Articles | Volume 19, issue 23
Atmos. Chem. Phys., 19, 14535–14558, 2019
https://doi.org/10.5194/acp-19-14535-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 19, 14535–14558, 2019
https://doi.org/10.5194/acp-19-14535-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 02 Dec 2019
Research article | 02 Dec 2019
Source attribution of European surface O3 using a tagged O3 mechanism
Aurelia Lupaşcu and Tim Butler
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Piyush Bhardwaj, Manish Naja, Maheswar Rupakheti, Aurelia Lupascu, Andrea Mues, Arnico Kumar Panday, Rajesh Kumar, Khadak Singh Mahata, Shyam Lal, Harish C. Chandola, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 11949–11971, https://doi.org/10.5194/acp-18-11949-2018, https://doi.org/10.5194/acp-18-11949-2018, 2018
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This study provides information about the regional variabilities in some of the pollutants using observations in Nepal and India. It is shown that agricultural crop residue burning leads to a significant enhancement in ozone and CO over a wider region. Further, the wintertime higher ozone levels are shown to be largely due to local emissions, while regional transport could be important in spring and hence shows the role of regional sources versus local sources in the Kathmandu Valley.
Tim Butler, Aurelia Lupascu, Jane Coates, and Shuai Zhu
Geosci. Model Dev., 11, 2825–2840, https://doi.org/10.5194/gmd-11-2825-2018, https://doi.org/10.5194/gmd-11-2825-2018, 2018
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This paper describes a method for determining origin of tropospheric ozone simulated in a global chemistry–climate model. This technique can show which precursor compounds were responsible for simulated ozone, and where they were emitted. In this paper we describe our technique, compare and contrast it with several other similar techniques, and use it to calculate the contribution of several different NOx and VOC precursor categories to the tropospheric ozone burden.
Friderike Kuik, Andreas Kerschbaumer, Axel Lauer, Aurelia Lupascu, Erika von Schneidemesser, and Tim M. Butler
Atmos. Chem. Phys., 18, 8203–8225, https://doi.org/10.5194/acp-18-8203-2018, https://doi.org/10.5194/acp-18-8203-2018, 2018
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Modelled NOx concentrations are often underestimated compared to observations, and measurement studies show that reported NOx emissions in urban areas are often too low when the contribution from traffic is largest. This modelling study quantifies the underestimation of traffic NOx emissions in the Berlin–Brandenburg and finds that they are underestimated by ca. 50 % in the core urban area. More research is needed in order to more accurately understand real-world NOx emissions from traffic.
Andrea Mues, Axel Lauer, Aurelia Lupascu, Maheswar Rupakheti, Friderike Kuik, and Mark G. Lawrence
Geosci. Model Dev., 11, 2067–2091, https://doi.org/10.5194/gmd-11-2067-2018, https://doi.org/10.5194/gmd-11-2067-2018, 2018
A. Lupascu, R. Easter, R. Zaveri, M. Shrivastava, M. Pekour, J. Tomlinson, Q. Yang, H. Matsui, A. Hodzic, Q. Zhang, and J. D. Fast
Atmos. Chem. Phys., 15, 12283–12313, https://doi.org/10.5194/acp-15-12283-2015, https://doi.org/10.5194/acp-15-12283-2015, 2015
Elena Macdonald, Noelia Otero Felipe, and Tim Butler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-951, https://doi.org/10.5194/acp-2020-951, 2020
Revised manuscript accepted for ACP
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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 with evaluating inaccuracies in emission inventories and with improving spatial imbalances in data availability.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys., 20, 10707–10731, https://doi.org/10.5194/acp-20-10707-2020, https://doi.org/10.5194/acp-20-10707-2020, 2020
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Ground-level ozone (O3) is not directly emitted; it is formed chemically in the atmosphere. Some ground-level O3 is transported from the stratosphere, but most O3 is produced from reactive precursors that are emitted by both natural and anthropogenic sources. We present the results of a novel source apportionment method for ground-level O3. Our results are consistent with previous work and also provide new insights. In particular, we highlight the roles of methane and international shipping.
Noelia Otero, Henning W. Rust, and Tim Butler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-691, https://doi.org/10.5194/acp-2020-691, 2020
Revised manuscript not accepted
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Surface ozone concentrations are strongly correlated with temperature in summertime. Using long-term measurements, we investigate changes in the observed relationship between ozone and temperature over Germany. We propose a new statistical approach based on Generalized Additive Models (GAMs) to describe ozone production rates as a function of nitrogen oxides (NOx) and temperature. Our results suggest that NOx reductions alone can not explain the changes in the temperature dependence of ozone.
