Articles | Volume 15, issue 17
https://doi.org/10.5194/acp-15-9997-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue:
https://doi.org/10.5194/acp-15-9997-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Can a coupled meteorology–chemistry model reproduce the historical trend in aerosol direct radiative effects over the Northern Hemisphere?
J. Xing
CORRESPONDING AUTHOR
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
R. Mathur
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
J. Pleim
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
C. Hogrefe
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
C.-M. Gan
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
D. C. Wong
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
The US Environmental Protection Agency, Research Triangle Park, Durham, NC 27711, USA
Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
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Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-368, https://doi.org/10.5194/acp-2022-368, 2022
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Future warming meteorological conditions may enhance the influence of regional transport on PM2.5 pollution. Our results prove that climate-friendly policy could lead to considerable co-benefits in mitigating the regional transport of PM2.5 in future. Meanwhile, climate change will exert larger impacts on across-regional (long-distance) transport than inner (neighboring provinces) regional transport, highlighting the significance of multi-regional cooperation in the future.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys., 21, 16051–16065, https://doi.org/10.5194/acp-21-16051-2021, https://doi.org/10.5194/acp-21-16051-2021, 2021
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In this study, we use a global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys., 21, 15809–15826, https://doi.org/10.5194/acp-21-15809-2021, https://doi.org/10.5194/acp-21-15809-2021, 2021
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
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.
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.
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.
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.
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.
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.
Yuqiang Zhang, Rohit Mathur, Jesse O. Bash, Christian Hogrefe, Jia Xing, and Shawn J. Roselle
Atmos. Chem. Phys., 18, 9091–9106, https://doi.org/10.5194/acp-18-9091-2018, https://doi.org/10.5194/acp-18-9091-2018, 2018
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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.
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.
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.
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.
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.
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.
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.
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
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
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
Geosci. Model Dev., 17, 8373–8397, https://doi.org/10.5194/gmd-17-8373-2024, https://doi.org/10.5194/gmd-17-8373-2024, 2024
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Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources and individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
David C. Wong, Jeff Willison, Jonathan E. Pleim, Golam Sarwar, James Beidler, Russ Bullock, Jerold A. Herwehe, Rob Gilliam, Daiwen Kang, Christian Hogrefe, George Pouliot, and Hosein Foroutan
Geosci. Model Dev., 17, 7855–7866, https://doi.org/10.5194/gmd-17-7855-2024, https://doi.org/10.5194/gmd-17-7855-2024, 2024
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This work describe how we linked the meteorological Model for Prediction Across Scales – Atmosphere (MPAS-A) with the Community Multiscale Air Quality (CMAQ) air quality model to form a coupled modelling system. This could be used to study air quality or climate and air quality interaction at a global scale. This new model scales well in high-performance computing environments and performs well with respect to ground surface networks in terms of ozone and PM2.5.
Anam M. Khan, Olivia E. Clifton, Jesse O. Bash, Sam Bland, Nathan Booth, Philip Cheung, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christian Hogrefe, Christopher D. Holmes, Laszlo Horvath, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Perez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Donna Schwede, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamas Weidinger, Zhiyong Wu, Leiming Zhang, and Paul C. Stoy
EGUsphere, https://doi.org/10.5194/egusphere-2024-3038, https://doi.org/10.5194/egusphere-2024-3038, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Vegetation removes tropospheric ozone through stomatal uptake, and accurately modeling the stomatal uptake of ozone is important for modeling dry deposition and air quality. We evaluated the stomatal component of ozone dry deposition modeled by atmospheric chemistry models at six sites. We find that models and observation-based estimates agree at times during the growing season at all sites, but some models overestimated the stomatal component during the dry summers at a seasonally dry site.
Christos I. Efstathiou, Elizabeth Adams, Carlie J. Coats, Robert Zelt, Mark Reed, John McGee, Kristen M. Foley, Fahim I. Sidi, David C. Wong, Steven Fine, and Saravanan Arunachalam
Geosci. Model Dev., 17, 7001–7027, https://doi.org/10.5194/gmd-17-7001-2024, https://doi.org/10.5194/gmd-17-7001-2024, 2024
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We present a summary of enabling high-performance computing of the Community Multiscale Air Quality Model (CMAQ) – a state-of-the-science community multiscale air quality model – on two cloud computing platforms through documenting the technologies, model performance, scaling and relative merits. This may be a new paradigm for computationally intense future model applications. We initiated this work due to a need to leverage cloud computing advances and to ease the learning curve for new users.
