Articles | Volume 11, issue 18
© Author(s) 2011. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
© Author(s) 2011. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Inversion of long-lived trace gas emissions using combined Eulerian and Lagrangian chemical transport models
Center for Global Change Science, Massachusetts Institute of Technology, 77 Massachusetts Ave., Cambridge, MA, 02139, UK
A. J. Manning
Atmospheric Dispersion Group, UK Met. Office, Exeter, EX1 3PB, UK
R. G. Prinn
Center for Global Change Science, Massachusetts Institute of Technology, 77 Massachusetts Ave., Cambridge, MA, 02139, UK
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Tropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from spacePotential impact of shipping on air pollution in the Mediterranean region – a multimodel evaluation: comparison of photooxidants NO2 and O3Summertime ozone pollution in China affected by stratospheric quasi-biennial oscillationDeclining, seasonal-varying emissions of sulfur hexafluoride from the United StatesNitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurementsClimate-driven deterioration of future ozone pollution in Asia predicted by machine learning with multi-source dataReconciling the bottom-up and top-down estimates of the methane chemical sink using multiple observationsArctic tropospheric ozone: assessment of current knowledge and model performanceChloride (HCl ∕ Cl−) dominates inorganic aerosol formation from ammonia in the Indo-Gangetic Plain during winter: modeling and comparison with observationsInferring and evaluating satellite-based constraints on NOx emissions estimates in air quality simulationsHow do Cl concentrations matter for the simulation of CH4 and δ13C(CH4) and estimation of the CH4 budget through atmospheric inversions?Cluster-based characterization of multi-dimensional tropospheric ozone variability in coastal regions: an analysis of lidar measurements and model resultsVariable effects of spatial resolution on modeling of nitrogen oxidesExamining the implications of photochemical indicators for O3–NOx–VOC sensitivity and control strategies: a case study in the Yangtze River Delta (YRD), ChinaEvaluation of isoprene nitrate chemistry in detailed chemical mechanismsSixteen years of MOPITT satellite data strongly constrain Amazon CO fire emissionsComparison of model and ground observations finds snowpack and blowing snow aerosols both contribute to Arctic tropospheric reactive bromineAssimilation of S5P/TROPOMI carbon monoxide data with the global CAMS near-real-time systemCOVID-19 lockdown emission reductions have the potential to explain over half of the coincident increase in global atmospheric methaneTransport patterns of global aviation NOx and their short-term O3 radiative forcing – a machine learning approachInverse modelling of Chinese NOx emissions using deep learning: integrating in situ observations with a satellite-based chemical reanalysisSources of surface O3 in the UK: tagging O3 within WRF-ChemGlobal tropospheric ozone trends, attributions, and radiative impacts in 1995–2017: an integrated analysis using aircraft (IAGOS) observations, ozonesonde, and multi-decadal chemical model simulationsOzone depletion events in the Arctic spring of 2019: a new modeling approach to bromine emissionsHigh-resolution inverse modelling of European CH4 emissions using the novel FLEXPART-COSMO TM5 4DVAR inverse modelling systemFour-dimensional variational assimilation for SO2 emission and its application around the COVID-19 lockdown in the spring 2020 over ChinaChanging ozone sensitivity in the South Coast Air Basin during the COVID-19 periodModelling the growth of atmospheric nitrous oxide using a global hierarchical inversionLong-term regional trends of nitrogen and sulfur deposition in the United States from 2002 to 2017A high-resolution satellite-based map of global methane emissions reveals missing wetland, fossil fuel and monsoon sourcesImpact of urbanization on gas-phase pollutant concentrations: a regional-scale, model-based analysis of the contributing factorsCorrecting ozone biases in a global chemistry–climate model: implications for future ozoneEvaluating the contribution of the unexplored photochemistry of aldehydes on the tropospheric levels of molecular hydrogen (H2)The ozone–climate penalty over South America and Africa by 2100An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivityImpact of present and future aircraft NOx and aerosol emissions on atmospheric composition and associated direct radiative forcing of climateAttribution of surface ozone to NOx and volatile organic compound sources during two different high ozone eventsModel output statistics (MOS) applied to Copernicus Atmospheric Monitoring Service (CAMS) O3 forecasts: trade-offs between continuous and categorical skill scoresBayesian assessment of chlorofluorocarbon (CFC), hydrochlorofluorocarbon (HCFC) and halon banks suggest large reservoirs still present in old equipmentGlobal and regional carbon budget for 2015–2020 inferred from OCO-2 based on an ensemble Kalman filter coupled with GEOS-ChemImpact of a subtropical high and a typhoon on a severe ozone pollution episode in the Pearl River Delta, ChinaA renewed rise in global HCFC-141b emissions between 2017–2021A model for simultaneous evaluation of NO2, O3, and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysisTechnical note: Entrainment-limited kinetics of bimolecular reactions in cloudsImproving NOx emission estimates in Beijing using network observations and a perturbed emissions ensembleObservation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, ChinaA machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurementsPotential environmental impact of bromoform from Asparagopsis farming in AustraliaA three-dimensional simulation and process analysis of tropospheric Ozone Depletion Events (ODEs) during the springtime of Arctic using CMAQ
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481,Short summary
A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Jana Moldanova, Sara Jutterström, Jukka-Pekka Jalkanen, and Elisa Majamäki
Atmos. Chem. Phys., 23, 1825–1862,Short summary
Potential ship impact on air pollution in the Mediterranean Sea was simulated with five chemistry transport models. An evaluation of the results for NO2 and O3 air concentrations and dry deposition is presented. Emission data, modeled year and domain were the same. Model run outputs were compared to measurements from background stations. We focused on comparing model outputs regarding the concentration of regulatory pollutants and the relative ship impact on total air pollution concentrations.
