Articles | Volume 20, issue 13
Atmos. Chem. Phys., 20, 7717–7740, 2020
https://doi.org/10.5194/acp-20-7717-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue: Air Quality Research at Street-Level (ACP/GMD inter-journal...
Atmos. Chem. Phys., 20, 7717–7740, 2020
https://doi.org/10.5194/acp-20-7717-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 03 Jul 2020
Research article | 03 Jul 2020
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
Lya Lugon et al.
Related authors
Lya Lugon, Jérémy Vigneron, Christophe Debert, Olivier Chrétien, and Karine Sartelet
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-386, https://doi.org/10.5194/gmd-2020-386, 2020
Revised manuscript accepted for GMD
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The multi-scale model Street-in-Grid is used to simulate black carbon (BC) concentrations in streets. To respect street-surface mass balance, particle resuspension is estimated with a new approach based on deposited mass. The contribution of resuspension is low, but non-exhaust emissions from tyre wear largely may contribute to BC concentrations. The impact of the two-way dynamic coupling between scales on BC concentrations varies depending on the street geometry and traffic emissions intensity.
Mario Eduardo Gavidia-Calderón, Sergio Ibarra-Espinosa, Youngseob Kim, Yang Zhang, and Maria de Fatima Andrade
Geosci. Model Dev., 14, 3251–3268, https://doi.org/10.5194/gmd-14-3251-2021, https://doi.org/10.5194/gmd-14-3251-2021, 2021
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The MUNICH model was used to calculate pollutant concentrations inside the streets of São Paulo. The VEIN emission model provided the vehicular emissions and the coordinates of the streets. We used information from an air quality station to account for pollutant concentrations over the street rooftops. Results showed that when emissions are calibrated, MUNICH satisfied the performance criteria. MUNICH can be used to evaluate the impact of traffic-related air pollution on public health.
Eve-Agnès Fiorentino, Henri Wortham, and Karine Sartelet
Geosci. Model Dev., 14, 2747–2780, https://doi.org/10.5194/gmd-14-2747-2021, https://doi.org/10.5194/gmd-14-2747-2021, 2021
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Indoor air quality (IAQ) is strongly influenced by reactivity with surfaces, which is called heterogeneous reactivity. To date, this reactivity is barely integrated into numerical models due to the strong uncertainties it is subjected to. In this work, an open-source IAQ model, called the H2I model, is developed to consider both gas-phase and heterogeneous reactivity and simulate indoor concentrations of inorganic compounds.
Boris Vansevenant, Cédric Louis, Corinne Ferronato, Ludovic Fine, Patrick Tassel, Pascal Perret, Evangelia Kostenidou, Brice Temime-Roussel, Barbara D'Anna, Karine Sartelet, Véronique Cerezo, and Yao Liu
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-43, https://doi.org/10.5194/amt-2021-43, 2021
Preprint under review for AMT
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A new method was developed to correct wall losses of particles on Teflon walls using a new environmental chamber. It was applied to experiments with 6 diesel vehicles (Euro 3 to 6), tested on a chassis dynamometer. Emissions of particles and precursors were obtained in urban and motorway conditions. The chamber experiments help understand the role of physical processes on diesel particle evolutions in the dark. These results can be applied to situations such as tunnels or winter rush hours.
Lya Lugon, Jérémy Vigneron, Christophe Debert, Olivier Chrétien, and Karine Sartelet
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-386, https://doi.org/10.5194/gmd-2020-386, 2020
Revised manuscript accepted for GMD
Short summary
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The multi-scale model Street-in-Grid is used to simulate black carbon (BC) concentrations in streets. To respect street-surface mass balance, particle resuspension is estimated with a new approach based on deposited mass. The contribution of resuspension is low, but non-exhaust emissions from tyre wear largely may contribute to BC concentrations. The impact of the two-way dynamic coupling between scales on BC concentrations varies depending on the street geometry and traffic emissions intensity.