Noelia Otero, Jana Sillmann, Kathleen A. Mar, Henning W. Rust, Sverre Solberg, Camilla Andersson, Magnuz Engardt, Robert Bergström, Bertrand Bessagnet, Augustin Colette, Florian Couvidat, Cournelius Cuvelier, Svetlana Tsyro, Hilde Fagerli, Martijn Schaap, Astrid Manders, Mihaela Mircea, Gino Briganti, Andrea Cappelletti, Mario Adani, Massimo D'Isidoro, María-Teresa Pay, Mark Theobald, Marta G. Vivanco, Peter Wind, Narendra Ojha, Valentin Raffort, and Tim Butler
Atmos. Chem. Phys., 18, 12269–12288, https://doi.org/10.5194/acp-18-12269-2018, https://doi.org/10.5194/acp-18-12269-2018, 2018
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This paper evaluates the capability of air-quality models to capture the observed relationship between surface ozone concentrations and meteorology over Europe. The air-quality models tended to overestimate the influence of maximum temperature and surface solar radiation. None of the air-quality models captured the strength of the observed relationship between ozone and relative humidity appropriately, underestimating the effect of relative humidity, a key factor in the ozone removal processes.
Piyush Bhardwaj, Manish Naja, Maheswar Rupakheti, Aurelia Lupascu, Andrea Mues, Arnico Kumar Panday, Rajesh Kumar, Khadak Singh Mahata, Shyam Lal, Harish C. Chandola, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 11949–11971, https://doi.org/10.5194/acp-18-11949-2018, https://doi.org/10.5194/acp-18-11949-2018, 2018
Short summary
Short summary
This study provides information about the regional variabilities in some of the pollutants using observations in Nepal and India. It is shown that agricultural crop residue burning leads to a significant enhancement in ozone and CO over a wider region. Further, the wintertime higher ozone levels are shown to be largely due to local emissions, while regional transport could be important in spring and hence shows the role of regional sources versus local sources in the Kathmandu Valley.
Tim Butler, Aurelia Lupascu, Jane Coates, and Shuai Zhu
Geosci. Model Dev., 11, 2825–2840, https://doi.org/10.5194/gmd-11-2825-2018, https://doi.org/10.5194/gmd-11-2825-2018, 2018
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This paper describes a method for determining origin of tropospheric ozone simulated in a global chemistry–climate model. This technique can show which precursor compounds were responsible for simulated ozone, and where they were emitted. In this paper we describe our technique, compare and contrast it with several other similar techniques, and use it to calculate the contribution of several different NOx and VOC precursor categories to the tropospheric ozone burden.
Erika von Schneidemesser, Boris Bonn, Tim M. Butler, Christian Ehlers, Holger Gerwig, Hannele Hakola, Heidi Hellén, Andreas Kerschbaumer, Dieter Klemp, Claudia Kofahl, Jürgen Kura, Anja Lüdecke, Rainer Nothard, Axel Pietsch, Jörn Quedenau, Klaus Schäfer, James J. Schauer, Ashish Singh, Ana-Maria Villalobos, Matthias Wiegner, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 8621–8645, https://doi.org/10.5194/acp-18-8621-2018, https://doi.org/10.5194/acp-18-8621-2018, 2018
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This paper provides an overview of the measurements done at an urban background site in Berlin from June-August of 2014. Results show that natural source contributions to ozone and particulate matter (PM) air pollutants are substantial. Large contributions of secondary aerosols formed in the atmosphere to PM10 concentrations were quantified. An analysis of the sources also identified contributions to PM from plant-based sources, vehicles, and a small contribution from wood burning.
Friderike Kuik, Andreas Kerschbaumer, Axel Lauer, Aurelia Lupascu, Erika von Schneidemesser, and Tim M. Butler
Atmos. Chem. Phys., 18, 8203–8225, https://doi.org/10.5194/acp-18-8203-2018, https://doi.org/10.5194/acp-18-8203-2018, 2018
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Modelled NOx concentrations are often underestimated compared to observations, and measurement studies show that reported NOx emissions in urban areas are often too low when the contribution from traffic is largest. This modelling study quantifies the underestimation of traffic NOx emissions in the Berlin–Brandenburg and finds that they are underestimated by ca. 50 % in the core urban area. More research is needed in order to more accurately understand real-world NOx emissions from traffic.