Mengyun Li, Yang Yang, Hailong Wang, Huimin Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1533–1544,Short summary
Using the GEOS-Chem model, the impact of the quasi-biennial oscillation (QBO) on summertime tropospheric O3 in China is investigated. In the warm phases of sea surface temperature anomalies over the eastern tropical Pacific, the QBO has a significant positive correlation with near-surface O3 concentrations over central China. The QBO impacts on O3 pollution in China are mainly a result of changing vertical transport of O3.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448,Short summary
Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257,Short summary
NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Huimin Li, Yang Yang, Jianbing Jin, Hailong Wang, Ke Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1131–1145,Short summary
Future climate change will aggravate ozone pollution in Asia, especially in high-forcing scenarios. Ozone pollution in China will expand from North China to South China and extend into the cold season in a warmer future. The emphasis of this work is to quantify the impacts of future climate change on O3 pollution in Asia, which is of great significance for future O3 pollution mitigation strategies.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, and Bo Zheng
Atmos. Chem. Phys., 23, 789–807,Short summary
The large uncertainties in OH simulated by atmospheric chemistry models hinder accurate estimates of CH4 chemical loss through the bottom-up method. This study presents a new approach based on OH precursor observations and a chemical box model to improve the tropospheric OH distributions simulated by atmospheric chemistry models. Through this approach, both the global OH burden and the corresponding methane chemical loss reach consistency with the top-down method based on MCF inversions.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661,Short summary
This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Pooja V. Pawar, Sachin D. Ghude, Gaurav Govardhan, Prodip Acharja, Rachana Kulkarni, Rajesh Kumar, Baerbel Sinha, Vinayak Sinha, Chinmay Jena, Preeti Gunwani, Tapan Kumar Adhya, Eiko Nemitz, and Mark A. Sutton
Atmos. Chem. Phys., 23, 41–59,Short summary
In this study, for the first time in South Asia we compare simulated ammonia, ammonium, and total ammonia using the WRF-Chem model and MARGA measurements during winter in the Indo-Gangetic Plain region. Since observations show HCl promotes the fraction of high chlorides in Delhi, we added HCl / Cl emissions to the model. We conducted three sensitivity experiments with changes in HCl emissions, and improvements are reported in accurately simulating ammonia, ammonium, and total ammonia.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001,Short summary
We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Joël Thanwerdas, Marielle Saunois, Isabelle Pison, Didier Hauglustaine, Antoine Berchet, Bianca Baier, Colm Sweeney, and Philippe Bousquet
Atmos. Chem. Phys., 22, 15489–15508,Short summary
Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 and δ13C(CH4) observations as constraints. The oxidation by chlorine (Cl) contributes little to the total oxidation of CH4 but strongly influences δ13C(CH4). Here, we compare multiple recent Cl fields and quantify the influence of Cl concentrations on CH4, δ13C(CH4), and CH4 budget estimates.
Claudia Bernier, Yuxuan Wang, Guillaume Gronoff, Timothy Berkoff, K. Emma Knowland, John T. Sullivan, Ruben Delgado, Vanessa Caicedo, and Brian Carroll
Atmos. Chem. Phys., 22, 15313–15331,Short summary
Coastal regions are susceptible to variable and high ozone which is difficult to simulate. We developed a method to characterize large datasets of multi-dimensional measurements from lidar instruments taken in coastal regions. Using the clustered ozone groups, we evaluated model performance in simulating the coastal ozone variability vertically and diurnally. The approach allowed us to pinpoint areas where the models succeed in simulating coastal ozone and areas where there are still gaps.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate 1) the variability of NOx resolution-dependent simulation biases; 2) how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and 3) how these biases affect the interpretation of satellite observations. High resolution simulation is thus critical to accurately interpret NOx and its relevance to air quality.
