Articles | Volume 18, issue 12
Atmos. Chem. Phys., 18, 9091–9106, 2018
https://doi.org/10.5194/acp-18-9091-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 18, 9091–9106, 2018
https://doi.org/10.5194/acp-18-9091-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
28 Jun 2018
Research article
| 28 Jun 2018
Long-term trends in total inorganic nitrogen and sulfur deposition in the US from 1990 to 2010
Yuqiang Zhang et al.
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Previous studies showed that black carbon (BC) could warm the surface with decreased incoming radiation. With climate models, we found that the surface energy redistribution plays a more crucial role in surface temperature compared with other forcing agents. Though BC could reduce the surface heating, the energy dissipates less efficiently, which is manifested by reduced convective and evaporative cooling, thereby warming the surface.
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Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
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Tao Tang, Drew Shindell, Yuqiang Zhang, Apostolos Voulgarakis, Jean-Francois Lamarque, Gunnar Myhre, Gregory Faluvegi, Bjørn H. Samset, Timothy Andrews, Dirk Olivié, Toshihiko Takemura, and Xuhui Lee
Atmos. Chem. Phys., 21, 13797–13809, https://doi.org/10.5194/acp-21-13797-2021, https://doi.org/10.5194/acp-21-13797-2021, 2021
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Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Geosci. Model Dev., 14, 5751–5768, https://doi.org/10.5194/gmd-14-5751-2021, https://doi.org/10.5194/gmd-14-5751-2021, 2021
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The Community Multiscale Air Quality (CMAQ) modeling system extended for hemispheric-scale applications (H-CMAQ) incorporated the satellite-constrained degassing SO2 emissions from 50 volcanos across the Northern Hemisphere. The impact on tropospheric sulfate aerosol (SO42−) is assessed for 2010. Although the considered volcanic emissions occurred at or below the middle of free troposphere (500 hPa), SO42− enhancements of more than 10 % were detected up to the top of free troposphere (250 hPa).
Lin Huang, Song Liu, Zeyuan Yang, Jia Xing, Jia Zhang, Jiang Bian, Siwei Li, Shovan Kumar Sahu, Shuxiao Wang, and Tie-Yan Liu
Geosci. Model Dev., 14, 4641–4654, https://doi.org/10.5194/gmd-14-4641-2021, https://doi.org/10.5194/gmd-14-4641-2021, 2021
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Accurate estimation of emissions is a prerequisite for effectively controlling air pollution, but current methods lack either sufficient data or a representation of nonlinearity. Here, we proposed a novel deep learning method to model the dual relationship between emissions and pollutant concentrations. Emissions can be updated by back-propagating the gradient of the loss function measuring the deviation between simulations and observations, resulting in better model performance.
Zhe Jiang, Hongrong Shi, Bin Zhao, Yu Gu, Yifang Zhu, Kazuyuki Miyazaki, Xin Lu, Yuqiang Zhang, Kevin W. Bowman, Takashi Sekiya, and Kuo-Nan Liou
Atmos. Chem. Phys., 21, 8693–8708, https://doi.org/10.5194/acp-21-8693-2021, https://doi.org/10.5194/acp-21-8693-2021, 2021
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We use the COVID-19 pandemic as a unique natural experiment to obtain a more robust understanding of the effectiveness of emission reductions toward air quality improvement by combining chemical transport simulations and observations. Our findings imply a shift from current control policies in California: a strengthened control on primary PM2.5 emissions and a well-balanced control on NOx and volatile organic compounds are needed to effectively and sustainably alleviate PM2.5 and O3 pollution.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
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K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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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.
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.
Huiying Luo, Marina Astitha, Christian Hogrefe, Rohit Mathur, and S. Trivikrama Rao
Atmos. Chem. Phys., 20, 13801–13815, https://doi.org/10.5194/acp-20-13801-2020, https://doi.org/10.5194/acp-20-13801-2020, 2020
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A new method is introduced to evaluate nonlinear, nonstationary modeled PM2.5 time series by decomposing decadal PM2.5 concentrations and its species onto various timescales. It does not require preselection of temporal scales and assumptions of linearity and stationarity. It provides a unique opportunity to assess the influence of each species on total PM2.5. The results reveal a phase shift in modeled EC/OC concentrations, indicating the need for improved model treatment of organic aerosols.
