Articles | Volume 18, issue 8
https://doi.org/10.5194/acp-18-6039-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-6039-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
02 May 2018
Research article |
| 02 May 2018
| 02 May 2018
The importance of vertical resolution in the free troposphere for modeling intercontinental plumes
Jiawei Zhuang
CORRESPONDING AUTHOR
School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA 02138, USA
Daniel J. Jacob
School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA 02138, USA
Sebastian D. Eastham
Laboratory for Aviation and the Environment, Department of Aeronautics
and Astronautics, Massachusetts Institute of Technology, Cambridge, MA
02139, USA
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Jack H. Bruno, Dylan Jervis, Daniel J. Varon, and Daniel J. Jacob
Atmos. Meas. Tech., 17, 2625–2636, https://doi.org/10.5194/amt-17-2625-2024, https://doi.org/10.5194/amt-17-2625-2024, 2024
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Methane is a potent greenhouse gas and a current high-priority target for short- to mid-term climate change mitigation. Detection of individual methane emitters from space has become possible in recent years, and the volume of data for this task has been rapidly growing, outpacing processing capabilities. We introduce an automated approach, U-Plume, which can detect and quantify emissions from individual methane sources in high-spatial-resolution satellite data.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
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Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Drew C. Pendergrass, Daniel J. Jacob, Hannah Nesser, Daniel J. Varon, Melissa Sulprizio, Kazuyuki Miyazaki, and Kevin W. Bowman
Geosci. Model Dev., 16, 4793–4810, https://doi.org/10.5194/gmd-16-4793-2023, https://doi.org/10.5194/gmd-16-4793-2023, 2023
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We have built a tool called CHEEREIO that allows scientists to use observations of pollutants or gases in the atmosphere, such as from satellites or surface stations, to update supercomputer models that simulate the Earth. CHEEREIO uses the difference between the model simulations of the atmosphere and real-world observations to come up with a good guess for the actual composition of our atmosphere, the true emissions of various pollutants, and whatever else they may want to study.
Nicholas Balasus, Daniel J. Jacob, Alba Lorente, Joannes D. Maasakkers, Robert J. Parker, Hartmut Boesch, Zichong Chen, Makoto M. Kelp, Hannah Nesser, and Daniel J. Varon
Atmos. Meas. Tech., 16, 3787–3807, https://doi.org/10.5194/amt-16-3787-2023, https://doi.org/10.5194/amt-16-3787-2023, 2023
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Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
Geosci. Model Dev., 15, 8669–8704, https://doi.org/10.5194/gmd-15-8669-2022, https://doi.org/10.5194/gmd-15-8669-2022, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM's CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular Earth system model and allows two strong but currently separate research communities to benefit from each other's advances.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
William Atkinson, Sebastian D. Eastham, Y.-H. Henry Chen, Jennifer Morris, Sergey Paltsev, C. Adam Schlosser, and Noelle E. Selin
Geosci. Model Dev., 15, 7767–7789, https://doi.org/10.5194/gmd-15-7767-2022, https://doi.org/10.5194/gmd-15-7767-2022, 2022
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Understanding policy effects on human-caused air pollutant emissions is key for assessing related health impacts. We develop a flexible scenario tool that combines updated emissions data sets, long-term economic modeling, and comprehensive technology pathways to clarify the impacts of climate and air quality policies. Results show the importance of both policy levers in the future to prevent long-term emission increases from offsetting near-term air quality improvements from existing policies.
Lu Shen, Ritesh Gautam, Mark Omara, Daniel Zavala-Araiza, Joannes D. Maasakkers, Tia R. Scarpelli, Alba Lorente, David Lyon, Jianxiong Sheng, Daniel J. Varon, Hannah Nesser, Zhen Qu, Xiao Lu, Melissa P. Sulprizio, Steven P. Hamburg, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 11203–11215, https://doi.org/10.5194/acp-22-11203-2022, https://doi.org/10.5194/acp-22-11203-2022, 2022
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We use 22 months of TROPOMI satellite observations to quantity methane emissions from the oil (O) and natural gas (G) sector in the US and Canada at the scale of both individual basins as well as country-wide aggregates. We find that O/G-related methane emissions are underestimated in these inventories by 80 % for the US and 40 % for Canada, and 70 % of the underestimate in the US is from five O/G basins, including Permian, Haynesville, Anadarko, Eagle Ford, and Barnett.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Daniel J. Jacob, Daniel J. Varon, Daniel H. Cusworth, Philip E. Dennison, Christian Frankenberg, Ritesh Gautam, Luis Guanter, John Kelley, Jason McKeever, Lesley E. Ott, Benjamin Poulter, Zhen Qu, Andrew K. Thorpe, John R. Worden, and Riley M. Duren
Atmos. Chem. Phys., 22, 9617–9646, https://doi.org/10.5194/acp-22-9617-2022, https://doi.org/10.5194/acp-22-9617-2022, 2022
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We review the capability of satellite observations of atmospheric methane to quantify methane emissions on all scales. We cover retrieval methods, precision requirements, inverse methods for inferring emissions, source detection thresholds, and observations of system completeness. We show that current instruments already enable quantification of regional and national emissions including contributions from large point sources. Coverage and resolution will increase significantly in coming years.
Daniel J. Varon, Daniel J. Jacob, Melissa Sulprizio, Lucas A. Estrada, William B. Downs, Lu Shen, Sarah E. Hancock, Hannah Nesser, Zhen Qu, Elise Penn, Zichong Chen, Xiao Lu, Alba Lorente, Ashutosh Tewari, and Cynthia A. Randles
Geosci. Model Dev., 15, 5787–5805, https://doi.org/10.5194/gmd-15-5787-2022, https://doi.org/10.5194/gmd-15-5787-2022, 2022
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Reducing atmospheric methane emissions is critical to slow near-term climate change. Globally surveying satellite instruments like the TROPOspheric Monitoring Instrument (TROPOMI) have unique capabilities for monitoring atmospheric methane around the world. Here we present a user-friendly cloud-computing tool that enables researchers and stakeholders to quantify methane emissions across user-selected regions of interest using TROPOMI satellite observations.