Eve-Agnès Fiorentino, Henri Wortham, and Karine Sartelet
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-192, https://doi.org/10.5194/gmd-2020-192, 2020
Preprint withdrawn
Marwa Majdi, Karine Sartelet, Grazia Maria Lanzafame, Florian Couvidat, Youngseob Kim, Mounir Chrit, and Solene Turquety
Atmos. Chem. Phys., 19, 5543–5569, https://doi.org/10.5194/acp-19-5543-2019, https://doi.org/10.5194/acp-19-5543-2019, 2019
Youngseob Kim, Karine Sartelet, and Florian Couvidat
Atmos. Chem. Phys., 19, 1241–1261, https://doi.org/10.5194/acp-19-1241-2019, https://doi.org/10.5194/acp-19-1241-2019, 2019
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Assumptions (ideality and thermodynamic equilibrium) commonly made in 3-dimensional air quality models were reconsidered to evaluate their impacts on secondary organic aerosol (SOA) formation. Non-ideality (short-, medium- and long-range interactions of organics and inorganics) influences SOA concentrations by about 30 % over Europe. If SOA are highly viscous rather than inviscid, hydrophobic SOA concentrations increase by 6 % but can increase by an order of magnitude for volatile compounds.
Marwa Majdi, Solene Turquety, Karine Sartelet, Carole Legorgeu, Laurent Menut, and Youngseob Kim
Atmos. Chem. Phys., 19, 785–812, https://doi.org/10.5194/acp-19-785-2019, https://doi.org/10.5194/acp-19-785-2019, 2019
Mounir Chrit, Karine Sartelet, Jean Sciare, Marwa Majdi, José Nicolas, Jean-Eudes Petit, and François Dulac
Atmos. Chem. Phys., 18, 18079–18100, https://doi.org/10.5194/acp-18-18079-2018, https://doi.org/10.5194/acp-18-18079-2018, 2018
Mounir Chrit, Karine Sartelet, Jean Sciare, Jorge Pey, José B. Nicolas, Nicolas Marchand, Evelyn Freney, Karine Sellegri, Matthias Beekmann, and François Dulac
Atmos. Chem. Phys., 18, 9631–9659, https://doi.org/10.5194/acp-18-9631-2018, https://doi.org/10.5194/acp-18-9631-2018, 2018
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Fine particulate matter (PM) in the atmosphere is of concern due to its effects on health, climate, ecosystems and biological cycles, and visibility.
These effects are especially important in the Mediterranean region. In this study, the air quality model Polyphemus is used to understand the
sources of inorganic and organic particles in the western Mediterranean and evaluate the uncertainties linked to the model parameters and hypotheses related to condensation/evaporation in the model.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
Evelyn Freney, Karine Sellegri, Mounir Chrit, Kouji Adachi, Joel Brito, Antoine Waked, Agnès Borbon, Aurélie Colomb, Régis Dupuy, Jean-Marc Pichon, Laetitia Bouvier, Claire Delon, Corinne Jambert, Pierre Durand, Thierry Bourianne, Cécile Gaimoz, Sylvain Triquet, Anaïs Féron, Matthias Beekmann, François Dulac, and Karine Sartelet
Atmos. Chem. Phys., 18, 7041–7056, https://doi.org/10.5194/acp-18-7041-2018, https://doi.org/10.5194/acp-18-7041-2018, 2018
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The focus of these experiments, within the ChArMEx project, were to better understand the chemical properties of ambient aerosols over the Mediterranean region. A series of airborne measurements were performed aboard the French research aircraft, the ATR42, during the summer period. Aerosol and gas-phase chemical mass spectrometry allowed us to understand the sources and formation of organic aerosols. Numerical models were incorporated into this study to help interpret our observations.
Youngseob Kim, You Wu, Christian Seigneur, and Yelva Roustan
Geosci. Model Dev., 11, 611–629, https://doi.org/10.5194/gmd-11-611-2018, https://doi.org/10.5194/gmd-11-611-2018, 2018
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A new multi-scale model of urban air pollution is presented. This model combines a regional chemical transport model (CTM) with spatial scales down to 1 km and a street-network model. The street-network model MUNICH is coupled to the Polair3D CTM to constitute the Street-in-Grid (SinG) model. SinG and MUNICH are used to simulate the concentrations of NOx and ozone in a Paris suburb. SinG shows better performance than MUNICH for NO2 measured at monitoring stations within a street canyon.
Mounir Chrit, Karine Sartelet, Jean Sciare, Jorge Pey, Nicolas Marchand, Florian Couvidat, Karine Sellegri, and Matthias Beekmann
Atmos. Chem. Phys., 17, 12509–12531, https://doi.org/10.5194/acp-17-12509-2017, https://doi.org/10.5194/acp-17-12509-2017, 2017
Kevin Berland, Clémence Rose, Jorge Pey, Anais Culot, Evelyn Freney, Nikolaos Kalivitis, Giorgios Kouvarakis, José Carlos Cerro, Marc Mallet, Karine Sartelet, Matthias Beckmann, Thierry Bourriane, Greg Roberts, Nicolas Marchand, Nikolaos Mihalopoulos, and Karine Sellegri
Atmos. Chem. Phys., 17, 9567–9583, https://doi.org/10.5194/acp-17-9567-2017, https://doi.org/10.5194/acp-17-9567-2017, 2017
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New particle formation (NPF) from gas-phase precursors is a process that is expected to drive the total number concentration of particles in the atmosphere. Here we use measurements performed simultaneously in Corsica, Crete and Mallorca to show that the spatial extent of the NPF events are several hundreds of kilometers large. Airborne measurements additionally show that nanoparticles in the marine atmosphere can either be of marine origin or from higher altitudes above the continent.