Tao Tang, Drew Shindell, Yuqiang Zhang, Apostolos Voulgarakis, Jean-Francois Lamarque, Gunnar Myhre, Camilla W. Stjern, Gregory Faluvegi, and Bjørn H. Samset
Atmos. Chem. Phys., 20, 8251–8266, https://doi.org/10.5194/acp-20-8251-2020, https://doi.org/10.5194/acp-20-8251-2020, 2020
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By using climate simulations, we found that both CO2 and black carbon aerosols could reduce low-level cloud cover, which is mainly due to changes in relative humidity, cloud water, dynamics, and stability. Because the impact of cloud on solar radiation is in effect only during daytime, such cloud reduction could enhance solar heating, thereby raising the daily maximum temperature by 10–50 %, varying by region, which has great implications for extreme climate events and socioeconomic activity.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, and Yang Zhang
Atmos. Chem. Phys., 20, 3373–3396, https://doi.org/10.5194/acp-20-3373-2020, https://doi.org/10.5194/acp-20-3373-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 1, modeled ozone is evaluated with observations at surface, by ozonesonde and airplane, and by satellite across the Northern Hemisphere. In addition, a newly developed air mass characterization method to estimate stratospheric intrusion is presented.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Atmos. Chem. Phys., 20, 3397–3413, https://doi.org/10.5194/acp-20-3397-2020, https://doi.org/10.5194/acp-20-3397-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 2, the higher-order decoupled direct method (HDDM) is applied to investigate the emission impacts from east Asia and the US during April 2010. Furthermore, changes in trans-Pacific transport caused by the recent emissions are examined.
S. Trivikrama Rao, Huiying Luo, Marina Astitha, Christian Hogrefe, Valerie Garcia, and Rohit Mathur
Atmos. Chem. Phys., 20, 1627–1639, https://doi.org/10.5194/acp-20-1627-2020, https://doi.org/10.5194/acp-20-1627-2020, 2020
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Since numerical air quality models do not explicitly simulate stochastic variations in the atmosphere, there will always be differences between modeled and measured pollutant levels even when the model's physics, chemistry, numerical analysis, and its input data are perfect. This paper quantifies the inherent uncertainty in regional models due to the stochastic nature of the atmosphere. A knowledge of the expected error helps model developers in evaluating the real progress in improving models.
Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy
Atmos. Chem. Phys., 20, 1497–1505, https://doi.org/10.5194/acp-20-1497-2020, https://doi.org/10.5194/acp-20-1497-2020, 2020
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We quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Meteorological conditions over the study period would have led to an increase of haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate.
Jia Xing, Dian Ding, Shuxiao Wang, Zhaoxin Dong, James T. Kelly, Carey Jang, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 19, 13627–13646, https://doi.org/10.5194/acp-19-13627-2019, https://doi.org/10.5194/acp-19-13627-2019, 2019
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The study aims at addressing the challenge in efficient quantification of the nonlinear response of air pollution to precursor emission perturbations. The newly developed observable response indicators can be easily calculated by a combination of ambient concentrations of certain species. Their capability in representing the spatial and temporal variation in PM2.5 and O3 chemistry has also been well evaluated and applied in China.
Daiwen Kang, Kristen M. Foley, Rohit Mathur, Shawn J. Roselle, Kenneth E. Pickering, and Dale J. Allen
Geosci. Model Dev., 12, 4409–4424, https://doi.org/10.5194/gmd-12-4409-2019, https://doi.org/10.5194/gmd-12-4409-2019, 2019
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This paper provides a comprehensive evaluation of the lightning production schemes in CMAQ as described in https://www.geosci-model-dev.net/12/3071/2019/gmd-12-3071-2019.html on model performance. The impact of lightning NOx from different schemes is evaluated in time and space using both ground–level network measurements and aloft (ozonesonde and aircraft) observations. These results provide users the benchmark model performance when the lightning NOx production schemes are applied.
Daiwen Kang, Kenneth E. Pickering, Dale J. Allen, Kristen M. Foley, David C. Wong, Rohit Mathur, and Shawn J. Roselle
Geosci. Model Dev., 12, 3071–3083, https://doi.org/10.5194/gmd-12-3071-2019, https://doi.org/10.5194/gmd-12-3071-2019, 2019
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Lightning strikes produce significant amount of nitrogen oxides and the resulting atmospheric chemistry causes one of the primary air pollutants, ground-level ozone, to change. In this paper, we documented the evolution of scientific updates for lightning-induced nitrogen oxides schemes in the CMAQ model. The updated observation-based schemes are good for retrospective applications, while the parameterized scheme can estimate lightning nitrogen oxides for applications without observations.
