Articles | Volume 20, issue 20
Atmos. Chem. Phys., 20, 12347–12361, 2020
https://doi.org/10.5194/acp-20-12347-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue: The Modular Earth Submodel System (MESSy) (ACP/GMD inter-journal...
Atmos. Chem. Phys., 20, 12347–12361, 2020
https://doi.org/10.5194/acp-20-12347-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 29 Oct 2020
Research article | 29 Oct 2020
The impact of weather patterns and related transport processes on aviation's contribution to ozone and methane concentrations from NOx emissions
Simon Rosanka et al.
Related authors
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1130, https://doi.org/10.5194/acp-2020-1130, 2020
Preprint under review for ACP
Short summary
Short summary
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.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1041, https://doi.org/10.5194/acp-2020-1041, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxidation of oxygenated volatile organic compounds (OVOCs). Only rudimentary representations of these processes are currently available in global atmospheric models, if any. 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 sink.
Simon Rosanka, Rolf Sander, Andreas Wahner, and Domenico Taraborrelli
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-337, https://doi.org/10.5194/gmd-2020-337, 2020
Preprint under review for GMD
Short summary
Short summary
The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented into the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), which is suitable for global model applications. Within in a box-model study, we show that JAMOC yields reduced gas-phase concentrations of most OVOCs and oxidants, except for nitrogen oxides.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-529, https://doi.org/10.5194/acp-2020-529, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
We investigate the influence of different weather situations on non-CO2 aviation climate impact to identify systematic weather related sensitivities. If aircraft avoid most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high pressure systems, jet stream, polar night, tropopause altitude. The results represent a comprehensive dataset for studies aiming at weather dependent flight trajectory optimization reducing total climate impact.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
Short summary
Short summary
Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
Short summary
Short summary
Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1130, https://doi.org/10.5194/acp-2020-1130, 2020
Preprint under review for ACP
Short summary
Short summary
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.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1041, https://doi.org/10.5194/acp-2020-1041, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxidation of oxygenated volatile organic compounds (OVOCs). Only rudimentary representations of these processes are currently available in global atmospheric models, if any. 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 sink.
Simon Rosanka, Rolf Sander, Andreas Wahner, and Domenico Taraborrelli
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-337, https://doi.org/10.5194/gmd-2020-337, 2020
Preprint under review for GMD
Short summary
Short summary
The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented into the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), which is suitable for global model applications. Within in a box-model study, we show that JAMOC yields reduced gas-phase concentrations of most OVOCs and oxidants, except for nitrogen oxides.
Hiroshi Yamashita, Feijia Yin, Volker Grewe, Patrick Jöckel, Sigrun Matthes, Bastian Kern, Katrin Dahlmann, and Christine Frömming
Geosci. Model Dev., 13, 4869–4890, https://doi.org/10.5194/gmd-13-4869-2020, https://doi.org/10.5194/gmd-13-4869-2020, 2020
Short summary
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This paper describes the updated submodel AirTraf 2.0 which simulates global air traffic in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. Nine aircraft routing options have been integrated, including contrail avoidance, minimum economic costs, and minimum climate impact. Example simulations reveal characteristics of different routing options on air traffic performances. The consistency of the AirTraf simulations is verified with literature data.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-529, https://doi.org/10.5194/acp-2020-529, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
We investigate the influence of different weather situations on non-CO2 aviation climate impact to identify systematic weather related sensitivities. If aircraft avoid most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high pressure systems, jet stream, polar night, tropopause altitude. The results represent a comprehensive dataset for studies aiming at weather dependent flight trajectory optimization reducing total climate impact.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873, https://doi.org/10.5194/acp-20-7843-2020, https://doi.org/10.5194/acp-20-7843-2020, 2020
Short summary
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We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
Short summary
Short summary
Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
Short summary
Short summary
Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Geosci. Model Dev., 13, 363–383, https://doi.org/10.5194/gmd-13-363-2020, https://doi.org/10.5194/gmd-13-363-2020, 2020
Short summary
Short summary
This study investigates if ozone source apportionment results using a tagged tracer approach depend on the resolutions of the applied model and/or emission inventory. For this we apply a global to regional atmospheric chemistry model, which allows us to compare the results on global and regional scales. Our results show that differences on the continental scale (e.g. Europe) are rather small (10 %); on the regional scale, however, differences of up to 30 % were found.