Jovanna Arndt, Jean Sciare, Marc Mallet, Greg C. Roberts, Nicolas Marchand, Karine Sartelet, Karine Sellegri, François Dulac, Robert M. Healy, and John C. Wenger
Atmos. Chem. Phys., 17, 6975–7001, https://doi.org/10.5194/acp-17-6975-2017, https://doi.org/10.5194/acp-17-6975-2017, 2017
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The chemical composition of individual PM2.5 particles was measured at a background site on Corsica in the Mediterranean to determine the contribution of different sources to background aerosol in the region. Most of the particles were from fossil fuel combustion and biomass burning, transported to the site from France, Italy and eastern Europe, and also accumulated other species en route. This work shows that largest impact on air quality in the Mediterranean is from anthropogenic emissions.
C. Di Biagio, L. Doppler, C. Gaimoz, N. Grand, G. Ancellet, J.-C. Raut, M. Beekmann, A. Borbon, K. Sartelet, J.-L. Attié, F. Ravetta, and P. Formenti
Atmos. Chem. Phys., 15, 9611–9630, https://doi.org/10.5194/acp-15-9611-2015, https://doi.org/10.5194/acp-15-9611-2015, 2015
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Observations from this study indicate that continental pollution largely affects the atmospheric composition and structure of the western Mediterranean basin. Pollution plumes reach 3000-4000 m in altitude and present a very complex and highly stratified structure, characterized by fresh and aged layers both in the boundary layer and in the free troposphere. Also we report the observations of high levels of ultrafine particles over the basin, possibly linked to new particle formation events.
S. Zhu, K. N. Sartelet, and C. Seigneur
Geosci. Model Dev., 8, 1595–1612, https://doi.org/10.5194/gmd-8-1595-2015, https://doi.org/10.5194/gmd-8-1595-2015, 2015
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This article presents the Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. Then, the importance of representing the mixing state when modelling atmospheric aerosol concentrations is investigated in a box model simulation using data representative of air pollution in Greater Paris.
F. Couvidat and K. Sartelet
Geosci. Model Dev., 8, 1111–1138, https://doi.org/10.5194/gmd-8-1111-2015, https://doi.org/10.5194/gmd-8-1111-2015, 2015
Y. Wang, K. N. Sartelet, M. Bocquet, P. Chazette, M. Sicard, G. D'Amico, J. F. Léon, L. Alados-Arboledas, A. Amodeo, P. Augustin, J. Bach, L. Belegante, I. Binietoglou, X. Bush, A. Comerón, H. Delbarre, D. García-Vízcaino, J. L. Guerrero-Rascado, M. Hervo, M. Iarlori, P. Kokkalis, D. Lange, F. Molero, N. Montoux, A. Muñoz, C. Muñoz, D. Nicolae, A. Papayannis, G. Pappalardo, J. Preissler, V. Rizi, F. Rocadenbosch, K. Sellegri, F. Wagner, and F. Dulac
Atmos. Chem. Phys., 14, 12031–12053, https://doi.org/10.5194/acp-14-12031-2014, https://doi.org/10.5194/acp-14-12031-2014, 2014
Y. Wang, K. N. Sartelet, M. Bocquet, and P. Chazette
Atmos. Chem. Phys., 14, 3511–3532, https://doi.org/10.5194/acp-14-3511-2014, https://doi.org/10.5194/acp-14-3511-2014, 2014
Y. Kim, C. Seigneur, and O. Duclaux
Geosci. Model Dev., 7, 569–585, https://doi.org/10.5194/gmd-7-569-2014, https://doi.org/10.5194/gmd-7-569-2014, 2014
Y. Zhang, K. Sartelet, S.-Y. Wu, and C. Seigneur
Atmos. Chem. Phys., 13, 6807–6843, https://doi.org/10.5194/acp-13-6807-2013, https://doi.org/10.5194/acp-13-6807-2013, 2013
Y. Zhang, K. Sartelet, S. Zhu, W. Wang, S.-Y. Wu, X. Zhang, K. Wang, P. Tran, C. Seigneur, and Z.-F. Wang
Atmos. Chem. Phys., 13, 6845–6875, https://doi.org/10.5194/acp-13-6845-2013, https://doi.org/10.5194/acp-13-6845-2013, 2013
M. R. Koohkan, M. Bocquet, Y. Roustan, Y. Kim, and C. Seigneur
Atmos. Chem. Phys., 13, 5887–5905, https://doi.org/10.5194/acp-13-5887-2013, https://doi.org/10.5194/acp-13-5887-2013, 2013
A. Waked, C. Seigneur, F. Couvidat, Y. Kim, K. Sartelet, C. Afif, A. Borbon, P. Formenti, and S. Sauvage
Atmos. Chem. Phys., 13, 5873–5886, https://doi.org/10.5194/acp-13-5873-2013, https://doi.org/10.5194/acp-13-5873-2013, 2013
E. Solazzo, R. Bianconi, G. Pirovano, M. D. Moran, R. Vautard, C. Hogrefe, K. W. Appel, V. Matthias, P. Grossi, B. Bessagnet, J. Brandt, C. Chemel, J. H. Christensen, R. Forkel, X. V. Francis, A. B. Hansen, S. McKeen, U. Nopmongcol, M. Prank, K. N. Sartelet, A. Segers, J. D. Silver, G. Yarwood, J. Werhahn, J. Zhang, S. T. Rao, and S. Galmarini