Xionghui Qiu, Qi Ying, Shuxiao Wang, Lei Duan, Jian Zhao, Jia Xing, Dian Ding, Yele Sun, Baoxian Liu, Aijun Shi, Xiao Yan, Qingcheng Xu, and Jiming Hao
Atmos. Chem. Phys., 19, 6737–6747, https://doi.org/10.5194/acp-19-6737-2019, https://doi.org/10.5194/acp-19-6737-2019, 2019
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Current chemical transport models cannot capture the diurnal and nocturnal variation in atmospheric nitrate, which may be relative to the missing atmospheric chlorine chemistry. In this work, the Community Multiscale Air Quality (CMAQ) model with improved chlorine heterogeneous chemistry is applied to simulate the impact of chlorine chemistry on summer nitrate concentrations in Beijing. The results of this work can improve our understanding of nitrate formation.
Quazi Z. Rasool, Jesse O. Bash, and Daniel S. Cohan
Geosci. Model Dev., 12, 849–878, https://doi.org/10.5194/gmd-12-849-2019, https://doi.org/10.5194/gmd-12-849-2019, 2019
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Soils have been overlooked as a source of reactive nitrogen (N) emissions that are pronounced in the summer ozone season (growing season) and increasingly important as fertilizer use grows, while fossil fuel combustion sources of N decline. Mechanistic process models of soil N emissions are used in Earth science and soil biogeochemical modeling on a site scale. This work mechanistically models soil N emissions for the first time on a regional scale to better understand their air quality impacts.
Gabriele Curci, Ummugulsum Alyuz, Rocio Barò, Roberto Bianconi, Johannes Bieser, Jesper H. Christensen, Augustin Colette, Aidan Farrow, Xavier Francis, Pedro Jiménez-Guerrero, Ulas Im, Peng Liu, Astrid Manders, Laura Palacios-Peña, Marje Prank, Luca Pozzoli, Ranjeet Sokhi, Efisio Solazzo, Paolo Tuccella, Alper Unal, Marta G. Vivanco, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 19, 181–204, https://doi.org/10.5194/acp-19-181-2019, https://doi.org/10.5194/acp-19-181-2019, 2019
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Atmospheric carbonaceous aerosols are able to absorb solar radiation and they continue to contribute some of the largest uncertainties in projected climate change. One important detail is how the chemical species are arranged inside each particle, i.e. the knowledge of their mixing state. We use an ensemble of regional model simulations to test different mixing state assumptions and found that a combination of internal and external mixing may better reproduce sunphotometer observations.
Peng Liu, Christian Hogrefe, Ulas Im, Jesper H. Christensen, Johannes Bieser, Uarporn Nopmongcol, Greg Yarwood, Rohit Mathur, Shawn Roselle, and Tanya Spero
Atmos. Chem. Phys., 18, 17157–17175, https://doi.org/10.5194/acp-18-17157-2018, https://doi.org/10.5194/acp-18-17157-2018, 2018
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This study represents an intercomparison of four regional-scale air quality simulations in order to understand the model similarities and differences in estimating the impact of ozone imported from outside of the US on the surface ozone within the US at process level. Vertical turbulent mixing stands out as a primary contributor to the model differences in inert tracers.
Yuqiang Zhang, J. Jason West, Rohit Mathur, Jia Xing, Christian Hogrefe, Shawn J. Roselle, Jesse O. Bash, Jonathan E. Pleim, Chuen-Meei Gan, and David C. Wong
Atmos. Chem. Phys., 18, 15003–15016, https://doi.org/10.5194/acp-18-15003-2018, https://doi.org/10.5194/acp-18-15003-2018, 2018
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Here we use a fine-resolution (36 km) self-consistent 21-year air quality simulation from 1990 to 2010, a health impact function, and annual county-level population and baseline mortality rate estimates to estimate annual mortality burdens from PM2.5 and O3 in the US, and also the contributions to the trends. We found that the PM2.5-related mortality burden has steadily decreased by 53 %, while the O3-related mortality burden has increased by 13 %, with larger inter-annual variabilities.
Marina Astitha, Ioannis Kioutsioukis, Ghezae Araya Fisseha, Roberto Bianconi, Johannes Bieser, Jesper H. Christensen, Owen R. Cooper, Stefano Galmarini, Christian Hogrefe, Ulas Im, Bryan Johnson, Peng Liu, Uarporn Nopmongcol, Irina Petropavlovskikh, Efisio Solazzo, David W. Tarasick, and Greg Yarwood
Atmos. Chem. Phys., 18, 13925–13945, https://doi.org/10.5194/acp-18-13925-2018, https://doi.org/10.5194/acp-18-13925-2018, 2018
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This work is unique in the detailed analyses of modeled ozone vertical profiles from sites in North America through the collaboration of four research groups from the US and EU. We assess the air quality models' performance and model inter-comparison for ozone vertical profiles and stratospheric ozone intrusions. Lastly, we designate the important role of lateral boundary conditions in the ozone vertical profiles using chemically inert tracers.
