643, https://doi.org/10.5194/acp-2019-643, 2020
Revised manuscript accepted for ACP
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An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally-measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation and reducing emissions.
Qinyi Li, Rafael Borge, Golam Sarwar, David de la Paz, Brett Gantt, Jessica Domingo, Carlos A. Cuevas, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 19, 15321–15337, https://doi.org/10.5194/acp-19-15321-2019, https://doi.org/10.5194/acp-19-15321-2019, 2019
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The abundance and distribution of reactive halogen species and their impact on air quality in Europe are poorly understood. We adopt a state-of-the-art regional model (CMAQ) to evaluate such effects, and the results demonstrate the significant influence of halogen chemistry on the capacity of atmospheric oxidation and the formation of air pollutants in Europe. Our study highlights the necessity of including halogen chemistry in the formulation of air pollution control policy.
Mark F. Lunt, Paul I. Palmer, Liang Feng, Christopher M. Taylor, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 19, 14721–14740, https://doi.org/10.5194/acp-19-14721-2019, https://doi.org/10.5194/acp-19-14721-2019, 2019
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Using data from the GOSAT satellite between 2010 and 2016 and a Bayesian inversion approach, we estimate monthly emissions of methane from tropical Africa. We find an increase in methane emissions during this period, driven in part by rising emissions from South Sudan. Using ancillary data we attribute this short-term emissions rise to an increase in the extent of the Sudd wetlands driven by increased outflow from the East African lakes.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-990, https://doi.org/10.5194/acp-2019-990, 2019
Revised manuscript accepted for ACP
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern U.S. is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia are important sources of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Aurelia Lupaşcu and Tim Butler
Atmos. Chem. Phys., 19, 14535–14558, https://doi.org/10.5194/acp-19-14535-2019, https://doi.org/10.5194/acp-19-14535-2019, 2019
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Short summary
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.
We updated the WRF/Chem-EnKF DA system to quantitatively estimate SO2 emissions using hourly...
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