Geosci. Model Dev., 6, 791–818, https://doi.org/10.5194/gmd-6-791-2013, https://doi.org/10.5194/gmd-6-791-2013, 2013
F. Couvidat, Y. Kim, K. Sartelet, C. Seigneur, N. Marchand, and J. Sciare
Atmos. Chem. Phys., 13, 983–996, https://doi.org/10.5194/acp-13-983-2013, https://doi.org/10.5194/acp-13-983-2013, 2013
Y. Wang, K. N. Sartelet, M. Bocquet, and P. Chazette
Atmos. Chem. Phys., 13, 269–283, https://doi.org/10.5194/acp-13-269-2013, https://doi.org/10.5194/acp-13-269-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Impact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model results
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
Opinion: The germicidal effect of ambient air (open-air factor) revisited
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Study of different Carbon Bond 6 (CB6) mechanisms by using a concentration sensitivity analysis
Accelerating methane growth rate from 2010 to 2017: leading contributions from the tropics and East Asia
Observation and modelling of ozone-destructive halogen chemistry in a passively degassing volcanic plume
Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget
The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition
Comprehensive evaluations of diurnal NO2 measurements during DISCOVER-AQ 2011: effects of resolution-dependent representation of NOx emissions
Downscaling system for modeling of atmospheric composition on regional, urban and street scales
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 1: An overview
Development of ozone reactivity scales for volatile organic compounds in a Chinese megacity
Measured and modelled air quality trends in Italy over the period 2003–2010
Large and increasing methane emissions from eastern Amazonia derived from satellite data, 2010–2018
Contrasting chemical environments in summertime for atmospheric ozone across major Chinese industrial regions: the effectiveness of emission control strategies
Unexpected enhancement of ozone exposure and health risks during National Day in China
Role of oceanic ozone deposition in explaining temporal variability in surface ozone at High Arctic sites
Technical note: Quality assessment of ozone reanalysis products over subarctic Europe for biome modeling and ozone risk mapping
Atmospheric observations consistent with reported decline in the UK's methane emissions, 2013–2020
Oxidation of low-molecular-weight organic compounds in cloud droplets: global impact on tropospheric oxidants
Bias-correcting carbon fluxes derived from land-surface satellite data for retrospective and near-real-time assimilation systems
Characterizing model errors in chemical transport modeling of methane: using GOSAT XCH4 data with weak-constraint four-dimensional variational data assimilation
Estimation of fire-induced carbon emissions from Equatorial Asia in 2015 using in situ aircraft and ship observations
Influence of weather situation on non-CO2 aviation climate effects: the REACT4C climate change functions
Influence of atmospheric in-cloud aqueous-phase chemistry on global simulation of SO2 in CESM2
Impact of international shipping emissions on ozone and PM2.5 in East Asia during summer: the important role of HONO and ClNO2
Modelling the impacts of iodine chemistry on the northern Indian Ocean marine boundary layer
Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem)
Assessing and improving cloud-height-based parameterisations of global lightning flash rate, and their impact on lightning-produced NOx and tropospheric composition in a chemistry–climate model
Impact of regional Northern Hemisphere mid-latitude anthropogenic sulfur dioxide emissions on local and remote tropospheric oxidants
Impact of organic molecular structure on the estimation of atmospherically relevant physicochemical parameters
Spatial and temporal variability in the hydroxyl (OH) radical: understanding the role of large-scale climate features and their influence on OH through its dynamical and photochemical drivers
Analysis of atmospheric ammonia over South and East Asia based on the MOZART-4 model and its comparison with satellite and surface observations
Air quality and health benefits from ultra-low emission control policy indicated by continuous emission monitoring: a case study in the Yangtze River Delta region, China