Vanessa S. Rieger, Mariano Mertens, and Volker Grewe
Geosci. Model Dev., 11, 2049–2066, https://doi.org/10.5194/gmd-11-2049-2018, https://doi.org/10.5194/gmd-11-2049-2018, 2018
Short summary
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To reduce the climate impact of human activities, it is crucial to attribute changes in atmospheric gases to anthropogenic emissions. We present an advanced method to determine the contribution of emissions to OH and HO2 concentrations. Compared to the former version, it contains the main reactions of the OH and HO2 chemistry in the troposphere and stratosphere, introduces the tagging of the H radical and closes the budget of the sum of all contributions and the total concentration.
Klaus-Dirk Gottschaldt, Hans Schlager, Robert Baumann, Duy Sinh Cai, Veronika Eyring, Phoebe Graf, Volker Grewe, Patrick Jöckel, Tina Jurkat-Witschas, Christiane Voigt, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 5655–5675, https://doi.org/10.5194/acp-18-5655-2018, https://doi.org/10.5194/acp-18-5655-2018, 2018
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This study places aircraft trace gas measurements from within the Asian summer monsoon anticyclone into the context of regional, intra- and interannual variability. We find that the processes reflected in the measurements are present throughout multiple simulated monsoon seasons. Dynamical instabilities, photochemical ozone production, lightning and entrainments from the lower troposphere and from the tropopause region determine the distinct composition of the anticyclone and its outflow.
Mariano Mertens, Volker Grewe, Vanessa S. Rieger, and Patrick Jöckel
Atmos. Chem. Phys., 18, 5567–5588, https://doi.org/10.5194/acp-18-5567-2018, https://doi.org/10.5194/acp-18-5567-2018, 2018
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We quantified the contribution of land transport and shipping emissions to tropospheric ozone using a global chemistry–climate model. Our results indicate a contribution to ground-level ozone from land transport emissions of up to 18 % in North America and Southern Europe as well as a contribution from shipping emissions of up to 30 % in the Pacific. Our estimates of the radiative ozone forcing due to land transport and shipping emissions are 92 mW m−2 and 62 mW m−2, respectively.
Volker Grewe, Eleni Tsati, Mariano Mertens, Christine Frömming, and Patrick Jöckel
Geosci. Model Dev., 10, 2615–2633, https://doi.org/10.5194/gmd-10-2615-2017, https://doi.org/10.5194/gmd-10-2615-2017, 2017
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We present a diagnostics, implemented in an Earth system model, which keeps track of the contribution of source categories (mainly emission sectors) to various concentrations (O3 and HOx). For the first time, it takes into account chemically competing effects, e.g., the competition between ozone precursors in the production of ozone. We show that the results are in-line with results from other tagging schemes and provide plausibility checks for OH and HO2, which have not previously been tagged.
Hiroshi Yamashita, Volker Grewe, Patrick Jöckel, Florian Linke, Martin Schaefer, and Daisuke Sasaki
Geosci. Model Dev., 9, 3363–3392, https://doi.org/10.5194/gmd-9-3363-2016, https://doi.org/10.5194/gmd-9-3363-2016, 2016
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This study introduces AirTraf v1.0 for climate impact evaluations, which performs global air traffic simulations in the ECHAM5/MESSy Atmospheric Chemistry model. AirTraf simulations were demonstrated with great circle and flight time routing options for a specific winter day, assuming an Airbus A330 aircraft. The results confirmed that AirTraf simulates the air traffic properly for the two options. Calculated flight time, fuel consumption and NOx emission index are comparable to reference data.
Simone Dietmüller, Patrick Jöckel, Holger Tost, Markus Kunze, Catrin Gellhorn, Sabine Brinkop, Christine Frömming, Michael Ponater, Benedikt Steil, Axel Lauer, and Johannes Hendricks
Geosci. Model Dev., 9, 2209–2222, https://doi.org/10.5194/gmd-9-2209-2016, https://doi.org/10.5194/gmd-9-2209-2016, 2016
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Four new radiation related submodels (RAD, AEROPT, CLOUDOPT, and ORBIT) are available within the MESSy framework now. They are largely based on the original radiation scheme of ECHAM5. RAD simulates radiative transfer, AEROPT calculates aerosol optical properties, CLOUDOPT calculates cloud optical properties, and ORBIT is responsible for Earth orbit calculations. Multiple diagnostic calls of the radiation routine are possible, so radiative forcing can be calculated during the model simulation.