John R. Worden, Daniel H. Cusworth, Zhen Qu, Yi Yin, Yuzhong Zhang, A. Anthony Bloom, Shuang Ma, Brendan K. Byrne, Tia Scarpelli, Joannes D. Maasakkers, David Crisp, Riley Duren, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 6811–6841, https://doi.org/10.5194/acp-22-6811-2022, https://doi.org/10.5194/acp-22-6811-2022, 2022
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This paper is intended to accomplish two goals: 1) describe a new algorithm by which remotely sensed measurements of methane or other tracers can be used to not just quantify methane fluxes, but also attribute these fluxes to specific sources and regions and characterize their uncertainties, and 2) use this new algorithm to provide methane emissions by sector and country in support of the global stock take.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Drew C. Pendergrass, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, Soontae Kim, Hong Liao, and Daniel J. Jacob
Atmos. Meas. Tech., 15, 1075–1091, https://doi.org/10.5194/amt-15-1075-2022, https://doi.org/10.5194/amt-15-1075-2022, 2022
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This paper uses a machine learning algorithm to infer high-resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula, using data from a geostationary satellite along with meteorology. We then perform an extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Sabour Baray, Daniel J. Jacob, Joannes D. Maasakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys., 21, 18101–18121, https://doi.org/10.5194/acp-21-18101-2021, https://doi.org/10.5194/acp-21-18101-2021, 2021
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada and lower natural emissions from Boreal wetlands.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
David R. Lyon, Benjamin Hmiel, Ritesh Gautam, Mark Omara, Katherine A. Roberts, Zachary R. Barkley, Kenneth J. Davis, Natasha L. Miles, Vanessa C. Monteiro, Scott J. Richardson, Stephen Conley, Mackenzie L. Smith, Daniel J. Jacob, Lu Shen, Daniel J. Varon, Aijun Deng, Xander Rudelis, Nikhil Sharma, Kyle T. Story, Adam R. Brandt, Mary Kang, Eric A. Kort, Anthony J. Marchese, and Steven P. Hamburg
Atmos. Chem. Phys., 21, 6605–6626, https://doi.org/10.5194/acp-21-6605-2021, https://doi.org/10.5194/acp-21-6605-2021, 2021
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The Permian Basin (USA) is the world’s largest oil field. We use tower- and aircraft-based approaches to measure how methane emissions in the Permian Basin changed throughout 2020. In early 2020, 3.3 % of the region’s gas was emitted; then in spring 2020, the loss rate temporarily dropped to 1.9 % as oil price crashed. We find this short-term reduction to be a result of reduced well development, less gas flaring, and fewer abnormal events despite minimal reductions in oil and gas production.
Daniel J. Varon, Dylan Jervis, Jason McKeever, Ian Spence, David Gains, and Daniel J. Jacob
Atmos. Meas. Tech., 14, 2771–2785, https://doi.org/10.5194/amt-14-2771-2021, https://doi.org/10.5194/amt-14-2771-2021, 2021
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Satellites can detect methane emissions by measuring sunlight reflected from the Earth's surface and atmosphere. Here we show that the European Space Agency's Sentinel-2 twin satellites can be used to monitor anomalously large methane point sources around the world, with global coverage every 2–5 days and 20 m spatial resolution. We demonstrate this previously unreported capability through high-frequency Sentinel-2 monitoring of two strong methane point sources in Algeria and Turkmenistan.
Xiao Lu, Daniel J. Jacob, Yuzhong Zhang, Joannes D. Maasakkers, Melissa P. Sulprizio, Lu Shen, Zhen Qu, Tia R. Scarpelli, Hannah Nesser, Robert M. Yantosca, Jianxiong Sheng, Arlyn Andrews, Robert J. Parker, Hartmut Boesch, A. Anthony Bloom, and Shuang Ma
Atmos. Chem. Phys., 21, 4637–4657, https://doi.org/10.5194/acp-21-4637-2021, https://doi.org/10.5194/acp-21-4637-2021, 2021
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We use an analytical solution to the Bayesian inverse problem to quantitatively compare and combine the information from satellite and in situ observations, and to estimate global methane budget and their trends over the 2010–2017 period. We find that satellite and in situ observations are to a large extent complementary in the inversion for estimating global methane budget, and reveal consistent corrections of regional anthropogenic and wetland methane emissions relative to the prior inventory.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jianxiong Sheng, Yuzhong Zhang, Xiao Lu, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, and Robert J. Parker
Atmos. Chem. Phys., 21, 4339–4356, https://doi.org/10.5194/acp-21-4339-2021, https://doi.org/10.5194/acp-21-4339-2021, 2021
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We use 2010–2015 GOSAT satellite observations of atmospheric methane over North America in a high-resolution inversion to estimate methane emissions. We find general consistency with the gridded EPA inventory but higher oil and gas production emissions, with oil production emissions twice as large as in the latest EPA Greenhouse Gas Inventory. We find lower wetland emissions than predicted by WetCHARTs and a small increasing trend in the eastern US, apparently related to unconventional oil/gas.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Inés Sanz-Morère, Sebastian D. Eastham, Florian Allroggen, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 21, 1649–1681, https://doi.org/10.5194/acp-21-1649-2021, https://doi.org/10.5194/acp-21-1649-2021, 2021
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Contrails cause ~50 % of aviation climate impacts, but this is highly uncertain. This is partly due to the effect of overlap between contrails and other cloud layers. We developed a model to quantify this effect, finding that overlap with natural clouds increased contrails' radiative forcing in 2015. This suggests that cloud avoidance may help in reducing aviation's climate impacts. We also find that contrail–contrail overlap reduces impacts by ~3 %, increasing non-linearly with optical depth.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Tia R. Scarpelli, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Kelly Rose, Lucy Romeo, John R. Worden, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 12, 563–575, https://doi.org/10.5194/essd-12-563-2020, https://doi.org/10.5194/essd-12-563-2020, 2020
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Methane, a potent greenhouse gas, is emitted through the exploitation of oil, gas, and coal resources, and many efforts to reduce emissions have targeted these sources. We have created a global inventory of oil, gas, and coal methane emissions based on country reporting to the United Nations. The inventory can be used along with satellite observations of methane to better understand the contribution of these sources to global emissions and to identify potential biases in emissions reporting.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Daniel H. Cusworth, Daniel J. Jacob, Daniel J. Varon, Christopher Chan Miller, Xiong Liu, Kelly Chance, Andrew K. Thorpe, Riley M. Duren, Charles E. Miller, David R. Thompson, Christian Frankenberg, Luis Guanter, and Cynthia A. Randles
Atmos. Meas. Tech., 12, 5655–5668, https://doi.org/10.5194/amt-12-5655-2019, https://doi.org/10.5194/amt-12-5655-2019, 2019
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We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers scheduled for launch in 2019–2025. We perform methane retrievals on simulated scenes with varying surfaces and atmospheric methane concentrations. Our results suggest that imaging spectrometers in space could play a transformative role in the future for quantifying methane emissions from point sources on a global scale.