Marta G. Vivanco, Mark R. Theobald, Héctor García-Gómez, Juan Luis Garrido, Marje Prank, Wenche Aas, Mario Adani, Ummugulsum Alyuz, Camilla Andersson, Roberto Bellasio, Bertrand Bessagnet, Roberto Bianconi, Johannes Bieser, Jørgen Brandt, Gino Briganti, Andrea Cappelletti, Gabriele Curci, Jesper H. Christensen, Augustin Colette, Florian Couvidat, Cornelis Cuvelier, Massimo D'Isidoro, Johannes Flemming, Andrea Fraser, Camilla Geels, Kaj M. Hansen, Christian Hogrefe, Ulas Im, Oriol Jorba, Nutthida Kitwiroon, Astrid Manders, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Luca Pozzoli, Efisio Solazzo, Svetlana Tsyro, Alper Unal, Peter Wind, and Stefano Galmarini
Atmos. Chem. Phys., 18, 10199–10218, https://doi.org/10.5194/acp-18-10199-2018, https://doi.org/10.5194/acp-18-10199-2018, 2018
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European wet and dry atmospheric deposition of N and S estimated by 14 air quality models was found to vary substantially. An ensemble of models meeting acceptability criteria was used to estimate the exceedances of the critical loads for N in habitats within the Natura 2000 network, as well as their lower and upper limits. Scenarios with 20 % emission reductions in different regions of the world showed that European emissions are responsible for most of the N and S deposition in Europe.
Ulas Im, Jesper Heile Christensen, Camilla Geels, Kaj Mantzius Hansen, Jørgen Brandt, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Rocio Baro, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Augustin Colette, Gabriele Curci, Aidan Farrow, Johannes Flemming, Andrea Fraser, Pedro Jimenez-Guerrero, Nutthida Kitwiroon, Peng Liu, Uarporn Nopmongcol, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marje Prank, Rebecca Rose, Ranjeet Sokhi, Paolo Tuccella, Alper Unal, Marta G. Vivanco, Greg Yarwood, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 18, 8929–8952, https://doi.org/10.5194/acp-18-8929-2018, https://doi.org/10.5194/acp-18-8929-2018, 2018
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We evaluate the impact of global and regional anthropogenic emission reductions on major air pollutant levels over Europe and North America, using a multi-model ensemble of regional chemistry and transport models. Results show that ozone levels are largely driven by long-range transport over both continents while other pollutants such as carbon monoxide or aerosols are mainly controlled by domestic sources. Use of multi-model ensembles can help to reduce the uncertainties in individual models.
Stefano Galmarini, Ioannis Kioutsioukis, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Roberto Bellasio, Anna M. K. Benedictow, Roberto Bianconi, Johannes Bieser, Joergen Brandt, Jesper H. Christensen, Augustin Colette, Gabriele Curci, Yanko Davila, Xinyi Dong, Johannes Flemming, Xavier Francis, Andrea Fraser, Joshua Fu, Daven K. Henze, Christian Hogrefe, Ulas Im, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Jan Eiof Jonson, Nutthida Kitwiroon, Astrid Manders, Rohit Mathur, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marie Prank, Martin Schultz, Rajeet S. Sokhi, Kengo Sudo, Paolo Tuccella, Toshihiko Takemura, Takashi Sekiya, and Alper Unal
Atmos. Chem. Phys., 18, 8727–8744, https://doi.org/10.5194/acp-18-8727-2018, https://doi.org/10.5194/acp-18-8727-2018, 2018
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An ensemble of model results relating to ozone concentrations in Europe in 2010 has been produced and studied. The novelty consists in the fact that the ensemble is made of results of models working at two different scales (regional and global), therefore contributing in detail two different parts of the atmospheric spectrum. The ensemble defined as a hybrid has been studied in detail and shown to bring additional value to the assessment of air quality.
Jia Xing, Dian Ding, Shuxiao Wang, Bin Zhao, Carey Jang, Wenjing Wu, Fenfen Zhang, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 18, 7799–7814, https://doi.org/10.5194/acp-18-7799-2018, https://doi.org/10.5194/acp-18-7799-2018, 2018
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NOx is the common precursor for both PM2.5 and O3 pollution, while the effectiveness of NOx controls for reducing PM2.5 and O3 are largely influenced by the ambient levels of NH3 and VOCs. This study developed a new method to quantify the nonlinear effectiveness of emission controls for reducing PM2.5 and O3. The new method not only substantially reduces the computational burden but also provides a series of quantitative indicators to quantify the nonlinear control effectiveness.