Patrick Jöckel, Holger Tost, Andrea Pozzer, Markus Kunze, Oliver Kirner, Carl A. M. Brenninkmeijer, Sabine Brinkop, Duy S. Cai, Christoph Dyroff, Johannes Eckstein, Franziska Frank, Hella Garny, Klaus-Dirk Gottschaldt, Phoebe Graf, Volker Grewe, Astrid Kerkweg, Bastian Kern, Sigrun Matthes, Mariano Mertens, Stefanie Meul, Marco Neumaier, Matthias Nützel, Sophie Oberländer-Hayn, Roland Ruhnke, Theresa Runde, Rolf Sander, Dieter Scharffe, and Andreas Zahn
Geosci. Model Dev., 9, 1153–1200, https://doi.org/10.5194/gmd-9-1153-2016, https://doi.org/10.5194/gmd-9-1153-2016, 2016
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With an advanced numerical global chemistry climate model (CCM) we performed several detailed
combined hind-cast and projection simulations of the period 1950 to 2100 to assess the
past, present, and potential future dynamical and chemical state of the Earth atmosphere.
The manuscript documents the model and the various applied model set-ups and provides
a first evaluation of the simulation results from a global perspective as a quality check of the data.
L. E. Revell, F. Tummon, A. Stenke, T. Sukhodolov, A. Coulon, E. Rozanov, H. Garny, V. Grewe, and T. Peter
Atmos. Chem. Phys., 15, 5887–5902, https://doi.org/10.5194/acp-15-5887-2015, https://doi.org/10.5194/acp-15-5887-2015, 2015
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We have examined the effects of ozone precursor emissions and climate change on the tropospheric ozone budget. Under RCP 6.0, ozone in the future is governed primarily by changes in nitrogen oxides (NOx). Methane is also important, and induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. This study highlights the critical role that emission policies globally have to play in determining tropospheric ozone evolution through the 21st century.
V. Grewe, C. Frömming, S. Matthes, S. Brinkop, M. Ponater, S. Dietmüller, P. Jöckel, H. Garny, E. Tsati, K. Dahlmann, O. A. Søvde, J. Fuglestvedt, T. K. Berntsen, K. P. Shine, E. A. Irvine, T. Champougny, and P. Hullah
Geosci. Model Dev., 7, 175–201, https://doi.org/10.5194/gmd-7-175-2014, https://doi.org/10.5194/gmd-7-175-2014, 2014
H. Garny, G. E. Bodeker, D. Smale, M. Dameris, and V. Grewe
Atmos. Chem. Phys., 13, 7279–7300, https://doi.org/10.5194/acp-13-7279-2013, https://doi.org/10.5194/acp-13-7279-2013, 2013
V. Grewe
Geosci. Model Dev., 6, 417–427, https://doi.org/10.5194/gmd-6-417-2013, https://doi.org/10.5194/gmd-6-417-2013, 2013
V. Grewe
Geosci. Model Dev., 6, 247–253, https://doi.org/10.5194/gmd-6-247-2013, https://doi.org/10.5194/gmd-6-247-2013, 2013
Ø. Hodnebrog, T. K. Berntsen, O. Dessens, M. Gauss, V. Grewe, I. S. A. Isaksen, B. Koffi, G. Myhre, D. Olivié, M. J. Prather, F. Stordal, S. Szopa, Q. Tang, P. van Velthoven, and J. E. Williams
Atmos. Chem. Phys., 12, 12211–12225, https://doi.org/10.5194/acp-12-12211-2012, https://doi.org/10.5194/acp-12-12211-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
Identifying forecast uncertainties for biogenic gases in the Po Valley related to model configuration in EURAD-IM during PEGASOS 2012
Impact of reduced anthropogenic emissions during COVID-19 on air quality in India
A comparison of long-term trends in observations and emission inventories of NOx
Attribution of the accelerating increase in atmospheric methane during 2010–2018 by inverse analysis of GOSAT observations
Global impact of COVID-19 restrictions on the surface concentrations of nitrogen dioxide and ozone
The impact of inhomogeneous emissions and topography on ozone photochemistry in the vicinity of Hong Kong Island
Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget
Influence of aromatics on tropospheric gas-phase composition
Emission inventory of air pollutants and chemical speciation for specific anthropogenic sources based on local measurements in the Yangtze River Delta region, China
Photochemical environment over Southeast Asia primed for hazardous ozone levels with influx of nitrogen oxides from seasonal biomass burning
Atmospheric-methane source and sink sensitivity analysis using Gaussian process emulation