Shixian Zhai, Daniel J. Jacob, Xuan Wang, Lu Shen, Ke Li, Yuzhong Zhang, Ke Gui, Tianliang Zhao, and Hong Liao
Atmos. Chem. Phys., 19, 11031–11041, https://doi.org/10.5194/acp-19-11031-2019, https://doi.org/10.5194/acp-19-11031-2019, 2019
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Observed annual mean PM2.5 decreased by 30–50 % in China from 2013–2018. However, meteorologically PM2.5 variability complicates trend attribution. We used a stepwise multiple linear regression model to quantitatively separate contributions from anthropogenic emissions and meteorology. Results show that 88 % of the PM2.5 decrease across China is attributable to anthropogenic emission changes, and 12 % is attributable to meteorology.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Kelvin H. Bates and Daniel J. Jacob
Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, https://doi.org/10.5194/acp-19-9613-2019, 2019
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Isoprene is a highly reactive chemical released to the atmosphere by plants. Its gas-phase reactions and interactions with chemicals released by human activity have far-reaching atmospheric consequences, contributing to ozone and particulate pollution and prolonging the lifetime of methane, a potent greenhouse gas. We use global simulations with a new isoprene reaction scheme to quantify those effects and to show how recently discovered aspects of isoprene chemistry play out on a global scale.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
Atmos. Chem. Phys., 19, 7859–7881, https://doi.org/10.5194/acp-19-7859-2019, https://doi.org/10.5194/acp-19-7859-2019, 2019
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We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Jian-Xiong Sheng, Daniel J. Jacob, Joannes D. Maasakkers, Yuzhong Zhang, and Melissa P. Sulprizio
Atmos. Meas. Tech., 11, 6379–6388, https://doi.org/10.5194/amt-11-6379-2018, https://doi.org/10.5194/amt-11-6379-2018, 2018
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We conduct Observing System Simulation Experiments to compare the ability of future satellite measurements of atmospheric methane columns for constraining methane emissions at the 25 km scale. We find that the geostationary instruments can do much better than TROPOMI and are less sensitive to cloud cover. GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission considered by NASA in response to the Decadal Survey of the US National Research Council.
Daniel H. Cusworth, Daniel J. Jacob, Jian-Xiong Sheng, Joshua Benmergui, Alexander J. Turner, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 16885–16896, https://doi.org/10.5194/acp-18-16885-2018, https://doi.org/10.5194/acp-18-16885-2018, 2018
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Methane emissions from oil/gas fields originate from a large number of small and densely clustered point sources. We examine the potential of recently launched or planned satellites to locate these high-mode emitters through measurements of atmospheric methane. We find that the recently launched TROPOMI and the planned GeoCARB instruments are successful at locating high-emitting sources for fields of 20-50 emitters within the 50 × 50 km2 geographic domain but are unsuccessful for denser fields.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Yuzhong Zhang, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Ritesh Gautam, and John Worden
Atmos. Chem. Phys., 18, 15959–15973, https://doi.org/10.5194/acp-18-15959-2018, https://doi.org/10.5194/acp-18-15959-2018, 2018
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We assess the potential of using satellite observations of atmospheric methane to monitor global mean tropospheric OH concentration, a key parameter for the oxidizing power of the atmosphere.
Daniel J. Varon, Daniel J. Jacob, Jason McKeever, Dylan Jervis, Berke O. A. Durak, Yan Xia, and Yi Huang
Atmos. Meas. Tech., 11, 5673–5686, https://doi.org/10.5194/amt-11-5673-2018, https://doi.org/10.5194/amt-11-5673-2018, 2018
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Methane is a powerful greenhouse gas emitted from numerous human activities. Space-based observation of point sources would be a cost-effective monitoring solution, but the resolution of most current and planned methane-observing satellites is too coarse to resolve individual emitters. We simulate fine-resolution (50 m) satellite observations of methane plumes as would be measured by GHGSat (to be launched in 2019) and show that such data can usefully quantify large methane point sources.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Joshua Benmergui, A. Anthony Bloom, Claudia Arndt, Ritesh Gautam, Daniel Zavala-Araiza, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 18, 12257–12267, https://doi.org/10.5194/acp-18-12257-2018, https://doi.org/10.5194/acp-18-12257-2018, 2018
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Analysis of 7 years (2010–2016) of GOSAT methane trends over Canada, the contiguous US, and Mexico suggests that US methane emissions increased by 2.5 ± 1.4 % a−1 over the 7-year period, with contributions from both oil–gas systems and livestock in the Midwest. Mexican emissions show a decrease that can be attributed to a decreasing cattle population. Canadian emissions show year-to-year variability driven by wetland emissions and correlated with wetland areal extent.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Alexander J. Turner, Daniel J. Jacob, Joshua Benmergui, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 8265–8278, https://doi.org/10.5194/acp-18-8265-2018, https://doi.org/10.5194/acp-18-8265-2018, 2018
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We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 km spatial resolution and hourly temporal resolution over the Barnett Shale. We find that a week of TROPOMI observations should provide regional (~30 km) information on temporally invariant sources and GeoCARB should provide information on temporally invariant sources at 2–7 km spatial resolution. An instrument precision better than 6 ppb is an important threshold for achieving fine resolution of emissions.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Melissa P. Sulprizio, A. Anthony Bloom, Arlyn E. Andrews, and Debra Wunch
Atmos. Chem. Phys., 18, 6483–6491, https://doi.org/10.5194/acp-18-6483-2018, https://doi.org/10.5194/acp-18-6483-2018, 2018
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We use observations of boundary layer methane from the SEAC4RS aircraft campaign over the Southeast US to estimate methane emissions in that region. Our results suggest that the EPA inventory is regionally unbiased but there are large local biases, suggesting variable emission factors. Our results also suggest that the choice of landcover map is the dominant source of error for wetland emission estimates.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
A. Anthony Bloom, Kevin W. Bowman, Meemong Lee, Alexander J. Turner, Ronny Schroeder, John R. Worden, Richard Weidner, Kyle C. McDonald, and Daniel J. Jacob
Geosci. Model Dev., 10, 2141–2156, https://doi.org/10.5194/gmd-10-2141-2017, https://doi.org/10.5194/gmd-10-2141-2017, 2017
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Wetland emissions are a principal source of uncertainty in the global atmospheric methane budget due to poor knowledge of wetland processes. We construct a wetland methane emission and uncertainty dataset for use in global atmospheric methane models. Our wetland model ensemble is based on static wetland maps, satellite-derived inundation and carbon cycle models. The ensemble performs favourably against regional flux estimates and atmospheric methane measurements relative to previous studies.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Sebastian D. Eastham and Daniel J. Jacob
Atmos. Chem. Phys., 17, 2543–2553, https://doi.org/10.5194/acp-17-2543-2017, https://doi.org/10.5194/acp-17-2543-2017, 2017
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Intercontinental atmospheric transport can disrupt local chemistry and cause air quality issues thousands of kilometers from the source, complicating correct attribution of air quality exceedances. This transport occurs in long, thin plumes which current-generation models consistently fail to reproduce. Our study investigates the cause of this failure, finding that greater vertical resolution than is currently available is required to reliably resolve the plumes and their effects.
Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Jianxiong Sheng, Kang Sun, Xiong Liu, Kelly Chance, Ilse Aben, Jason McKeever, and Christian Frankenberg
Atmos. Chem. Phys., 16, 14371–14396, https://doi.org/10.5194/acp-16-14371-2016, https://doi.org/10.5194/acp-16-14371-2016, 2016
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Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned to launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify methane emissions from the global scale down to the scale of point sources.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Christopher Chan Miller, Daniel J. Jacob, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 16, 4631–4639, https://doi.org/10.5194/acp-16-4631-2016, https://doi.org/10.5194/acp-16-4631-2016, 2016
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Volatile organic compounds (VOCs) are important precursors for photochemical smog.
Glyoxal is an organic compound produced in the atmosphere from reactions of larger VOCs. OMI satellite observations of glyoxal show a large hotspot over the Pearl River delta. The hotspot can be explained by industrial paint and solvent emissions of aromatic VOCs. Our work shows OMI observations are consistent with current VOC emissions estimates, whereas previous work has suggested large underestimates.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
A. J. Turner and D. J. Jacob
Atmos. Chem. Phys., 15, 7039–7048, https://doi.org/10.5194/acp-15-7039-2015, https://doi.org/10.5194/acp-15-7039-2015, 2015
A. J. Turner, D. J. Jacob, K. J. Wecht, J. D. Maasakkers, E. Lundgren, A. E. Andrews, S. C. Biraud, H. Boesch, K. W. Bowman, N. M. Deutscher, M. K. Dubey, D. W. T. Griffith, F. Hase, A. Kuze, J. Notholt, H. Ohyama, R. Parker, V. H. Payne, R. Sussmann, C. Sweeney, V. A. Velazco, T. Warneke, P. O. Wennberg, and D. Wunch
Atmos. Chem. Phys., 15, 7049–7069, https://doi.org/10.5194/acp-15-7049-2015, https://doi.org/10.5194/acp-15-7049-2015, 2015
M. S. Long, R. Yantosca, J. E. Nielsen, C. A. Keller, A. da Silva, M. P. Sulprizio, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 8, 595–602, https://doi.org/10.5194/gmd-8-595-2015, https://doi.org/10.5194/gmd-8-595-2015, 2015
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This paper presents results from the modularization of the GEOS-Chem chemical transport model, and its coupling as the chemical operator within the NASA-GMAO GEOS-5 Earth system model (ESM). The key findings are that chemistry within the modular GEOS-Chem system shows consistent, high strong-scaling properties across the range of distributed processors, transport is the limiting component prohibiting efficient scalability, and GEOS-Chem is able to generate suitable chemical results in an ESM.
C. Chan Miller, G. Gonzalez Abad, H. Wang, X. Liu, T. Kurosu, D. J. Jacob, and K. Chance
Atmos. Meas. Tech., 7, 3891–3907, https://doi.org/10.5194/amt-7-3891-2014, https://doi.org/10.5194/amt-7-3891-2014, 2014
K. J. Wecht, D. J. Jacob, M. P. Sulprizio, G. W. Santoni, S. C. Wofsy, R. Parker, H. Bösch, and J. Worden
Atmos. Chem. Phys., 14, 8173–8184, https://doi.org/10.5194/acp-14-8173-2014, https://doi.org/10.5194/acp-14-8173-2014, 2014
C. A. Keller, M. S. Long, R. M. Yantosca, A. M. Da Silva, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 7, 1409–1417, https://doi.org/10.5194/gmd-7-1409-2014, https://doi.org/10.5194/gmd-7-1409-2014, 2014
P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
Atmos. Chem. Phys., 14, 6261–6271, https://doi.org/10.5194/acp-14-6261-2014, https://doi.org/10.5194/acp-14-6261-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
E. V. Fischer, D. J. Jacob, R. M. Yantosca, M. P. Sulprizio, D. B. Millet, J. Mao, F. Paulot, H. B. Singh, A. Roiger, L. Ries, R.W. Talbot, K. Dzepina, and S. Pandey Deolal
Atmos. Chem. Phys., 14, 2679–2698, https://doi.org/10.5194/acp-14-2679-2014, https://doi.org/10.5194/acp-14-2679-2014, 2014
P. S. Kim, D. J. Jacob, X. Liu, J. X. Warner, K. Yang, K. Chance, V. Thouret, and P. Nedelec
Atmos. Chem. Phys., 13, 9321–9335, https://doi.org/10.5194/acp-13-9321-2013, https://doi.org/10.5194/acp-13-9321-2013, 2013
J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
Related subject area
Subject: Dynamics | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Synoptic and microphysical lifetime constraints for contrails
Country- and species-dependent parameters for the heating degree day method to distribute NOx and PM emissions from residential heating in the EU 27: application to air quality modelling and multi-year emission projections
Physical processes influencing the Asian climate due to black carbon emission over East and South Asia
Valley floor inclination affecting valley winds and transport of passive tracers in idealised simulations
To what extent is the description of streets important in estimating local air quality: a case study over Paris
Variability and trends in the potential vorticity (PV)-gradient dynamical tropopause
Kinematic properties of regions that can involve persistent contrails
The spatiotemporal evolution of atmospheric boundary layers over a thermally heterogeneous landscape
The marinada fall wind in the eastern Ebro sub-basin: physical mechanisms and role of the sea, orography and irrigation
The influences of El Niño–Southern Oscillation on tropospheric ozone in CMIP6 models
Technical note: Exploring parameter and meteorological uncertainty via emulation in volcanic ash atmospheric dispersion modelling
Role of the Indian Ocean basin mode in driving the interdecadal variations of summer precipitation over the East Asian monsoon boundary zone
Extreme ozone episodes in a major Mediterranean urban area
Wintertime extreme warming events in the high Arctic: characteristics, drivers, trends, and the role of atmospheric rivers
Influence of lower-tropospheric moisture on local soil moisture–precipitation feedback over the US Southern Great Plains
The Lagrangian Atmospheric Radionuclide Transport Model (ARTM) – sensitivity studies and evaluation using airborne measurements of power plant emissions
Large-eddy-model closure and simulation of turbulent flux patterns over oasis surface
Impact of the Guinea coast upwelling on atmospheric dynamics, precipitation and pollutant transport over southern West Africa