Ulas Im, Jørgen Brandt, Camilla Geels, Kaj Mantzius Hansen, Jesper Heile Christensen, Mikael Skou Andersen, Efisio Solazzo, Ioannis Kioutsioukis, Ummugulsum Alyuz, Alessandra Balzarini, Rocio Baro, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Augustin Colette, Gabriele Curci, Aidan Farrow, Johannes Flemming, Andrea Fraser, Pedro Jimenez-Guerrero, Nutthida Kitwiroon, Ciao-Kai Liang, Uarporn Nopmongcol, Guido Pirovano, Luca Pozzoli, Marje Prank, Rebecca Rose, Ranjeet Sokhi, Paolo Tuccella, Alper Unal, Marta Garcia Vivanco, Jason West, Greg Yarwood, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 18, 5967–5989, https://doi.org/10.5194/acp-18-5967-2018, https://doi.org/10.5194/acp-18-5967-2018, 2018
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The impacts of air pollution on human health and their costs in Europe and the United States for the year 2010 ared modeled by a multi-model ensemble. In Europe, the number of premature deaths is calculated to be 414 000, while in the US it is estimated to be 160 000. Health impacts estimated by individual models can vary up to a factor of 3. Results show that the domestic emissions have the largest impact on premature deaths, compared to foreign sources.
Christian Hogrefe, Peng Liu, George Pouliot, Rohit Mathur, Shawn Roselle, Johannes Flemming, Meiyun Lin, and Rokjin J. Park
Atmos. Chem. Phys., 18, 3839–3864, https://doi.org/10.5194/acp-18-3839-2018, https://doi.org/10.5194/acp-18-3839-2018, 2018
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This study quantifies the impacts of different representations of background ozone in state-of-the-science large-scale models on surface and aloft ozone burdens simulated by the CMAQ regional model over the United States. It also compares both the CMAQ simulations and the driving large-scale models to surface and upper air observations.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Rohit Mathur, Jia Xing, Robert Gilliam, Golam Sarwar, Christian Hogrefe, Jonathan Pleim, George Pouliot, Shawn Roselle, Tanya L. Spero, David C. Wong, and Jeffrey Young
Atmos. Chem. Phys., 17, 12449–12474, https://doi.org/10.5194/acp-17-12449-2017, https://doi.org/10.5194/acp-17-12449-2017, 2017
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We extend CMAQ's applicability to the entire Northern Hemisphere to enable consistent examination of interactions between atmospheric processes occurring on various spatial and temporal scales. Improvements were made in model process representation, structure, and input data sets that enable a range of model applications including episodic intercontinental pollutant transport, long-term trends in air pollution across the Northern Hemisphere, and air pollution–climate interactions.
Efisio Solazzo, Christian Hogrefe, Augustin Colette, Marta Garcia-Vivanco, and Stefano Galmarini
Atmos. Chem. Phys., 17, 10435–10465, https://doi.org/10.5194/acp-17-10435-2017, https://doi.org/10.5194/acp-17-10435-2017, 2017
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The work here is conducted within the frame of AQMEII3 and promotes the use of diagnostic methods for the evaluation of air quality models. We highlight the need to move away from aggregated error metrics and to focus on the quality of the information that can be extracted from the model and the observation. This aids the understanding of the causes of model error, providing more useful information to model developers and users than can be gained from common evaluations.
Jia Xing, Jiandong Wang, Rohit Mathur, Shuxiao Wang, Golam Sarwar, Jonathan Pleim, Christian Hogrefe, Yuqiang Zhang, Jingkun Jiang, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 17, 9869–9883, https://doi.org/10.5194/acp-17-9869-2017, https://doi.org/10.5194/acp-17-9869-2017, 2017
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The assessment of the impacts of aerosol direct effects (ADE) is important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particulate matter and ozone. This study quantifies the ADE impacts on tropospheric ozone by using a two-way coupled meteorology and atmospheric chemistry model. Results suggest that reducing ADE may have the potential risk of increasing ozone in winter, but it will benefit the reduction of maxima ozone in summer.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Efisio Solazzo, Roberto Bianconi, Christian Hogrefe, Gabriele Curci, Paolo Tuccella, Ummugulsum Alyuz, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Johannes Bieser, Jørgen Brandt, Jesper H. Christensen, Augistin Colette, Xavier Francis, Andrea Fraser, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Ulas Im, Astrid Manders, Uarporn Nopmongcol, Nutthida Kitwiroon, Guido Pirovano, Luca Pozzoli, Marje Prank, Ranjeet S. Sokhi, Alper Unal, Greg Yarwood, and Stefano Galmarini
Atmos. Chem. Phys., 17, 3001–3054, https://doi.org/10.5194/acp-17-3001-2017, https://doi.org/10.5194/acp-17-3001-2017, 2017
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As part of the third phase of AQMEII, this study uses timescale analysis to apportion error to the responsible processes, detect causes of model error, and identify the processes and scales that require dedicated investigations. The analysis tackles model performance gauging through measurement-to-model comparison, error decomposition, and time series analysis of model biases for ozone, CO, SO2, NO, NO2, PM10, PM2.5, wind speed, and temperature over Europe and North America.