Background conditions for an urban greenhouse gas network in the Washington, DC, and Baltimore metropolitan region
Explicit modeling of isoprene chemical processing in polluted air masses in suburban areas of the Yangtze River Delta region: radical cycling and formation of ozone and formaldehyde
Evaluation of the LOTOS-EUROS NO2 simulations using ground-based measurements and S5P/TROPOMI observations over Greece
Reactive organic carbon emissions from volatile chemical products
A three-dimensional-model inversion of methyl chloroform to constrain the atmospheric oxidative capacity
Technical note: On comparing greenhouse gas emission metrics
Late-spring and summertime tropospheric ozone and NO2 in western Siberia and the Russian Arctic: regional model evaluation and sensitivities
10-year satellite-constrained fluxes of ammonia improve performance of chemistry transport models
Revealing the sulfur dioxide emission reductions in China by assimilating surface observations in WRF-Chem
Tropospheric ozone in CMIP6 simulations
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
Le Cao, Simeng Li, and Luhang Sun
Atmos. Chem. Phys., 21, 12687–12714, https://doi.org/10.5194/acp-21-12687-2021, https://doi.org/10.5194/acp-21-12687-2021, 2021
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Gas-phase chemical reaction mechanisms, e.g., CB6 mechanism, are essential parts of the atmospheric transport model. In order to better understand the changes caused by the updates between different versions of the CB6 mechanism, in this study, the behavior of three different CB6 mechanisms in simulating ozone, nitrogen oxides and formaldehyde under two different emission conditions was analyzed using a concentration sensitivity analysis, and the reasons causing the deviations were figured out.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Luke Surl, Tjarda Roberts, and Slimane Bekki
Atmos. Chem. Phys., 21, 12413–12441, https://doi.org/10.5194/acp-21-12413-2021, https://doi.org/10.5194/acp-21-12413-2021, 2021
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Many different chemical reactions happen when the gases from a volcano mix with air, but what effects do they have? We present aircraft measurements which show that there is less ozone within the plume of Etna than outside it. We have also made a computer model of this chemistry. This model can reproduce the effects seen when halogens (bromine and chlorine) are included in the volcanic emissions.
We look closely at the simulation to discover how complicated halogen reactions cause ozone loss.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Roman Nuterman, Alexander Mahura, Alexander Baklanov, Bjarne Amstrup, and Ashraf Zakey
Atmos. Chem. Phys., 21, 11099–11112, https://doi.org/10.5194/acp-21-11099-2021, https://doi.org/10.5194/acp-21-11099-2021, 2021
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The street air pollution is usually higher than the pollution at regional and urban scales. It mostly associated with both local emission sources and urban weather conditions. We present the downscaling system for regional, subregional-urban and street scales and evaluate it for acute air-pollution episode. Its evaluation showed a good prediction score across various spatiotemporal scales as well as feasibility of deterministic modelling approach for the operational street scale forecasting.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
Yingnan Zhang, Likun Xue, William P. L. Carter, Chenglei Pei, Tianshu Chen, Jiangshan Mu, Yujun Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 21, 11053–11068, https://doi.org/10.5194/acp-21-11053-2021, https://doi.org/10.5194/acp-21-11053-2021, 2021
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We developed the localized incremental reactivity (IR) for VOCs in a Chinese megacity and elucidated their applications in calculating the ozone formation potential (OFP). The IR scales showed a strong dependence on chemical mechanisms. Both emission- and observation-based inputs are suitable for the MIR calculation but not the case under mixed-limited or NOx-limited O3 formation regimes. We provide suggestions for the application of IR and OFP scales to aid in VOC control in China.