Investigating multiscale meteorological controls and impact of soil moisture heterogeneity on radiation fog in complex terrain using semi-idealised simulations
Effect of the boundary layer low-level jet on fast fog spatial propagation
Mediterranean tropical-like cyclone forecasts and analysis using the ECMWF ensemble forecasting system with physical parameterization perturbations
Using synthetic case studies to explore the spread and calibration of ensemble atmospheric dispersion forecasts
Meteorological modeling sensitivity to parameterizations and satellite-derived surface datasets during the 2017 Lake Michigan Ozone Study
Trajectory enhancement of low-earth orbiter thermodynamic retrievals to predict convection: a simulation experiment
Lagrangian transport simulations using the extreme convection parameterization: an assessment for the ECMWF reanalyses
Better-constrained climate sensitivity when accounting for dataset dependency on pattern effect estimates
Determination of the chemical equator from GEOS-Chem model simulation: a focus on the tropical western Pacific region
Uncertainty in parameterized convection remains a key obstacle for estimating surface fluxes of carbon dioxide
Antarctic atmospheric Richardson number from radiosonde measurements and AMPS
Divergent convective outflow in large-eddy simulations
Modulation of daily PM2.5 concentrations over China in winter by large-scale circulation and climate change
Modeling of street-scale pollutant dispersion by coupled simulation of chemical reaction, aerosol dynamics, and CFD
Daytime along-valley winds in the Himalayas as simulated by the Weather Research and Forecasting (WRF) model
Evolution of squall line variability and error growth in an ensemble of large eddy simulations
Climatology and variability of air mass transport from the boundary layer to the Asian monsoon anticyclone
Evaluation and bias correction of probabilistic volcanic ash forecasts
The representation of the trade winds in ECMWF forecasts and reanalyses during EUREC4A
Modeling approaches for atmospheric ion–dipole collisions: all-atom trajectory simulations and central field methods
Parameterizing the aerodynamic effect of trees in street canyons for the street network model MUNICH using the CFD model Code_Saturne
Quantifying the impact of meteorological uncertainty on emission estimates and the risk to aviation using source inversion for the Raikoke 2019 eruption
Acceleration of the southern African easterly jet driven by the radiative effect of biomass burning aerosols and its impact on transport during AEROCLO-sA
The Sun's role in decadal climate predictability in the North Atlantic
Future projections of daily haze-conducive and clear weather conditions over the North China Plain using a perturbed parameter ensemble
Refining an ensemble of volcanic ash forecasts using satellite retrievals: Raikoke 2019
Ship-based estimates of momentum transfer coefficient over sea ice and recommendations for its parameterization
Revising the definition of anthropogenic heat flux from buildings: role of human activities and building storage heat flux
An assessment of tropopause characteristics of the ERA5 and ERA-Interim meteorological reanalyses
Distinct evolutions of haze pollution from winter to the following spring over the North China Plain: role of the North Atlantic sea surface temperature anomalies
The foehn effect during easterly flow over Svalbard
Effect of rainfall-induced diabatic heating over southern China on the formation of wintertime haze on the North China Plain
Sina Maria Hofer and Klaus Martin Gierens
EGUsphere, https://doi.org/10.5194/egusphere-2025-326, https://doi.org/10.5194/egusphere-2025-326, 2025
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The climate effect of contrails depends on contrail lifetime. Thus, it is important to know what constrains the lifetime. In this paper we characterize the two most important contrail dissolution processes via their respective time-scales. Both time-scales are in the order of a couple of hours, depending on the synoptic situation and the size of the contrail ice crystals. The combined time-scale which combines both processes is the harmonic mean of the two single time-scales.
Antoine Guion, Florian Couvidat, Marc Guevara, and Augustin Colette
Atmos. Chem. Phys., 25, 2807–2827, https://doi.org/10.5194/acp-25-2807-2025, https://doi.org/10.5194/acp-25-2807-2025, 2025
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The residential sector can cause high background levels of pollutants and pollution peaks in winter. Its emissions are dominated by space heating and show strong daily variations linked to changes in outside temperature. Using heating degree days, we provide country- and species-dependent parameters for the distribution of these emissions, improving the performance of the CHIMERE air quality model. This also allows annual residential emissions to be projected before official publications.
Feifei Luo, Bjørn Samset, Camilla Stjern, Manoj Joshi, Laura Wilcox, Robert Allen, Wei Hua, and Shuanglin Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3867, https://doi.org/10.5194/egusphere-2024-3867, 2025
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Black carbon (BC) aerosol is emitted from the incomplete combustion of biomass and fossil fuels. We found that Asian BC lead to a strong local cooling and drying. Reductions in precipitation primarily depend on the thermodynamic effects due to solar radiation absorption by BC. The combined thermodynamic and Dynamic effects shape the spatial pattern of precipitation responses to Asian BC. These results help further understand the impact of emissions of anthropogenic aerosols on Asian climate.
Johannes Mikkola, Alexander Gohm, Victoria A. Sinclair, and Federico Bianchi
Atmos. Chem. Phys., 25, 511–533, https://doi.org/10.5194/acp-25-511-2025, https://doi.org/10.5194/acp-25-511-2025, 2025
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This study investigates the influence of valley floor inclination on diurnal winds and passive tracer transport within idealised mountain valleys using numerical simulations. The valley inclination strengthens the daytime up-valley winds but only up to a certain point. Beyond that critical angle, the winds weaken again. The inclined valleys transport the tracers higher up in the free troposphere, which would, for example, lead to higher potential for long-range transport.