Stefano Galmarini, Brigitte Koffi, Efisio Solazzo, Terry Keating, Christian Hogrefe, Michael Schulz, Anna Benedictow, Jan Jurgen Griesfeller, Greet Janssens-Maenhout, Greg Carmichael, Joshua Fu, and Frank Dentener
Atmos. Chem. Phys., 17, 1543–1555, https://doi.org/10.5194/acp-17-1543-2017, https://doi.org/10.5194/acp-17-1543-2017, 2017
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We present an overview of the coordinated global numerical modelling experiments performed during 2012–2016 by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP), the regional experiments by the Air Quality Model Evaluation International Initiative (AQMEII) over Europe and North America, and the Model Intercomparison Study for Asia (MICS-Asia). Given the organizational complexity of bringing together these three initiatives, the experiment organization is presented.
Ioannis Kioutsioukis, Ulas Im, Efisio Solazzo, Roberto Bianconi, Alba Badia, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Dominik Brunner, Charles Chemel, Gabriele Curci, Hugo Denier van der Gon, Johannes Flemming, Renate Forkel, Lea Giordano, Pedro Jiménez-Guerrero, Marcus Hirtl, Oriol Jorba, Astrid Manders-Groot, Lucy Neal, Juan L. Pérez, Guidio Pirovano, Roberto San Jose, Nicholas Savage, Wolfram Schroder, Ranjeet S. Sokhi, Dimiter Syrakov, Paolo Tuccella, Johannes Werhahn, Ralf Wolke, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 16, 15629–15652, https://doi.org/10.5194/acp-16-15629-2016, https://doi.org/10.5194/acp-16-15629-2016, 2016
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Four ensemble methods are applied to two annual AQMEII datasets and their performance is compared for O3, NO2 and PM10. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill at each station over the single models and the ensemble mean. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way.
Quazi Z. Rasool, Rui Zhang, Benjamin Lash, Daniel S. Cohan, Ellen J. Cooter, Jesse O. Bash, and Lok N. Lamsal
Geosci. Model Dev., 9, 3177–3197, https://doi.org/10.5194/gmd-9-3177-2016, https://doi.org/10.5194/gmd-9-3177-2016, 2016
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This study updates the representation of soil NO emissions in a regional air quality model. The implementation enhances the representation of biome types and dynamic fertilizer use. Previous modeling of soil NO in CMAQ had tended to under-estimate emissions and misrepresent their response to soil conditions and meteorology. We evaluate results against satellite observations of NO2, and quantify the impacts of the new parameterization on simulations of ozone and particulate matter.
Jia Xing, Rohit Mathur, Jonathan Pleim, Christian Hogrefe, Jiandong Wang, Chuen-Meei Gan, Golam Sarwar, David C. Wong, and Stuart McKeen
Atmos. Chem. Phys., 16, 10865–10877, https://doi.org/10.5194/acp-16-10865-2016, https://doi.org/10.5194/acp-16-10865-2016, 2016
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Downward transport of ozone from the stratosphere has large impacts on surface concentration and needs to be properly represented in regional models. This study developed a seasonally and spatially varying PV-based function from an investigation of the relationship between PV and O3. The implementation of the new function significantly improves the model's performance in O3 simulation, which enables a more accurate simulation of the vertical distribution of O3 across the Northern Hemisphere.
Yuqiang Zhang, Jared H. Bowden, Zachariah Adelman, Vaishali Naik, Larry W. Horowitz, Steven J. Smith, and J. Jason West
Atmos. Chem. Phys., 16, 9533–9548, https://doi.org/10.5194/acp-16-9533-2016, https://doi.org/10.5194/acp-16-9533-2016, 2016
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Reducing greenhouse gas (GHG) emissions can also improve air quality. We estimate the co-benefits of global GHG mitigation for US air quality in 2050 at fine resolution by downscaling from a previous global study. Foreign GHG mitigation under RCP4.5 contributes more to the US O3 reduction (76 % of the total) than domestic mitigation and contributes 26 % of the PM2.5 reduction. Therefore, the US gains significantly greater air quality co-benefits by coordinating GHG controls internationally.