Xun Li, Momei Qin, Lin Li, Kangjia Gong, Huizhong Shen, Jingyi Li, and Jianlin Hu
Atmos. Chem. Phys., 22, 14799–14811,Short summary
Photochemical indicators have been widely used to predict O3–NOx–VOC sensitivity with given thresholds. Here we assessed the effectiveness of four indicators with a case study in the Yangtze River Delta, China. The overall performance was good, while some indicators showed inconsistencies with the O3 isopleths. The methodology used to determine the thresholds may produce uncertainties. These results would improve our understanding of the use of photochemical indicators in policy implications.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798,Short summary
Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Stijn Naus, Lucas G. Domingues, Maarten Krol, Ingrid T. Luijkx, Luciana V. Gatti, John B. Miller, Emanuel Gloor, Sourish Basu, Caio Correia, Gerbrand Koren, Helen M. Worden, Johannes Flemming, Gabrielle Pétron, and Wouter Peters
Atmos. Chem. Phys., 22, 14735–14750,Short summary
We assimilate MOPITT CO satellite data in the TM5-4D-Var inverse modelling framework to estimate Amazon fire CO emissions for 2003–2018. We show that fire emissions have decreased over the analysis period, coincident with a decrease in deforestation rates. However, interannual variations in fire emissions are large, and they correlate strongly with soil moisture. Our results reveal an important role for robust, top-down fire CO emissions in quantifying and attributing Amazon fire intensity.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488,Short summary
Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Antje Inness, Ilse Aben, Melanie Ades, Tobias Borsdorff, Johannes Flemming, Luke Jones, Jochen Landgraf, Bavo Langerock, Philippe Nedelec, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 14355–14376,Short summary
The Copernicus Atmosphere Monitoring Service (CAMS) provides daily global air quality forecasts to users worldwide. One of the species of interest is carbon monoxide (CO), an important trace gas in the atmosphere with anthropogenic and natural sources, produced by incomplete combustion, for example, by wildfires. This paper looks at how well CAMS can model CO in the atmosphere and shows that the fields can be improved when blending CO data from the TROPOMI instrument with the CAMS model.
David S. Stevenson, Richard G. Derwent, Oliver Wild, and William J. Collins
Atmos. Chem. Phys., 22, 14243–14252,Short summary
Atmospheric methane’s growth rate rose by 50 % in 2020 relative to 2019. Lower nitrogen oxide (NOx) emissions tend to increase methane’s atmospheric residence time; lower carbon monoxide (CO) and non-methane volatile organic compound (NMVOC) emissions decrease its lifetime. Combining model sensitivities with emission changes, we find that COVID-19 lockdown emission reductions can explain over half the observed increases in methane in 2020.
Jin Maruhashi, Volker Grewe, Christine Frömming, Patrick Jöckel, and Irene C. Dedoussi
Atmos. Chem. Phys., 22, 14253–14282,Short summary
Aviation NOx emissions lead to the formation of ozone in the atmosphere in the short term, which has a climate warming effect. This study uses global-scale simulations to characterize the transport patterns between NOx emissions at an altitude of ~ 10.4 km and the resulting ozone. Results show a strong spatial and temporal dependence of NOx in disturbing atmospheric O3 concentrations, with the location that is most impacted in terms of warming not necessarily coinciding with the emission region.
Tai-Long He, Dylan B. A. Jones, Kazuyuki Miyazaki, Kevin W. Bowman, Zhe Jiang, Xiaokang Chen, Rui Li, Yuxiang Zhang, and Kunna Li
Atmos. Chem. Phys., 22, 14059–14074,Short summary
We use a deep-learning (DL) model to estimate Chinese NOx emissions by combining satellite analysis and in situ measurements. Our results are consistent with conventional analyses of Chinese NOx emissions. Comparison with mobility data shows that the DL model has a better capability to capture changes in NOx. We analyse Chinese NOx emissions during the COVID-19 pandemic lockdown period. Our results illustrate the potential use of DL as a complementary tool for conventional air quality studies.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys., 22, 13797–13815,Short summary
As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emission controls would be necessary over western Europe to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782,Short summary
We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Maximilian Herrmann, Moritz Schöne, Christian Borger, Simon Warnach, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 22, 13495–13526,Short summary
Ozone depletion events (ODEs) are a common occurrence in the boundary layer during Arctic spring. Ozone is depleted by bromine species in an autocatalytic reaction cycle. Previous modeling studies assumed an infinite bromine source at the ground. An alternative emission scheme is presented in which a finite amount of bromide in the snow is tracked over time. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to study ODEs in the Arctic from February to May 2019.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268,Short summary
We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Yiwen Hu, Zengliang Zang, Xiaoyan Ma, Yi Li, Yanfei Liang, Wei You, Xiaobin Pan, and Zhijin Li
Atmos. Chem. Phys., 22, 13183–13200,Short summary
This study developed a four-dimensional variational assimilation (4DVAR) system based on WRF–Chem to optimise SO2 emissions. The 4DVAR system was applied to obtain the SO2 emissions during the early period of the COVID-19 pandemic over China. The results showed that the 4DVAR system effectively optimised emissions to describe the actual changes in SO2 emissions related to the COVID lockdown, and it can thus be used to improve the accuracy of forecasts.