Alexis Squarcioni, Yelva Roustan, Myrto Valari, Youngseob Kim, Karine Sartelet, Lya Lugon, Fabrice Dugay, and Robin Voitot
Atmos. Chem. Phys., 25, 93–117, https://doi.org/10.5194/acp-25-93-2025, https://doi.org/10.5194/acp-25-93-2025, 2025
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This study highlights the interest of using a street-network model to estimate pollutant concentrations of NOx, NO2, and PM2.5 in heterogeneous urban areas, particularly those adjacent to highways, compared with the subgrid-scale approach embedded in the 3D Eulerian model CHIMERE. However, the study also reveals comparable performances between the two approaches for the aforementioned pollutants in areas near the city center, where urban characteristics are more uniform.
Katharina Turhal, Felix Plöger, Jan Clemens, Thomas Birner, Franziska Weyland, Paul Konopka, and Peter Hoor
Atmos. Chem. Phys., 24, 13653–13679, https://doi.org/10.5194/acp-24-13653-2024, https://doi.org/10.5194/acp-24-13653-2024, 2024
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The tropopause separates the troposphere, where many greenhouse gases originate, from the stratosphere. This study examines a tropopause defined by potential vorticity – an analogue for angular momentum that changes sharply in the subtropics, creating a transport barrier. Between 1980 and 2017, this tropopause shifted poleward at lower altitudes and equatorward above, suggesting height-dependent changes in atmospheric circulation that may affect greenhouse gas distribution and global warming.
Sina Maria Hofer and Klaus Martin Gierens
EGUsphere, https://doi.org/10.5194/egusphere-2024-3520, https://doi.org/10.5194/egusphere-2024-3520, 2024
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Ice supersaturation is an immaterial feature, which does not generally move with the wind that carries contrails and cirrus clouds. Here we analyse the different motions and show that ice supersaturated regions (ISSRs) on average move slower than the wind, the direction of movement is usually quite similar and the distributions of both velocities follow Weibull distributions. The almost identical direction of the movements is beneficial for contrail lifetimes.
Mary Rose Mangan, Jordi Vilà-Guerau de Arellano, Bart J. H. van Stratum, Marie Lothon, Guylaine Canut-Rocafort, and Oscar K. Hartogensis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3000, https://doi.org/10.5194/egusphere-2024-3000, 2024
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Using observations and high-resolution turbulence modeling, we examine the influence of irrigation-driven surface heterogeneity on the atmospheric boundary layer (ABL). We employ different spatial scales of heterogeneity to explore how the influence of surface heterogeneity on the ABL within a single grid cell would change in higher resolution global models. We find that the height of the ABL is highly variable, and that the surface heterogeneity is felt least strongly in the middle of the ABL.
Tanguy Lunel, Maria Antonia Jimenez, Joan Cuxart, Daniel Martinez-Villagrasa, Aaron Boone, and Patrick Le Moigne
Atmos. Chem. Phys., 24, 7637–7666, https://doi.org/10.5194/acp-24-7637-2024, https://doi.org/10.5194/acp-24-7637-2024, 2024
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During the summer in Catalonia, a cool wind, the marinada, blows into the eastern Ebro basin in the afternoon. This study investigates its previously unclear dynamics using observations and a meteorological model. It is found to be driven by a cool marine air mass that flows over the mountains into the basin. The study shows how the sea breeze, upslope winds, larger weather patterns and irrigation play a prominent role in the formation and characteristics of the marinada.
Thanh Le, Seon-Ho Kim, Jae-Yeong Heo, and Deg-Hyo Bae
Atmos. Chem. Phys., 24, 6555–6566, https://doi.org/10.5194/acp-24-6555-2024, https://doi.org/10.5194/acp-24-6555-2024, 2024
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We examined the links between the El Niño–Southern Oscillation (ENSO) and tropospheric ozone (O3) using model data. Our results show that ENSO impacts on tropospheric O3 are mainly found over oceans, while the signature of ENSO over continents is largely unclear. These impacts in the midlatitude regions over the Southern Hemisphere may be more significant than previously known. The responses of O3 to ENSO are weak in the middle troposphere and stronger in the upper and lower troposphere.
James M. Salter, Helen N. Webster, and Cameron Saint
Atmos. Chem. Phys., 24, 6251–6274, https://doi.org/10.5194/acp-24-6251-2024, https://doi.org/10.5194/acp-24-6251-2024, 2024
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Models are used to make forecasts of volcanic ash dispersion during eruptions. These models have unknown inputs relating to the eruption itself, physical processes, and meteorological conditions. We use statistical models to predict the output of the expensive physical model and show we can account for the effects of the different inputs. We compare the model to real-world observations and show that accounting for all sources of uncertainty may lead to different conclusions about the inputs.
Jing Wang, Yanju Liu, Fei Cheng, Chengyu Song, Qiaoping Li, Yihui Ding, and Xiangde Xu
Atmos. Chem. Phys., 24, 5099–5115, https://doi.org/10.5194/acp-24-5099-2024, https://doi.org/10.5194/acp-24-5099-2024, 2024
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Based on long-term observational, reanalysis, and numerical model simulation datasets from 1901 through 2014, this study shows that precipitation over the East Asian monsoon boundary zone featured prominent interdecadal changes, with dry summers during the periods preceding 1927, 1939–1945, 1968–1982, and 1998–2010 and wet summers during 1928–1938, 1946–1967, and 2011 onwards. The Indian Ocean basin mode is an important oceanic modulator responsible for its interdecadal variations.
Jordi Massagué, Eduardo Torre-Pascual, Cristina Carnerero, Miguel Escudero, Andrés Alastuey, Marco Pandolfi, Xavier Querol, and Gotzon Gangoiti
Atmos. Chem. Phys., 24, 4827–4850, https://doi.org/10.5194/acp-24-4827-2024, https://doi.org/10.5194/acp-24-4827-2024, 2024
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This study analyses three acute ozone episodes in Barcelona (NE Spain) which have occurred only in recent years and are of particular concern due to the city's significant population. The findings uncover a complex interplay of factors, notably shared among episodes, including pollution transport at different scales and specific weather and emission patterns. These insights significantly enhance our understanding of these occurrences and improve predictive capabilities.
Weiming Ma, Hailong Wang, Gang Chen, Yun Qian, Ian Baxter, Yiling Huo, and Mark W. Seefeldt
Atmos. Chem. Phys., 24, 4451–4472, https://doi.org/10.5194/acp-24-4451-2024, https://doi.org/10.5194/acp-24-4451-2024, 2024
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Extreme warming events with surface temperature going above 0°C can occur in the high-Arctic winter. Although reanalysis data show that these events were short-lived and occurred rarely during 1980–2021, they have become more frequent, stronger, and longer lasting latterly. A dipole pattern, comprising high- and low-pressure systems, is found to be the key in driving them. These findings have implications for the recent changes in sea ice, hydrological cycle, and ecosystem over the Arctic.