Jesse O. Bash, Kirk R. Baker, and Melinda R. Beaver
Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, https://doi.org/10.5194/gmd-9-2191-2016, 2016
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Biogenic volatile organic compounds (BVOCs) participate in reactions that can lead to secondarily formed ozone and particulate matter impacting air quality and climate and are important inputs for atmospheric models. BVOC emissions are sensitive to the vegetation species and leaf temperature. Here, we have improved the vegetation data and modeled leaf temperature of the Biogenic Emission Inventory System model. Updated algorithms improved model evaluation against observations in California.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
B. Gantt, J. T. Kelly, and J. O. Bash
Geosci. Model Dev., 8, 3733–3746, https://doi.org/10.5194/gmd-8-3733-2015, https://doi.org/10.5194/gmd-8-3733-2015, 2015
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, D. Wong, R. Gilliam, and C. Wei
Atmos. Chem. Phys., 15, 12193–12209, https://doi.org/10.5194/acp-15-12193-2015, https://doi.org/10.5194/acp-15-12193-2015, 2015
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This study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act especially on trends in solar radiation. Comparisons of model results with observations of aerosol optical depth, aerosol concentration, and radiation demonstrate that the coupled WRF-CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD.
Y. Zhou, H. Mao, K. Demerjian, C. Hogrefe, and J. Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-27253-2015, https://doi.org/10.5194/acpd-15-27253-2015, 2015
Revised manuscript not accepted
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Baseline carbon monoxide (CO) and ozone (O3) were studied at seven rural sites in the Northeast U.S. during varying periods over 2001 – 2010. Baseline CO at all sites decreased significantly at a rate between -4.3 – -2.3 ppbv yr-1, while baseline O3 was relatively constant. Interannual and seasonal variations of baseline CO and O3 were related to increasing Asian emissions, NOx emissions reduction in urban areas, global biomass burning emissions, and meteorological conditions.
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, and C. Wei
Atmos. Chem. Phys., 15, 9997–10018, https://doi.org/10.5194/acp-15-9997-2015, https://doi.org/10.5194/acp-15-9997-2015, 2015
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The ability of a coupled meteorology-chemistry model (WRF-CMAQ) to reproduce the historical trend in AOD and clear-sky SWR over the N. Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Questions of how well the model represents the regional and temporal variability of aerosol burden and DRE, and whether the model is able to capture past trends in aerosol loading and associated radiation effects, will be addressed.
X. Fu, S. X. Wang, L. M. Ran, J. E. Pleim, E. Cooter, J. O. Bash, V. Benson, and J. M. Hao
Atmos. Chem. Phys., 15, 6637–6649, https://doi.org/10.5194/acp-15-6637-2015, https://doi.org/10.5194/acp-15-6637-2015, 2015
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In this study, we estimate, for the first time, the NH3 emission from the agricultural fertilizer application in China online using the bi-directional CMAQ model coupled to an agro-ecosystem model. Compared with previous researches, this method considers more influencing factors, such as meteorological fields, soil and the fertilizer application, and provides improved NH3 emission with higher spatial and temporal resolution.
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, C. Wei, R. Gilliam, and G. Pouliot
Atmos. Chem. Phys., 15, 2723–2747, https://doi.org/10.5194/acp-15-2723-2015, https://doi.org/10.5194/acp-15-2723-2015, 2015
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Model-simulated air quality trends over the past 2 decades largely agree with those derived from observations. In the relative amounts of VOC and NOx emission controls in different regions across the northern hemisphere have led to significantly different trends in tropospheric O3. Differences in the historical changes in the relative amounts of NH3, NOx and SO2 emissions also impact the trends in inorganic particulate matter amounts and composition in China, the U.S. and Europe.