Andrea Mues, Axel Lauer, Aurelia Lupascu, Maheswar Rupakheti, Friderike Kuik, and Mark G. Lawrence
Geosci. Model Dev., 11, 2067–2091, https://doi.org/10.5194/gmd-11-2067-2018, https://doi.org/10.5194/gmd-11-2067-2018, 2018
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Augustin Colette, Camilla Andersson, Astrid Manders, Kathleen Mar, Mihaela Mircea, Maria-Teresa Pay, Valentin Raffort, Svetlana Tsyro, Cornelius Cuvelier, Mario Adani, Bertrand Bessagnet, Robert Bergström, Gino Briganti, Tim Butler, Andrea Cappelletti, Florian Couvidat, Massimo D'Isidoro, Thierno Doumbia, Hilde Fagerli, Claire Granier, Chris Heyes, Zig Klimont, Narendra Ojha, Noelia Otero, Martijn Schaap, Katarina Sindelarova, Annemiek I. Stegehuis, Yelva Roustan, Robert Vautard, Erik van Meijgaard, Marta Garcia Vivanco, and Peter Wind
Geosci. Model Dev., 10, 3255–3276, https://doi.org/10.5194/gmd-10-3255-2017, https://doi.org/10.5194/gmd-10-3255-2017, 2017
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The EURODELTA-Trends numerical experiment has been designed to assess the capability of chemistry-transport models to capture the evolution of surface air quality over the 1990–2010 period in Europe. It also includes sensitivity experiments in order to analyse the relative contribution of (i) emission changes, (ii) meteorological variability, and (iii) boundary conditions to air quality trends. The article is a detailed presentation of the experiment design and participating models.
Andrea Mues, Maheswar Rupakheti, Christoph Münkel, Axel Lauer, Heiko Bozem, Peter Hoor, Tim Butler, and Mark G. Lawrence
Atmos. Chem. Phys., 17, 8157–8176, https://doi.org/10.5194/acp-17-8157-2017, https://doi.org/10.5194/acp-17-8157-2017, 2017
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Ceilometer measurements taken in the Kathmandu Valley, Nepal, were used to study the temporal and spatial evolution of the mixing layer height in the valley. This provides important information on the vertical structure of the atmosphere and can thus also help to understand the mixing of air pollutants (e.g. black carbon) in the valley. The seasonal and diurnal cycles of the mixing layer were found to be highly dependent on meteorology and mainly anticorrelated to black carbon concentrations.
Friderike Kuik, Axel Lauer, Galina Churkina, Hugo A. C. Denier van der Gon, Daniel Fenner, Kathleen A. Mar, and Tim M. Butler
Geosci. Model Dev., 9, 4339–4363, https://doi.org/10.5194/gmd-9-4339-2016, https://doi.org/10.5194/gmd-9-4339-2016, 2016
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The study evaluates the performance of a setup of the Weather Research and Forecasting model with chemistry and aerosols (WRF–Chem) for the Berlin–Brandenburg region of Germany. Its sensitivity to updating urban input parameters based on structural data for Berlin is tested, specifying land use classes on a sub-grid scale, downscaling the original emissions to a resolution of ca. 1 km by 1 km for Berlin based on proxy data and model resolution.
Carolina Cavazos Guerra, Axel Lauer, Andreas B. Herber, Tim M. Butler, Annette Rinke, and Klaus Dethloff
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-942, https://doi.org/10.5194/acp-2016-942, 2016
Revised manuscript has not been submitted
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Accurate description of the Arctic atmosphere is a challenge for the modelling comunity. We evaluate the performance of the Weather Research and Forecast model (WRF) in the Eurasian Arctic and analyse the implications of data to initialise the model and a land surface scheme. The results show that biases can be related to the quality of data used and in the case of black carbon concentrations, to emission data. More long term measurements are need for model Validation in the area.
Kathleen A. Mar, Narendra Ojha, Andrea Pozzer, and Tim M. Butler
Geosci. Model Dev., 9, 3699–3728, https://doi.org/10.5194/gmd-9-3699-2016, https://doi.org/10.5194/gmd-9-3699-2016, 2016
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Ground-level ozone is an air pollutant with adverse effects on human and ecosystem health and is also a climate forcer with a significant warming effect. This paper presents the setup and evaluation of a model for ozone air quality over Europe. Within the model evaluation, we compare the use of two commonly used photochemical schemes, and we conclude that uncertainties in the representation of chemistry are important to consider when using air quality models for policy applications.