Carbon and air pollutant emissions from China's cement industry 1990–2015: trends, evolution of technologies, and drivers
Assessment of pre-industrial to present-day anthropogenic climate forcing in UKESM1
Technical note: A high-resolution inverse modelling technique for estimating surface CO2 fluxes based on the NIES-TM–FLEXPART coupled transport model and its adjoint
Improvement of the satellite-derived NOx emissions on air quality modeling and its effect on ozone and secondary inorganic aerosol formation in the Yangtze River Delta, China
Aircraft-based inversions quantify the importance of wetlands and livestock for Upper Midwest methane emissions
Time-resolved emission reductions for atmospheric chemistry modelling in Europe during the COVID-19 lockdowns
Background conditions for an urban greenhouse gas network in the Washington, D.C. and Baltimore metropolitan region
Impact of northern hemisphere mid-latitude anthropogenic sulfur dioxide emissions on local and remote tropospheric oxidants
Rapid increase in summer surface ozone over the North China Plain during 2013–2019: a side effect of particulate matter reduction control?
Pan-Arctic surface ozone: modelling vs. measurements
Influence of aerosol copper on HO2 uptake: a novel parameterized equation
Role of ammonia in European air quality with changing land and ship emissions between 1990 and 2030
Spatial and temporal variability of the hydroxyl radical: Understanding the role of large-scale climate features and their influence on OH through its dynamical and photochemical drivers
Modelling the Impacts of Iodine Chemistry on the Northern Indian Ocean Marine Boundary Layer
Discrepancies between MICS-Asia III simulation and observation for surface ozone in the marine atmosphere over the northwestern Pacific Asian Rim region
Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ
Quantifying the emission changes and associated air quality impacts during the COVID-19 pandemic on the North China Plain: a response modeling study
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
3D simulations of tropospheric ozone depletion events using WRF-Chem
Do alternative inventories converge on the spatiotemporal representation of spring ammonia emissions in France?
Impacts of global NOx inversions on NO2 and ozone simulations
Quantifying sources of Brazil's CH4 emissions between 2010 and 2018 from satellite data
On the role of trend and variability in the hydroxyl radical (OH) in the global methane budget
Trends in global tropospheric hydroxyl radical and methane lifetime since 1850 from AerChemMIP
Estimation of rate coefficients for the reactions of O3 with unsaturated organic compounds for use in automated mechanism construction
Long-term historical trends in air pollutant emissions in Asia: Regional Emission inventory in ASia (REAS) version 3
Oxidation of low-molecular weight organic compounds in cloud droplets: global impact on tropospheric oxidants
Northwestward cropland expansion and growing urea-based fertilizer use enhanced NH3 emission loss in the contiguous United States
Impact of structure on the estimation of atmospherically relevant physicochemical parameters
Evaluating China's fossil-fuel CO2 emissions from a comprehensive dataset of nine inventories
Increases in surface ozone pollution in China from 2013 to 2019: anthropogenic and meteorological influences
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.
Annika Vogel and Hendrik Elbern
Atmos. Chem. Phys., 21, 4039–4057, https://doi.org/10.5194/acp-21-4039-2021, https://doi.org/10.5194/acp-21-4039-2021, 2021
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Forecasts of biogenic trace gases highly depend on the model setup and input fields. This study identifies sources of related forecast uncertainties for biogenic gases. Exceptionally high differences in both biogenic emissions and pollutant transport in the Po Valley are identified to be caused by the representation of the land surface and boundary layer dynamics. Consequently, changes in the model configuration are shown to induce significantly different local concentrations of biogenic gases.