Jason R. Schroeder, Chenxia Cai, Jin Xu, David Ridley, Jin Lu, Nancy Bui, Fang Yan, and Jeremy Avise
Atmos. Chem. Phys., 22, 12985–13000,Short summary
Ozone, a key component of smog, has plagued the Los Angeles (LA) region for decades. Ozone is created by complex chemical reactions that can be greatly impacted by anthropogenic emissions. This study makes use of the COVID-19 period to study the sensitivity of ozone chemistry in LA to certain anthropogenic emissions, notably from vehicles. We find that vehicular emissions of key pollutants dropped by up to 25 % during COVID-19, which caused a fundamental shift in ozone chemistry in the region.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960,Short summary
Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767,Short summary
We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
Peter Huszar, Jan Karlický, Lukáš Bartík, Marina Liaskoni, Alvaro Patricio Prieto Perez, and Kateřina Šindelářová
Atmos. Chem. Phys., 22, 12647–12674,Short summary
Urbanization turns rural land cover into artificial land cover, while due to human activities, it introduces a great quantity of emissions. We attempt to quantify the impact of urbanization on the final air pollutant levels by looking not only at these emissions, but also 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.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 12543–12557,Short summary
Weaknesses in process representation in chemistry–climate models lead to biases in simulating surface ozone and to uncertainty in projections of future ozone change. We develop a deep learning model to demonstrate the feasibility of ozone bias correction and show its capability in providing improved assessments of the impacts of climate and emission changes on future air quality, along with valuable information to guide future model development.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386,Short summary
We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Flossie Brown, Gerd A. Folberth, Stephen Sitch, Susanne Bauer, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos Vieira, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
Atmos. Chem. Phys., 22, 12331–12352,Short summary
Surface ozone can decrease plant productivity and impair human health. In this study, we evaluate the change in surface ozone due to climate change over South America and Africa using Earth system models. We find that if the climate were to change according to the worst-case scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of ozone exposure, but other areas will experience a climate benefit.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111,Short summary
Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Etienne Terrenoire, Didier A. Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys., 22, 11987–12023,Short summary
Aviation NOx emissions not only have an impact on global climate by changing ozone and methane levels in the atmosphere, but also contribute to the deterioration of local air quality. The LMDZ-INCA global model is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate for ozone, methane and aerosol direct forcings.
Aurelia Lupaşcu, Noelia Otero, Andrea Minkos, and Tim Butler
Atmos. Chem. Phys., 22, 11675–11699,Short summary
Ground-level ozone is an important air pollutant that affects human health, ecosystems, and climate. Ozone is not emitted directly but rather formed in the atmosphere through chemical reactions involving two distinct precursors. Our results provide detailed information about the origin of ozone in Germany during two peak ozone events that took place in 2015 and 2018, thus improving our understanding of ground-level ozone.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys., 22, 11603–11630,Short summary
This study investigates the extent to which ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts while at the same time highlighting the complexity of improving the detection of the highest O3 concentrations.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys., 22, 11125–11136,Short summary
Halocarbons contained in equipment continue to be emitted after production has ceased. These
banksmust be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find that banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone-hole recovery if left unrecovered.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 22, 10769–10788,Short summary
We developed a Bayesian atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) algorithm coupled with GEOS-Chem from the latest Orbiting Carbon Observatory-2 (OCO-2) V10r XCO2 retrievals. This is the first adaptation of 4D-LETKF to an OCO-2-based global carbon inversion system. We inferred global gridded carbon fluxes and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets for 2015–2020.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 10751–10767,Short summary
A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mitag in the Pearl River Delta (PRD) in early Autumn 2019. Through WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in the PRD in 2006.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616,Short summary
The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127,Short summary
A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015,Short summary
Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637,Short summary
Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416,Short summary
We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402,Short summary
We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826,Short summary
We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646,Short summary
In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Simeng Li, Le Cao, Yicheng Gu, and Yuhan Luo
We performed a 3-D mesoscale model study on ODEs occurring in the spring of 2019 in Barrow by using an air-quality model, CMAQ. Several ODEs observed at Barrow were captured by the model, and the contribution from each physical or chemical process to ozone and bromine species during ODEs was quantitatively evaluated. We found the ODEs occurring in Barrow strongly influenced by the horizontal transport. In contrast, over the sea, the local chemistry significantly reduces the surface ozone.
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