Jane Coates, Kathleen A. Mar, Narendra Ojha, and Tim M. Butler
Atmos. Chem. Phys., 16, 11601–11615, https://doi.org/10.5194/acp-16-11601-2016, https://doi.org/10.5194/acp-16-11601-2016, 2016
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This modelling study reproduced the non-linear relationship of ozone, NOx and temperature using various chemical mechanisms previously determined from observational studies. Under urban conditions, faster reaction rates rather than increased isoprene emissions led to a slightly greater increase of ozone with temperature using different NOx conditions. This study also shows that the increase of ozone with temperature is more sensitive to atmospheric mixing than the choice of chemical mechanism.
Boris Bonn, Erika von Schneidemesser, Dorota Andrich, Jörn Quedenau, Holger Gerwig, Anja Lüdecke, Jürgen Kura, Axel Pietsch, Christian Ehlers, Dieter Klemp, Claudia Kofahl, Rainer Nothard, Andreas Kerschbaumer, Wolfgang Junkermann, Rüdiger Grote, Tobias Pohl, Konradin Weber, Birgit Lode, Philipp Schönberger, Galina Churkina, Tim M. Butler, and Mark G. Lawrence
Atmos. Chem. Phys., 16, 7785–7811, https://doi.org/10.5194/acp-16-7785-2016, https://doi.org/10.5194/acp-16-7785-2016, 2016
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The distribution of air pollutants (gases and particles) have been investigated in different environments in Potsdam, Germany. Remarkable variations of the pollutants have been observed for distances of tens of meters by bicycles, vans and aircraft. Vegetated areas caused reductions depending on the pollutants, the vegetation type and dimensions. Our measurements show the pollutants to be of predominantly local origin, resulting in a huge challenge for common models to resolve.
A. Lupascu, R. Easter, R. Zaveri, M. Shrivastava, M. Pekour, J. Tomlinson, Q. Yang, H. Matsui, A. Hodzic, Q. Zhang, and J. D. Fast
Atmos. Chem. Phys., 15, 12283–12313, https://doi.org/10.5194/acp-15-12283-2015, https://doi.org/10.5194/acp-15-12283-2015, 2015
J. Coates and T. M. Butler
Atmos. Chem. Phys., 15, 8795–8808, https://doi.org/10.5194/acp-15-8795-2015, https://doi.org/10.5194/acp-15-8795-2015, 2015
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We show that simplified chemical mechanisms break down VOC into smaller sized degradation products on the first day faster than the near-explicit MCM chemical mechanism which would lead to an underprediction of ozone levels downwind of VOC emissions, and an underestimation of the VOC contribution to tropospheric background ozone when using simplified chemical mechanisms in regional or global modelling studies.
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Z. S. Stock, M. R. Russo, T. M. Butler, A. T. Archibald, M. G. Lawrence, P. J. Telford, N. L. Abraham, and J. A. Pyle
Atmos. Chem. Phys., 13, 12215–12231, https://doi.org/10.5194/acp-13-12215-2013, https://doi.org/10.5194/acp-13-12215-2013, 2013
S. M. Burrows, P. J. Rayner, T. Butler, and M. G. Lawrence
Atmos. Chem. Phys., 13, 5473–5488, https://doi.org/10.5194/acp-13-5473-2013, https://doi.org/10.5194/acp-13-5473-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
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
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
Do alternative inventories converge on the spatiotemporal representation of spring ammonia emissions in France?