Mengyuan Zhang, Arpit Katiyar, Shengqiang Zhu, Juanyong Shen, Men Xia, Jinlong Ma, Sri Harsha Kota, Peng Wang, and Hongliang Zhang
Atmos. Chem. Phys., 21, 4025–4037, https://doi.org/10.5194/acp-21-4025-2021, https://doi.org/10.5194/acp-21-4025-2021, 2021
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We studied changes in air quality in India induced by the COVID-19 lockdown through both surface observations and the CMAQ model. Our results show that emission reductions improved the air quality across India during the lockdown. On average, the levels of PM2.5 and O3 decreased by 28 % and 15 %, indicating positive effects of lockdown measures. We suggest that more stringent and localized emission control strategies should be implemented in India to mitigate air pollutions.
Elena Macdonald, Noelia Otero, and Tim Butler
Atmos. Chem. Phys., 21, 4007–4023, https://doi.org/10.5194/acp-21-4007-2021, https://doi.org/10.5194/acp-21-4007-2021, 2021
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NO2 limit values are still regularly exceeded in many European cities despite decreasing emissions. Measurements of NOx concentrations from stations across Europe were systematically analysed to assess long-term changes observed in urban areas. We compared trends in concentration increments to trends in total and traffic emissions to find potential discrepancies. The results can help in evaluating inaccuracies in emission inventories and in improving spatial imbalances in data availability.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys., 21, 3531–3553, https://doi.org/10.5194/acp-21-3531-2021, https://doi.org/10.5194/acp-21-3531-2021, 2021
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Large-eddy simulations (LESs) were performed in the mountainous region of the island of Hong Kong to investigate the degree to which the rates of chemical reactions between two reactive species are reduced due to the segregation of species within the convective boundary layer. We show that the inhomogeneity in emissions plays an important role in the segregation effect. Topography also has a significant influence on the segregation locally.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Jingyu An, Yiwei Huang, Cheng Huang, Xin Wang, Rusha Yan, Qian Wang, Hongli Wang, Sheng'ao Jing, Yan Zhang, Yiming Liu, Yuan Chen, Chang Xu, Liping Qiao, Min Zhou, Shuhui Zhu, Qingyao Hu, Jun Lu, and Changhong Chen
Atmos. Chem. Phys., 21, 2003–2025, https://doi.org/10.5194/acp-21-2003-2021, https://doi.org/10.5194/acp-21-2003-2021, 2021
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This study established a 4 km × 4 km anthropogenic emission inventory in the Yangtze River Delta region, China, for 2017 based on locally measured emission factors and source profiles. There are high-intensity NOx and NMVOC species emissions in the eastern areas of the region. Toluene, 1,2,4-trimethylbenzene, m,p-xylene, propylene, ethylene, o-xylene, and OVOCs from industry and mobile sources have the highest comprehensive potentials for ozone and secondary organic aerosol formation.
Margaret R. Marvin, Paul I. Palmer, Barry G. Latter, Richard Siddans, Brian J. Kerridge, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 21, 1917–1935, https://doi.org/10.5194/acp-21-1917-2021, https://doi.org/10.5194/acp-21-1917-2021, 2021
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We use an atmospheric chemistry model in combination with satellite and surface observations to investigate how biomass burning affects tropospheric ozone over Southeast Asia during its fire seasons. We find that nitrogen oxides from biomass burning were responsible for about 30 % of the regional ozone formation potential, and we estimate that ozone from biomass burning caused more than 400 excess premature deaths in Southeast Asia during the peak burning months of March and September 2014.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Jun Liu, Dan Tong, Yixuan Zheng, Jing Cheng, Xinying Qin, Qinren Shi, Liu Yan, Yu Lei, and Qiang Zhang
Atmos. Chem. Phys., 21, 1627–1647, https://doi.org/10.5194/acp-21-1627-2021, https://doi.org/10.5194/acp-21-1627-2021, 2021
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In this study, we investigated the decadal changes in carbon dioxide and air pollutant emissions in China's cement industry for the period 1990–2015 based on intensive unit-based information. We found that from 1990 to 2015, accompanied by a 10.3-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 627 %, 56 %, and 659 %, whereas CO, PM2.5, and PM10 emissions decreased by 9 %, 63 %, and 59 %, respectively.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266, https://doi.org/10.5194/acp-21-1245-2021, https://doi.org/10.5194/acp-21-1245-2021, 2021
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In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Yang Yang, Yu Zhao, Lei Zhang, Jie Zhang, Xin Huang, Xuefen Zhao, Yan Zhang, Mengxiao Xi, and Yi Lu
Atmos. Chem. Phys., 21, 1191–1209, https://doi.org/10.5194/acp-21-1191-2021, https://doi.org/10.5194/acp-21-1191-2021, 2021
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We conducted new NOx emission estimation based on the satellite-derived NO2 column constraint and found reduced emissions compared to previous estimates for a developed region in east China. The subsequent improvement in air quality modeling was demonstrated based on available ground observations. With multiple emission reduction cases for various pollutants, we explored the effective control approaches for ozone and inorganic aerosol pollution.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Marc Guevara, Oriol Jorba, Albert Soret, Hervé Petetin, Dene Bowdalo, Kim Serradell, Carles Tena, Hugo Denier van der Gon, Jeroen Kuenen, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 21, 773–797, https://doi.org/10.5194/acp-21-773-2021, https://doi.org/10.5194/acp-21-773-2021, 2021
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Most European countries have imposed lockdowns to combat the spread of the COVID-19 pandemic. Such a socioeconomic disruption has resulted in a sudden drop of atmospheric emissions and air pollution levels. This study quantifies the daily reductions in national emissions and associated levels of nitrogen dioxide (NO2) due to the COVID-19 lockdowns in Europe, by making use of multiple open-access measured activity data as well as artificial intelligence and modelling techniques.