Gaoyun Wang, Rong Fu, Yizhou Zhuang, Paul A. Dirmeyer, Joseph A. Santanello, Guiling Wang, Kun Yang, and Kaighin McColl
Atmos. Chem. Phys., 24, 3857–3868, https://doi.org/10.5194/acp-24-3857-2024, https://doi.org/10.5194/acp-24-3857-2024, 2024
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This study investigates the influence of lower-tropospheric humidity on land–atmosphere coupling (LAC) during warm seasons in the US Southern Great Plains. Using radiosonde data and a buoyancy model, we find that elevated LT humidity is crucial for generating afternoon precipitation events under dry soil conditions not accounted for by conventional LAC indices. This underscores the importance of considering LT humidity in understanding LAC over dry soil during droughts in the SGP.
Robert Hanfland, Dominik Brunner, Christiane Voigt, Alina Fiehn, Anke Roiger, and Margit Pattantyús-Ábrahám
Atmos. Chem. Phys., 24, 2511–2534, https://doi.org/10.5194/acp-24-2511-2024, https://doi.org/10.5194/acp-24-2511-2024, 2024
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To show that the three-dimensional dispersion of plumes simulated by the Atmospheric Radionuclide Transport Model within the planetary boundary layer agrees with real plumes, we identify the most important input parameters and analyse the turbulence properties of five different turbulence models in very unstable stratification conditions using their deviation from the well-mixed state. Simulations show that one model agrees slightly better in unstable stratification conditions.
Bangjun Cao, Yaping Shao, Xianyu Yang, Xin Yin, and Shaofeng Liu
Atmos. Chem. Phys., 24, 275–285, https://doi.org/10.5194/acp-24-275-2024, https://doi.org/10.5194/acp-24-275-2024, 2024
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Our novel scheme enhances large-eddy simulations (LESs) for atmosphere–land interactions. It couples LES subgrid closure with Monin–Obukhov similarity theory (MOST), overcoming MOST's limitations. Validated over diverse land surfaces, our approach outperforms existing methods, aligning well with field measurements. Robustness is demonstrated across varying model resolutions. MOST's influence strengthens with decreasing grid spacing, particularly for sensible heat flux.
Gaëlle de Coëtlogon, Adrien Deroubaix, Cyrille Flamant, Laurent Menut, and Marco Gaetani
Atmos. Chem. Phys., 23, 15507–15521, https://doi.org/10.5194/acp-23-15507-2023, https://doi.org/10.5194/acp-23-15507-2023, 2023
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Using a numerical atmospheric model, we found that cooling sea surface temperatures along the southern coast of West Africa in July cause the “little dry season”. This effect reduces humidity and pollutant transport inland, potentially enhancing West Africa's synoptic and seasonal forecasting.
Dongqi Lin, Marwan Katurji, Laura E. Revell, Basit Khan, and Andrew Sturman
Atmos. Chem. Phys., 23, 14451–14479, https://doi.org/10.5194/acp-23-14451-2023, https://doi.org/10.5194/acp-23-14451-2023, 2023
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Accurate fog forecasting is difficult in a complex environment. Spatial variations in soil moisture could impact fog. Here, we carried out fog simulations with spatially different soil moisture in complex topography. The soil moisture was calculated using satellite observations. The results show that the spatial variations in soil moisture do not have a significant impact on where fog occurs but do impact how long fog lasts. This finding could improve fog forecasts in the future.
Shuqi Yan, Hongbin Wang, Xiaohui Liu, Fan Zu, and Duanyang Liu
Atmos. Chem. Phys., 23, 13987–14002, https://doi.org/10.5194/acp-23-13987-2023, https://doi.org/10.5194/acp-23-13987-2023, 2023
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In this study, we quantitatively study the effect of the boundary layer low-level jet (BLLJ) on fast fog spatial propagation; i.e., the fog area expands very fast along a certain direction. The wind speed (10 m s−1) and direction (southeast) of the BLLJ core are consistent with fog propagation (9.6 m s−1). The BLLJ-induced temperature and moisture advections are possible reasons for fast fog propagation. The propagation speed would decrease by 6.4 m s−1 if these advections were turned off.
Miriam Saraceni, Lorenzo Silvestri, Peter Bechtold, and Paolina Bongioannini Cerlini
Atmos. Chem. Phys., 23, 13883–13909, https://doi.org/10.5194/acp-23-13883-2023, https://doi.org/10.5194/acp-23-13883-2023, 2023
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This study focuses on three medicanes, tropical-like cyclones that form in the Mediterranean Sea, studied by ensemble forecasting. This involved multiple simulations of the same event by varying initial conditions and model physics parameters, especially related to convection, which showed comparable results. It is found that medicane development is influenced by the model's ability to predict precursor events and the interaction between upper and lower atmosphere dynamics and thermodynamics.
Andrew R. Jones, Susan J. Leadbetter, and Matthew C. Hort
Atmos. Chem. Phys., 23, 12477–12503, https://doi.org/10.5194/acp-23-12477-2023, https://doi.org/10.5194/acp-23-12477-2023, 2023
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The paper explores spread and calibration properties of ensemble atmospheric dispersion forecasts for hypothetical release events. Real-time forecasts from an ensemble weather prediction system were used to generate an ensemble of dispersion predictions and assessed against simulations produced using analysis meteorology. Results demonstrate good performance overall but highlight more skilful predictions for material released in the upper air compared with releases near the surface.
Jason A. Otkin, Lee M. Cronce, Jonathan L. Case, R. Bradley Pierce, Monica Harkey, Allen Lenzen, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 7935–7954, https://doi.org/10.5194/acp-23-7935-2023, https://doi.org/10.5194/acp-23-7935-2023, 2023
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We performed model simulations to assess the impact of different parameterization schemes, surface initialization datasets, and analysis nudging on lower-tropospheric conditions near Lake Michigan. Simulations were run with high-resolution, real-time datasets depicting lake surface temperatures, green vegetation fraction, and soil moisture. The most accurate results were obtained when using high-resolution sea surface temperature and soil datasets to constrain the model simulations.