Impacts of global NOx inversions on NO2 and ozone simulations
Reactive Organic Carbon Emissions from Volatile Chemical Products
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
A Comparison of Long-term Trends in Observations and Emission Inventories of NOx
The impact of weather patterns and related transport processes on aviation's contribution to ozone and methane concentrations from NOx emissions
Northwestward cropland expansion and growing urea-based fertilizer use enhanced NH3 emission loss in the contiguous United States
Technical note: On comparing greenhouse gas emission metrics
Impact of reduced anthropogenic emissions during COVID-19 on air quality in India
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
The impact of inhomogeneous emissions and topography on ozone photochemistry in the vicinity of the Hong Kong island
Meteorology-normalized impact of the COVID-19 lockdown upon NO2 pollution in Spain
Attribution of the accelerating increase in atmospheric methane during 2010–2018 by inverse analysis of GOSAT observations
Tropospheric ozone radiative forcing uncertainty due to pre-industrial fire and biogenic emissions
CRI-HOM: A novel chemical mechanism for simulating highly oxygenated organic molecules (HOMs) in global chemistry–aerosol–climate models
Global Impact of COVID-19 Restrictions on the Surface Concentrations of Nitrogen Dioxide and Ozone
Identifying forecast uncertainties for biogenic gases in the Po valley related to model configuration in EURAD-IM during PEGASOS 2012
The impact of ship emissions on air quality and human health in the Gothenburg area – Part II: Scenarios for 2040
Attribution of ground-level ozone to anthropogenic and natural sources of nitrogen oxides and reactive carbon in a global chemical transport model
Characterizing sources of high surface ozone events in the southwestern US with intensive field measurements and two global models
An inversion of NOx and non-methane volatile organic compound (NMVOC) emissions using satellite observations during the KORUS-AQ campaign and implications for surface ozone over East Asia
Influences of hydroxyl radicals (OH) on top-down estimates of the global and regional methane budgets
Evaluation of nitrogen oxides (NOx) sources and sinks and ozone production in Colombia and surrounding areas
The impact of biomass burning on upper tropospheric carbon monoxide: a study using MOCAGE global model and IAGOS airborne data
Temporal and spatial analysis of ozone concentrations in Europe based on timescale decomposition and a multi-clustering approach
Why is the Indo-Gangetic Plain the region with the largest NH3 column in the globe during pre-monsoon and monsoon seasons?
Improving the prediction of an atmospheric chemistry transport model using gradient-boosted regression trees
Inverse modelling of carbonyl sulfide: implementation, evaluation and implications for the global budget
Attributing ozone and its precursors to land transport emissions in Europe and Germany
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.
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.
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.
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.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1111, https://doi.org/10.5194/acp-2020-1111, 2020
Revised manuscript accepted for ACP
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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.
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.
Elena Macdonald, Noelia Otero Felipe, and Tim Butler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-951, https://doi.org/10.5194/acp-2020-951, 2020
Revised manuscript accepted for ACP
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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 with evaluating inaccuracies in emission inventories and with improving spatial imbalances in data availability.
Simon Rosanka, Christine Frömming, and Volker Grewe
Atmos. Chem. Phys., 20, 12347–12361, https://doi.org/10.5194/acp-20-12347-2020, https://doi.org/10.5194/acp-20-12347-2020, 2020
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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.
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.
Ian Enting and Nathan Clisby
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-996, https://doi.org/10.5194/acp-2020-996, 2020
Revised manuscript accepted for ACP
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We provide a new framework for comparing short-lived greenhouse
gases, using methane as an example, to long-lived greenhouse
gases such as carbon dioxide. 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.
Mengyuan Zhang, Apit Katiyar, Shengqiang Zhu, Juanyong Shen, Men Xia, Jinlong Ma, Sri Harsha Kota, Peng Wang, and Hongliang Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-903, https://doi.org/10.5194/acp-2020-903, 2020
Revised manuscript accepted for ACP
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We studied changes in air quality in India induced by the lockdown of COVID-19 through both surface observations and the CMAQ model. Our results show that emission reductions have improved the air quality across India during the lockdown. On average, the levels of PM2.5 and O3 have decreased by 28% and 15%, indicating positive effects of lockdown measures. We suggest that more stringent and localized emissions control strategies should be implemented in India to mitigate air pollutions.
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.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-877, https://doi.org/10.5194/acp-2020-877, 2020
Revised manuscript accepted for ACP
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Large-eddy simulations (LES) were performed in the mountainous region of the Hong Kong island 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.
Hervé Petetin, Dene Bowdalo, Albert Soret, Marc Guevara, Oriol Jorba, Kim Serradell, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 20, 11119–11141, https://doi.org/10.5194/acp-20-11119-2020, https://doi.org/10.5194/acp-20-11119-2020, 2020
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To control the spread of the COVID-19 coronavirus, the Spanish Government recently implemented a strict lockdown of the population, which strongly reduced the levels of nitrogen dioxide (NO2), one of the most critical air pollutants in Spain. This study quantifies the contribution of the lockdown on these reduced NO2 levels in Spain, taking the confounding effect of meteorology on artificial intelligence techniques into account.