S. Yu, R. Mathur, J. Pleim, D. Wong, R. Gilliam, K. Alapaty, C. Zhao, and X. Liu
Atmos. Chem. Phys., 14, 11247–11285, https://doi.org/10.5194/acp-14-11247-2014, https://doi.org/10.5194/acp-14-11247-2014, 2014
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, S. Roselle, and C. Wei
Atmos. Chem. Phys., 14, 1701–1715, https://doi.org/10.5194/acp-14-1701-2014, https://doi.org/10.5194/acp-14-1701-2014, 2014
G. Sarwar, J. Godowitch, B. H. Henderson, K. Fahey, G. Pouliot, W. T. Hutzell, R. Mathur, D. Kang, W. S. Goliff, and W. R. Stockwell
Atmos. Chem. Phys., 13, 9695–9712, https://doi.org/10.5194/acp-13-9695-2013, https://doi.org/10.5194/acp-13-9695-2013, 2013
J. Xing, J. Pleim, R. Mathur, G. Pouliot, C. Hogrefe, C.-M. Gan, and C. Wei
Atmos. Chem. Phys., 13, 7531–7549, https://doi.org/10.5194/acp-13-7531-2013, https://doi.org/10.5194/acp-13-7531-2013, 2013
J. O. Bash, E. J. Cooter, R. L. Dennis, J. T. Walker, and J. E. Pleim
Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, https://doi.org/10.5194/bg-10-1635-2013, 2013
J. T. Walker, M. R. Jones, J. O. Bash, L. Myles, T. Meyers, D. Schwede, J. Herrick, E. Nemitz, and W. Robarge
Biogeosciences, 10, 981–998, https://doi.org/10.5194/bg-10-981-2013, https://doi.org/10.5194/bg-10-981-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Observation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, China
A machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019
Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurements
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizations
The impacts of marine-emitted halogens on OH radicals in East Asia during summer
Impact of eastern and central Pacific El Niño on lower tropospheric ozone in China
Contribution of Asian emissions to upper tropospheric CO over the remote Pacific
An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018
Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism construction
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Quantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversion
Model evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model study
Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products
A model for simultaneous evaluation of NO2, O3 and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysis
Influence of photochemical loss of volatile organic compounds on understanding ozone formation mechanism
North China Plain as a hot spot of ozone pollution exacerbated by extreme high temperatures
Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants
Impact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphere
Influence of total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODEs) in the Antarctic
Changes in anthropogenic precursor emissions drive shifts in the ozone seasonal cycle throughout the northern midlatitude troposphere
Amplified role of potential HONO sources in O3 formation in North China Plain during autumn haze aggravating processes
Improving NOX emissions in Beijing using network observations and a novel perturbed emissions ensemble
Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017
Surface ozone impacts on major crop production in China from 2010 to 2017
Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in China
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
Tropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathways
An integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulations
An assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonyls
Methane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observations
Evaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System Model
Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models
Ozone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescales
Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI
Model Output Statistics (MOS) applied to CAMS O3 forecasts: trade-offs between continuous and categorical skill scores
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Improving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaign
Atmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)
Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2
Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mapping
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Impact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model results
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation
Technical note: Entrainment-limited kinetics of bimolecular reactions in clouds
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416, https://doi.org/10.5194/acp-22-8403-2022, https://doi.org/10.5194/acp-22-8403-2022, 2022
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285, https://doi.org/10.5194/acp-22-7273-2022, https://doi.org/10.5194/acp-22-7273-2022, 2022
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This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981, https://doi.org/10.5194/acp-22-5961-2022, https://doi.org/10.5194/acp-22-5961-2022, 2022
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Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
EGUsphere, https://doi.org/10.5194/egusphere-2022-117, https://doi.org/10.5194/egusphere-2022-117, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easy interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants even when having missing data.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Le Yuan, Olalekan Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-161, https://doi.org/10.5194/acp-2022-161, 2022
Revised manuscript accepted for ACP
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Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing emissions inventories using air quality models and routine in situ observations. Using this approach, we derived estimates of NOX emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949, https://doi.org/10.5194/acp-22-929-2022, https://doi.org/10.5194/acp-22-929-2022, 2022
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Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-864, https://doi.org/10.5194/acp-2021-864, 2021
Revised manuscript accepted for ACP
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This study investigates to which extent ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts, while highlighting at the same time the complexity of improving the detection of highest O3 concentrations.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys., 21, 16093–16120, https://doi.org/10.5194/acp-21-16093-2021, https://doi.org/10.5194/acp-21-16093-2021, 2021
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Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661, https://doi.org/10.5194/acp-21-15647-2021, https://doi.org/10.5194/acp-21-15647-2021, 2021
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Christopher D. Holmes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-752, https://doi.org/10.5194/acp-2021-752, 2021
Revised manuscript accepted for ACP
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
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Short summary
For this study, we evaluated the WRF–CMAQ coupled model's ability to simulate the long-term trends of wet deposition of nitrogen and sulfur from 1990 to 2010 by comparing the model results with long-term observation datasets in the US. The model generally underestimates the wet deposition of both nitrogen and sulfur but captured well the decreasing trends for the deposition. Then we estimated the deposition budget in the US, including wet deposition and dry deposition from model simulations.
For this study, we evaluated the WRF–CMAQ coupled model's ability to simulate the long-term...
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