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. Discuss., https://doi.org/10.5194/acp-2020-1256, https://doi.org/10.5194/acp-2020-1256, 2021
Revised manuscript accepted for ACP
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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.
Daniel M. Westervelt, Arlene M. Fiore, Colleen B. Baublitz, and Gustavo Correa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1255, https://doi.org/10.5194/acp-2020-1255, 2021
Revised manuscript accepted for ACP
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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.
Xiaodan Ma, Jianping Huang, Tianliang Zhao, Cheng Liu, Kaihui Zhao, Jia Xing, and Wei Xiao
Atmos. Chem. Phys., 21, 1–16, https://doi.org/10.5194/acp-21-1-2021, https://doi.org/10.5194/acp-21-1-2021, 2021
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The present work aims at identifying and quantifying the relative contributions of the key factors in driving a rapid increase in summertime surface O3 over the North China Plain during 2013–2019. In addition to anthropogenic emission reduction and meteorological variabilities, our study highlights the importance of inclusion of aerosol absorption and scattering properties rather than aerosol abundance only in accurate assessment of aerosol radiative effect on surface O3 formation and change.
Xin Yang, Anne-M. Blechschmidt, Kristof Bognar, Audra McClure-Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David W. Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
Atmos. Chem. Phys., 20, 15937–15967, https://doi.org/10.5194/acp-20-15937-2020, https://doi.org/10.5194/acp-20-15937-2020, 2020
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This is a modelling-based study on Arctic surface ozone, with a particular focus on spring ozone depletion events (i.e. with concentrations < 10 ppbv). Model experiments show that model runs with blowing-snow-sourced sea salt aerosols implemented as a source of reactive bromine can reproduce well large-scale ozone depletion events observed in the Arctic. This study supplies modelling evidence of the proposed mechanism of reactive-bromine release from blowing snow on sea ice (Yang et al., 2008).
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
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. Discuss., https://doi.org/10.5194/acp-2020-1192, https://doi.org/10.5194/acp-2020-1192, 2020
Revised manuscript accepted for ACP
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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 Nino Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Nino 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.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1219, https://doi.org/10.5194/acp-2020-1219, 2020
Revised manuscript accepted for ACP
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Using a regional model, we show that iodine catalysed reactions cause large regional changes to 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.
Hajime Akimoto, Tatsuya Nagashima, Natsumi Kawano, Li Jie, Joshua S. Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 15003–15014, https://doi.org/10.5194/acp-20-15003-2020, https://doi.org/10.5194/acp-20-15003-2020, 2020
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In order to perform proper model simulation of ozone near the ground in the coastal area of northeastern Asia, it has been found that it is very important to select appropriate dry deposition velocities of ozone on the oceanic water of specific area of the northwestern Pacific. Empirical measurement of the mixing ratios and dry deposition flux of ozone over the ocean in this area is highly recommended.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Jia Xing, Siwei Li, Yueqi Jiang, Shuxiao Wang, Dian Ding, Zhaoxin Dong, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 20, 14347–14359, https://doi.org/10.5194/acp-20-14347-2020, https://doi.org/10.5194/acp-20-14347-2020, 2020
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Quantifying emission changes is a prerequisite for assessment of control effectiveness in improving air quality. However, traditional bottom-up methods usually take months to perform and limit timely assessments. A novel method was developed by using a response model that provides real-time estimation of emission changes based on air quality observations. It was successfully applied to quantify emission changes on the North China Plain due to the COVID-19 pandemic shutdown.