Ilaria D'Elia, Gino Briganti, Lina Vitali, Antonio Piersanti, Gaia Righini, Massimo D'Isidoro, Andrea Cappelletti, Mihaela Mircea, Mario Adani, Gabriele Zanini, and Luisella Ciancarella
Atmos. Chem. Phys., 21, 10825–10849, https://doi.org/10.5194/acp-21-10825-2021, https://doi.org/10.5194/acp-21-10825-2021, 2021
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We present an analysis of modelled trends of PM10, NO2, and O3 airborne concentrations over the Italian territory in 2003–2010. Our analysis shows a general downward simulated trend for all pollutants, with good agreement between observed and modelled values and the model widening both coverage and significance of air concentration trends. Due to the complex atmospheric dynamics, emission reductions do not always result in decreasing concentrations, especially for secondary pollutants.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Michael Hollaway, and Fiona M. O’Connor
Atmos. Chem. Phys., 21, 10689–10706, https://doi.org/10.5194/acp-21-10689-2021, https://doi.org/10.5194/acp-21-10689-2021, 2021
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Surface ozone (O3) has become the main cause of atmospheric pollution in the summertime in China since 2013. We find that 70 % reductions in NOx emissions are required to reduce O3 pollution in most of industrial regions of China, and controls in VOC emissions are very important. The new chemical scheme developed for a global chemistry–climate model not only captures the regional air pollution but also benefits the future studies of regional air-quality–climate interactions.
Peng Wang, Juanyong Shen, Men Xia, Shida Sun, Yanli Zhang, Hongliang Zhang, and Xinming Wang
Atmos. Chem. Phys., 21, 10347–10356, https://doi.org/10.5194/acp-21-10347-2021, https://doi.org/10.5194/acp-21-10347-2021, 2021
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Ozone (O3) pollution has received extensive attention due to worsening air quality and rising health risks. The Chinese National Day holiday (CNDH), which is associated with intensive commercial and tourist activities, serves as a valuable experiment to evaluate the O3 response during the holiday. We find sharply increasing trends of observed O3 concentrations throughout China during the CNDH, leading to 33 % additional total daily deaths.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
Stefanie Falk, Ane Victoria Vollsnes, Aud Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-527, https://doi.org/10.5194/acp-2021-527, 2021
Revised manuscript accepted for ACP
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 78 % accuracy compared to the regional model (73 %).
Mark Lunt, Alistair Manning, Grant Allen, Tim Arnold, Stéphane Bauguitte, Hartmut Boesch, Anita Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon O'Doherty, Paul Palmer, Joseph Pitt, Chris Rennick, Daniel Say, Kieran Stanley, Ann Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-548, https://doi.org/10.5194/acp-2021-548, 2021
Revised manuscript accepted for ACP
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling setup on these findings are explored through a number of sensitivity studies.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Brad Weir, Lesley E. Ott, George J. Collatz, Stephan R. Kawa, Benjamin Poulter, Abhishek Chatterjee, Tomohiro Oda, and Steven Pawson
Atmos. Chem. Phys., 21, 9609–9628, https://doi.org/10.5194/acp-21-9609-2021, https://doi.org/10.5194/acp-21-9609-2021, 2021
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We present a collection of carbon surface fluxes, the Low-order Flux Inversion (LoFI), derived from satellite observations of the Earth's surface and calibrated to match long-term inventories and atmospheric and oceanic records. Simulations using LoFI reproduce background atmospheric carbon dioxide measurements with comparable skill to the leading surface flux products. Available both retrospectively and as a forecast, LoFI enables the study of the carbon cycle as it occurs.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Yosuke Niwa, Yousuke Sawa, Hideki Nara, Toshinobu Machida, Hidekazu Matsueda, Taku Umezawa, Akihiko Ito, Shin-Ichiro Nakaoka, Hiroshi Tanimoto, and Yasunori Tohjima
Atmos. Chem. Phys., 21, 9455–9473, https://doi.org/10.5194/acp-21-9455-2021, https://doi.org/10.5194/acp-21-9455-2021, 2021
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Fires in Equatorial Asia release a large amount of carbon into the atmosphere. Extensively using high-precision atmospheric carbon dioxide (CO2) data from a commercial aircraft observation project, we estimated fire carbon emissions in Equatorial Asia induced by the big El Niño event in 2015. Additional shipboard measurement data elucidated the validity of the analysis and the best estimate indicated 273 Tg C for fire emissions during September–October 2015.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys., 21, 9151–9172, https://doi.org/10.5194/acp-21-9151-2021, https://doi.org/10.5194/acp-21-9151-2021, 2021