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, Anthony A. Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-964, https://doi.org/10.5194/acp-2020-964, 2020
Revised manuscript accepted for ACP
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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 (Amazon, tropical Africa) and boreal wetlands (Eurasia), and tropical livestock (South Asia, Africa, Brazil), with no significant trend in oil/gas emissions. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
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. Discuss., https://doi.org/10.5194/acp-2020-685, https://doi.org/10.5194/acp-2020-685, 2020
Revised manuscript accepted for ACP
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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 compounding 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.
Annika Vogel and Hendrik Elbern
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-608, https://doi.org/10.5194/acp-2020-608, 2020
Revised manuscript accepted for ACP
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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.
Martin O. P. Ramacher, Lin Tang, Jana Moldanová, Volker Matthias, Matthias Karl, Erik Fridell, and Lasse Johansson
Atmos. Chem. Phys., 20, 10667–10686, https://doi.org/10.5194/acp-20-10667-2020, https://doi.org/10.5194/acp-20-10667-2020, 2020
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The effects of shipping emissions on air quality and health in the harbour city of Gothenburg were simulated for different scenarios for the year 2040 with coupled regional and city-scale chemistry transport models to evaluate the impact of regional emission regulations and onshore electricity for ships at berth. The results show that contributions of shipping to exposure and associated health impacts from particulate matter and NO2 decrease significantly compared to 2012 in all scenarios.
Tim Butler, Aurelia Lupascu, and Aditya Nalam
Atmos. Chem. Phys., 20, 10707–10731, https://doi.org/10.5194/acp-20-10707-2020, https://doi.org/10.5194/acp-20-10707-2020, 2020
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Ground-level ozone (O3) is not directly emitted; it is formed chemically in the atmosphere. Some ground-level O3 is transported from the stratosphere, but most O3 is produced from reactive precursors that are emitted by both natural and anthropogenic sources. We present the results of a novel source apportionment method for ground-level O3. Our results are consistent with previous work and also provide new insights. In particular, we highlight the roles of methane and international shipping.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546, https://doi.org/10.5194/acp-20-9525-2020, https://doi.org/10.5194/acp-20-9525-2020, 2020
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The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458, https://doi.org/10.5194/acp-20-9441-2020, https://doi.org/10.5194/acp-20-9441-2020, 2020
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Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Martin Cussac, Virginie Marécal, Valérie Thouret, Béatrice Josse, and Bastien Sauvage
Atmos. Chem. Phys., 20, 9393–9417, https://doi.org/10.5194/acp-20-9393-2020, https://doi.org/10.5194/acp-20-9393-2020, 2020
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Biomass burning emissions are a major source of carbon monoxide in the atmosphere. Here, the vertical transport that these emissions can undergo until the upper troposphere is investigated, as well as their contribution to carbon monoxide concentrations. It was found that boreal forest emissions were specific to the occurrence of pyroconvection directly above the fires, whereas biomass burning emissions from other regions of the globe relied more on the occurrence of deep convection.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tiantian Wang, Yu Song, Zhenying Xu, Mingxu Liu, Tingting Xu, Wenling Liao, Lifei Yin, Xuhui Cai, Ling Kang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 20, 8727–8736, https://doi.org/10.5194/acp-20-8727-2020, https://doi.org/10.5194/acp-20-8727-2020, 2020
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Satellite measurements have revealed that the Indo-Gangetic Plain (IGP) has the global maximum ammonia concentrations, with a peak from June to August. Here, we studied the reasons for this phenomenon through computer simulations. Low sulfur dioxide and nitrogen oxides emissions and high air temperature over the IGP weaken the swallowing of gaseous ammonia by acidic gases. Additionally, the barrier effects of the Himalayas, like a windshield, are also conducive to the accumulation of ammonia.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
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. Discuss., https://doi.org/10.5194/acp-2020-603, https://doi.org/10.5194/acp-2020-603, 2020
Revised manuscript accepted for ACP
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimate gross primary productivity in ecosystem, 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 tropics and more uptake in high latitudes. We also stress on the necessity of more ground-based observations and satellite data assimilation in future.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873, https://doi.org/10.5194/acp-20-7843-2020, https://doi.org/10.5194/acp-20-7843-2020, 2020
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We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
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