Yan Zhang, Yu Zhao, Meng Gao, Xin Bo, and Chris P. Nielsen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-818, https://doi.org/10.5194/acp-2020-818, 2020
Revised manuscript accepted for ACP
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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 emissionpolicy 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 %.
Maximilian Herrmann, Holger Sihler, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-952, https://doi.org/10.5194/acp-2020-952, 2020
Revised manuscript accepted for ACP
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Three-dimensional numerical simulations of tropospheric bromine release and ozone depletion events in the Arctic polar spring of 2009 are analyzed and 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 is found to be beneficial for the correct prediction of the observations.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys., 20, 13481–13495, https://doi.org/10.5194/acp-20-13481-2020, https://doi.org/10.5194/acp-20-13481-2020, 2020
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Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories, both with a reference inventory, that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over northeastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys., 20, 13109–13130, https://doi.org/10.5194/acp-20-13109-2020, https://doi.org/10.5194/acp-20-13109-2020, 2020
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We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Mike J. Newland, and Andrew R. Rickard
Atmos. Chem. Phys., 20, 12921–12937, https://doi.org/10.5194/acp-20-12921-2020, https://doi.org/10.5194/acp-20-12921-2020, 2020
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Unsaturated organic compounds are emitted in large quantities from natural and human-influenced sources. Atmospheric removal occurs significantly by reaction with ozone, initiating reaction sequences forming free radicals and organic pollutants in the gaseous and particulate phases. Due to their very large number, it is impossible to study the reaction rate for every compound, and most have to be estimated. Updated and extended estimation methods are reported for use in atmospheric models.
Junichi Kurokawa and Toshimasa Ohara
Atmos. Chem. Phys., 20, 12761–12793, https://doi.org/10.5194/acp-20-12761-2020, https://doi.org/10.5194/acp-20-12761-2020, 2020
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A long historical emission inventory of major air pollutants in Asia during 1950–2015 was developed as Regional Emission inventory in ASia version 3 (REASv3). Trends of emissions and changes in source contributions in countries and regions in Asia during these 6 decades were analyzed. REASv3 provides monthly gridded data with 0.25° by 0.25° resolution for major source categories as well as table of emissions by countries and sub-regions for major sectors and fuel types.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1041, https://doi.org/10.5194/acp-2020-1041, 2020
Revised manuscript accepted for ACP
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxidation of oxygenated volatile organic compounds (OVOCs). Only rudimentary representations of these processes are currently available in global atmospheric models, if any. 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 sink.
Peiyu Cao, Chaoqun Lu, Jien Zhang, and Avani Khadilkar
Atmos. Chem. Phys., 20, 11907–11922, https://doi.org/10.5194/acp-20-11907-2020, https://doi.org/10.5194/acp-20-11907-2020, 2020
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In this study, we estimate monthly ammonia emission from synthetic nitrogen fertilizer use across the contiguous US from 1900 to 2015. The results indicate the important role that cropland expansion and nitrogen fertilizer enrichment played in enhancing NH3 emissions. It shows such long-term human activities have dramatically changed the spatiotemporal and seasonal patterns of NH3 emission, impacting air pollution and public health in the US.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1038, https://doi.org/10.5194/acp-2020-1038, 2020
Revised manuscript accepted for ACP
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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.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys., 20, 11371–11385, https://doi.org/10.5194/acp-20-11371-2020, https://doi.org/10.5194/acp-20-11371-2020, 2020
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An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation, and reducing emissions.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
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Short summary
Aviation-attributed nitrogen oxide (NOx) emissions lead to an increase in ozone and a depletion of methane. We investigate the impact of weather-related transport processes on these induced composition changes. Subsidence in high-pressure systems leads to earlier ozone maxima due to an enhanced chemical activity. Background NOx and hydroperoxyl radicals limit the total ozone change during summer and winter, respectively. High water vapour concentrations lead to a high methane depletion.
Aviation-attributed nitrogen oxide (NOx) emissions lead to an increase in ozone and a depletion...
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