Yuzhi Jin, Jiandong Wang, David C. Wong, Chao Liu, Golam Sarwar, Kathleen M. Fahey, Shang Wu, Jiaping Wang, Jing Cai, Zeyuan Tian, Zhouyang Zhang, Jia Xing, Aijun Ding, and Shuxiao Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2372, https://doi.org/10.5194/egusphere-2024-2372, 2024
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Black carbon (BC) affects climate and the environment, and its aging process alters its properties. Current models, like WRF-CMAQ, lack full account. We developed the WRF-CMAQ-BCG model to better represent BC aging by introducing Bare/Coated BC species and their conversion. Our findings show that BC mixing states have distinct spatiotemporal distribution characteristics, and BC wet deposition is dominated by Coated BC. Accounting for BC aging process improves aerosol optics simulation accuracy.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz-Ozdemir, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Iannis Koutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark Shephard, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2024-2226, https://doi.org/10.5194/egusphere-2024-2226, 2024
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The large range of sulphur and nitrogen deposition estimates from air-quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulphur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by droplets, rain, snow, etc., aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, and gas deposition via plant cuticles and soil.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Michael S. Walters and David C. Wong
Geosci. Model Dev., 16, 1179–1190, https://doi.org/10.5194/gmd-16-1179-2023, https://doi.org/10.5194/gmd-16-1179-2023, 2023
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A typical numerical simulation that associates with a large amount of input and output data, applying popular compression software, gzip or bzip2, on data is one good way to mitigate data storage burden. This article proposes a simple technique to alter input, output, or input and output by keeping a specific number of significant digits in data and demonstrates an enhancement in compression efficiency on the altered data but maintains similar statistical performance of the numerical simulation.
Daiwen Kang, Nicholas K. Heath, Robert C. Gilliam, Tanya L. Spero, and Jonathan E. Pleim
Geosci. Model Dev., 15, 8561–8579, https://doi.org/10.5194/gmd-15-8561-2022, https://doi.org/10.5194/gmd-15-8561-2022, 2022
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A lightning assimilation (LTA) technique implemented in the WRF model's Kain–Fritsch (KF) convective scheme is updated and applied to simulations from regional to hemispheric scales using observed lightning flashes from ground-based lightning detection networks. Different user-toggled options associated with the KF scheme on simulations with and without LTA are assessed. The model's performance is improved significantly by LTA, but it is sensitive to various factors.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Shansi Wang, Siwei Li, Jia Xing, Yu Ding, Senlin Hu, Shuchang Liu, Yu Qin, Zhaoxin Dong, Jiaxin Dong, Ge Song, and Lechao Dong
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-368, https://doi.org/10.5194/acp-2022-368, 2022
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Future warming meteorological conditions may enhance the influence of regional transport on PM2.5 pollution. Our results prove that climate-friendly policy could lead to considerable co-benefits in mitigating the regional transport of PM2.5 in future. Meanwhile, climate change will exert larger impacts on across-regional (long-distance) transport than inner (neighboring provinces) regional transport, highlighting the significance of multi-regional cooperation in the future.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
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.
Kai Wang, Yang Zhang, Shaocai Yu, David C. Wong, Jonathan Pleim, Rohit Mathur, James T. Kelly, and Michelle Bell
Geosci. Model Dev., 14, 7189–7221, https://doi.org/10.5194/gmd-14-7189-2021, https://doi.org/10.5194/gmd-14-7189-2021, 2021
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The two-way coupled WRF-CMAQ model accounting for complex chemistry–meteorology feedbacks has been applied to the long-term predictions of regional meteorology and air quality over the US. The model results show superior performance and importance of chemistry–meteorology feedbacks when compared to the offline coupled WRF and CMAQ simulations, which suggests that feedbacks should be considered along with other factors in developing future model applications to inform policy making.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys., 21, 16051–16065, https://doi.org/10.5194/acp-21-16051-2021, https://doi.org/10.5194/acp-21-16051-2021, 2021
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In this study, we use a global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys., 21, 15809–15826, https://doi.org/10.5194/acp-21-15809-2021, https://doi.org/10.5194/acp-21-15809-2021, 2021
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
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
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
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.
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
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
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).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
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.
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.
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.
Yuqiang Zhang, Rohit Mathur, Jesse O. Bash, Christian Hogrefe, Jia Xing, and Shawn J. Roselle
Atmos. Chem. Phys., 18, 9091–9106, https://doi.org/10.5194/acp-18-9091-2018, https://doi.org/10.5194/acp-18-9091-2018, 2018
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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.
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.
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.
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.
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.
D. C. Wong, C. E. Yang, J. S. Fu, K. Wong, and Y. Gao
Geosci. Model Dev., 8, 1033–1046, https://doi.org/10.5194/gmd-8-1033-2015, https://doi.org/10.5194/gmd-8-1033-2015, 2015
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
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
The surface tension and CCN activation of sea spray aerosol particles
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain: Insights from six-year simulations
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Exploring the processes controlling secondary inorganic aerosol: Evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Land use change influence on atmospheric organic gases, aerosols, and radiative effects
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2838, https://doi.org/10.5194/egusphere-2024-2838, 2024
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We model the CCN activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updrafts.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2704, https://doi.org/10.5194/egusphere-2024-2704, 2024
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This study use the WRF-Chem model to assess how meteorological conditions and unexpected emission reductions affected PM2.5 in the North China Plain (NCP). It highlights regional disparities: in the Northern NCP, adverse weather negated emission reduction effects. In contrast, the Southern NCP with PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology and air quality.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Olivia G. Norman, Colette L. Heald, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2024-2014, https://doi.org/10.5194/egusphere-2024-2014, 2024
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry-climate/vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation, and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1579, https://doi.org/10.5194/egusphere-2024-1579, 2024
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol-radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are -0.11 and +0.17 W/m², respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
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Short summary
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.
The ability of a coupled meteorology-chemistry model (WRF-CMAQ) to reproduce the historical...
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