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The influence of weather situations on non-CO2 aviation climate impact is investigated to identify systematic weather-related sensitivities. If aircraft avoid the most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high-pressure systems, jet stream, polar night, and tropopause altitude. The results represent a comprehensive data set for studies aiming at weather-dependent flight trajectory optimization to reduce total climate impact.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-406, https://doi.org/10.5194/acp-2021-406, 2021
Revised manuscript accepted for ACP
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Compared with the observations, the results incorporating detailed aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations decreased by 46 %, 41 %, and 22 % in Europe, the United States and China, respectively. Fe-chemistry and HOx-chemistry contributed more to SO2 oxidation than N-chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Jianing Dai and Tao Wang
Atmos. Chem. Phys., 21, 8747–8759, https://doi.org/10.5194/acp-21-8747-2021, https://doi.org/10.5194/acp-21-8747-2021, 2021
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We used the WRF–Chem model with the latest HONO and ClNO2 processes to investigate their effects on the concentrations of ROx radicals, O3, and PM2.5 in Asia during summer. The results show that the ship-derived HONO and ClNO2 increased the ROx radical concentration by 2–3 times and subsequently increased the O3 and PM2.5 concentrations in marine areas. These findings indicate the importance of these nitrogen processes in the evaluation of the impact of ship emissions on air quality.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
Maximilian Herrmann, Holger Sihler, Udo Frieß, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 21, 7611–7638, https://doi.org/10.5194/acp-21-7611-2021, https://doi.org/10.5194/acp-21-7611-2021, 2021
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Time-dependent 3D numerical simulations of tropospheric bromine release and ozone depletion events (ODEs) in the Arctic polar spring of 2009 are compared to observations. Simulation results agree well with the observations at both Utqiaġvik, Alaska, and at Summit, Greenland. In a parameter study, different settings for the bromine release mechanism are evaluated. An enhancement of the bromine release mechanism improves the agreement regarding the occurrence of ODEs with the observations.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Daniel M. Westervelt, Arlene M. Fiore, Colleen B. Baublitz, and Gustavo Correa
Atmos. Chem. Phys., 21, 6799–6810, https://doi.org/10.5194/acp-21-6799-2021, https://doi.org/10.5194/acp-21-6799-2021, 2021
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Particulate air pollution in the atmosphere can impact the availability of gas-phase chemical constituents, which can then have feedbacks on gas-phase air pollutants. We use a chemistry–climate computer model to simulate the impact of particulate pollution from three major world regions on gas-phase chemical constituents. We find that surface-level ozone air pollution decreases by up to 5 ppbv over China in response to Chinese particulate air pollution, which has implications for policy.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Pooja V. Pawar, Sachin D. Ghude, Chinmay Jena, Andrea Móring, Mark A. Sutton, Santosh Kulkarni, Deen Mani Lal, Divya Surendran, Martin Van Damme, Lieven Clarisse, Pierre-François Coheur, Xuejun Liu, Gaurav Govardhan, Wen Xu, Jize Jiang, and Tapan Kumar Adhya
Atmos. Chem. Phys., 21, 6389–6409, https://doi.org/10.5194/acp-21-6389-2021, https://doi.org/10.5194/acp-21-6389-2021, 2021
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In this study, simulations of atmospheric ammonia (NH3) with MOZART-4 and HTAP-v2 are compared with satellite (IASI) and ground-based measurements to understand the spatial and temporal variability of NH3 over two emission hotspot regions of Asia, the IGP and the NCP. Our simulations indicate that the formation of ammonium aerosols is quicker over the NCP than the IGP, leading to smaller NH3 columns over the higher NH3-emitting NCP compared to the IGP region for comparable emissions.
Yan Zhang, Yu Zhao, Meng Gao, Xin Bo, and Chris P. Nielsen
Atmos. Chem. Phys., 21, 6411–6430, https://doi.org/10.5194/acp-21-6411-2021, https://doi.org/10.5194/acp-21-6411-2021, 2021
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We combined air quality and exposure response models to analyze the benefits for air quality and human health of China’s ultra-low emission policy in one of its most developed regions. Atmospheric observations and the air quality model were also used to demonstrate improvement of emission inventories incorporating online emission monitoring data. With implementation of the policy in both power and industrial sectors, the attributable deaths due to PM2.5 exposure are estimated to decrease 5.5 %.
Anna Karion, Israel Lopez-Coto, Sharon M. Gourdji, Kimberly Mueller, Subhomoy Ghosh, William Callahan, Michael Stock, Elizabeth DiGangi, Steve Prinzivalli, and James Whetstone
Atmos. Chem. Phys., 21, 6257–6273, https://doi.org/10.5194/acp-21-6257-2021, https://doi.org/10.5194/acp-21-6257-2021, 2021
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Estimating city emissions based on atmospheric observations requires that the portion of observed greenhouse gases that originated in the city be separated from the portion that originated outside the city, also known as the background concentration. Here, we investigate different methods to determine background concentrations for the Washington, DC, and Baltimore, MD, region and evaluate how well those methods work and the uncertainties they involve.
Kun Zhang, Ling Huang, Qing Li, Juntao Huo, Yusen Duan, Yuhang Wang, Elly Yaluk, Yangjun Wang, Qingyan Fu, and Li Li
Atmos. Chem. Phys., 21, 5905–5917, https://doi.org/10.5194/acp-21-5905-2021, https://doi.org/10.5194/acp-21-5905-2021, 2021
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Recently, high O3 concentrations were frequently observed in rural areas of the Yangtze River Delta (YRD) region under stagnant conditions. Using an online measurement and observation-based model, we investigated the budget of ROx radicals and the influence of isoprene chemistry on O3 formation. Our results underline that isoprene chemistry in the rural atmosphere becomes important with the participation of anthropogenic NOx.
Ioanna Skoulidou, Maria-Elissavet Koukouli, Astrid Manders, Arjo Segers, Dimitris Karagkiozidis, Myrto Gratsea, Dimitris Balis, Alkiviadis Bais, Evangelos Gerasopoulos, Trisevgeni Stavrakou, Jos van Geffen, Henk Eskes, and Andreas Richter
Atmos. Chem. Phys., 21, 5269–5288, https://doi.org/10.5194/acp-21-5269-2021, https://doi.org/10.5194/acp-21-5269-2021, 2021
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The performance of LOTOS-EUROS v2.2.001 regional chemical transport model NO2 simulations is investigated over Greece from June to December 2018. Comparison with in situ NO2 measurements shows a spatial correlation coefficient of 0.86, while the model underestimates the concentrations mostly during daytime (12 to 15:00 local time). Further, the simulated tropospheric NO2 columns are evaluated against ground-based MAX-DOAS NO2 measurements and S5P/TROPOMI observations for July and December 2018.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Ian Enting and Nathan Clisby
Atmos. Chem. Phys., 21, 4699–4708, https://doi.org/10.5194/acp-21-4699-2021, https://doi.org/10.5194/acp-21-4699-2021, 2021
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We provide a new framework for comparing short-lived greenhouse gases to long-lived greenhouse gases such as carbon dioxide using methane as an example. This can clarify the differences between various proposals that have been introduced in order to overcome the use of global warming potentials as a measure of greenhouse gas equivalence.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Nikolaos Evangeliou, Yves Balkanski, Sabine Eckhardt, Anne Cozic, Martin Van Damme, Pierre-François Coheur, Lieven Clarisse, Mark W. Shephard, Karen E. Cady-Pereira, and Didier Hauglustaine
Atmos. Chem. Phys., 21, 4431–4451, https://doi.org/10.5194/acp-21-4431-2021, https://doi.org/10.5194/acp-21-4431-2021, 2021
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Ammonia, a substance that has played a key role in sustaining life, has been increasing in the atmosphere, affecting climate and humans. Understanding the reasons for this increase is important for the beneficial use of ammonia. The evolution of satellite products gives us the opportunity to calculate ammonia emissions easier. We calculated global ammonia emissions over the last 10 years, incorporated them into a chemistry model and recorded notable improvement in reproducing observations.
Tie Dai, Yueming Cheng, Daisuke Goto, Yingruo Li, Xiao Tang, Guangyu Shi, and Teruyuki Nakajima
Atmos. Chem. Phys., 21, 4357–4379, https://doi.org/10.5194/acp-21-4357-2021, https://doi.org/10.5194/acp-21-4357-2021, 2021
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The anthropogenic emission of sulfur dioxide (SO2) over China has significantly declined as a consequence of the clean air actions. We have developed a new emission inversion system to dynamically update the SO2 emission grid by grid over China by assimilating ground-based SO2 observations. The inverted SO2 emission over China in November 2016 on average had declined by 49.4 % since 2010, which is well in agreement with the bottom-up estimation of 48.0 %.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
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Short summary
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.
This study presents a new version of the multi-scale model Street-in-Grid (SinG) that...
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