Mark T. Richardson, Brian H. Kahn, and Peter Kalmus
Atmos. Chem. Phys., 23, 7699–7717, https://doi.org/10.5194/acp-23-7699-2023, https://doi.org/10.5194/acp-23-7699-2023, 2023
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Convection over land often triggers hours after a satellite last passed overhead and measured the state of the atmosphere, and during those hours the atmosphere can change greatly. Here we show that it is possible to reconstruct most of those changes by using weather forecast winds to predict where warm and moist air parcels will travel. The results can be used to better predict where precipitation is likely to happen in the hours after satellite measurements.
Lars Hoffmann, Paul Konopka, Jan Clemens, and Bärbel Vogel
Atmos. Chem. Phys., 23, 7589–7609, https://doi.org/10.5194/acp-23-7589-2023, https://doi.org/10.5194/acp-23-7589-2023, 2023
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Atmospheric convection plays a key role in tracer transport in the troposphere. Global meteorological forecasts and reanalyses typically have a coarse spatiotemporal resolution that does not adequately resolve the dynamics, transport, and mixing of air associated with storm systems or deep convection. We discuss the application of the extreme convection parameterization in a Lagrangian transport model to improve simulations of tracer transport from the boundary layer into the free troposphere.
Angshuman Modak and Thorsten Mauritsen
Atmos. Chem. Phys., 23, 7535–7549, https://doi.org/10.5194/acp-23-7535-2023, https://doi.org/10.5194/acp-23-7535-2023, 2023
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We provide an improved estimate of equilibrium climate sensitivity (ECS) constrained based on the instrumental temperature record including the corrections for the pattern effect. The improved estimate factors in the uncertainty caused by the underlying sea-surface temperature datasets used in the estimates of pattern effect. This together with the inter-model spread lifts the corresponding IPCC AR6 estimate to 3.2 K [1.8 to 11.0], which is lower and better constrained than in past studies.
Xiaoyu Sun, Mathias Palm, Katrin Müller, Jonas Hachmeister, and Justus Notholt
Atmos. Chem. Phys., 23, 7075–7090, https://doi.org/10.5194/acp-23-7075-2023, https://doi.org/10.5194/acp-23-7075-2023, 2023
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The tropical western Pacific (TWP) is an active interhemispheric transport region contributing significantly to the global climate. A method to determine the chemical equator was developed by model simulations of a virtual passive tracer to analyze transport in the tropics, with a focus on the TWP region. We compare the chemical equator with tropical rain belts and wind fields and obtain a vertical pattern of interhemispheric transport processes which shows tilt structure in certain seasons.
Andrew E. Schuh and Andrew R. Jacobson
Atmos. Chem. Phys., 23, 6285–6297, https://doi.org/10.5194/acp-23-6285-2023, https://doi.org/10.5194/acp-23-6285-2023, 2023
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A comparison of atmospheric carbon dioxide concentrations resulting from two different atmospheric transport models showed large differences in predicted concentrations with significant space–time correlations. The vertical mixing of long-lived trace gases by convection was determined to be the main driver of these differences. The resulting uncertainty was deemed significant to the application of using atmospheric gradients of carbon dioxide to estimate surface fluxes of carbon dioxide.
Qike Yang, Xiaoqing Wu, Xiaodan Hu, Zhiyuan Wang, Chun Qing, Tao Luo, Pengfei Wu, Xianmei Qian, and Yiming Guo
Atmos. Chem. Phys., 23, 6339–6355, https://doi.org/10.5194/acp-23-6339-2023, https://doi.org/10.5194/acp-23-6339-2023, 2023
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The AMPS-forecasted Richardson number was first comprehensively validated over the Antarctic continent. Some potential underlying reasons for the discrepancies between the forecasts and observations were analyzed. The underlying physical processes of triggering atmospheric turbulence in Antarctica were investigated. Our results suggest that the estimated Richardson number by the AMPS is reasonable and the turbulence conditions in Antarctica are well revealed.
Edward Groot and Holger Tost
Atmos. Chem. Phys., 23, 6065–6081, https://doi.org/10.5194/acp-23-6065-2023, https://doi.org/10.5194/acp-23-6065-2023, 2023
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It is shown that the outflow from cumulonimbus clouds or thunderstorms in the upper troposphere and lower stratosphere in idealized high-resolution simulations (LESs) depends linearly on the net amount of latent heat released by the cloud for fixed geometry of the clouds. However, it is shown that, in more realistic situations, convective organization and aggregation (collecting mechanisms of cumulonimbus clouds) affect the amount of outflow non-linearly through non-idealized geometry.
Zixuan Jia, Carlos Ordóñez, Ruth M. Doherty, Oliver Wild, Steven T. Turnock, and Fiona M. O'Connor
Atmos. Chem. Phys., 23, 2829–2842, https://doi.org/10.5194/acp-23-2829-2023, https://doi.org/10.5194/acp-23-2829-2023, 2023
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This study investigates the influence of the winter large-scale circulation on daily concentrations of PM2.5 and their sensitivity to emissions. The new proposed circulation index can effectively distinguish different levels of air pollution and explain changes in PM2.5 sensitivity to emissions from local and surrounding regions. We then project future changes in PM2.5 concentrations using this index and find an increase in PM2.5 concentrations over the region due to climate change.
Chao Lin, Yunyi Wang, Ryozo Ooka, Cédric Flageul, Youngseob Kim, Hideki Kikumoto, Zhizhao Wang, and Karine Sartelet
Atmos. Chem. Phys., 23, 1421–1436, https://doi.org/10.5194/acp-23-1421-2023, https://doi.org/10.5194/acp-23-1421-2023, 2023
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In this study, SSH-aerosol, a modular box model that simulates the evolution of gas, primary, and secondary aerosols, is coupled with the computational fluid dynamics (CFD) software, OpenFOAM and Code_Saturne. The transient dispersion of pollutants emitted from traffic in a street canyon of Greater Paris is simulated. The coupled model achieved better agreement in NO2 and PM10 with measurement data than the conventional CFD simulation which regards pollutants as passive scalars.
Johannes Mikkola, Victoria A. Sinclair, Marja Bister, and Federico Bianchi
Atmos. Chem. Phys., 23, 821–842, https://doi.org/10.5194/acp-23-821-2023, https://doi.org/10.5194/acp-23-821-2023, 2023
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Local winds in four valleys located in the Nepal Himalayas are studied by means of high-resolution meteorological modelling. Well-defined daytime up-valley winds are simulated in all of the valleys with some variation in the flow depth and strength among the valleys and their parts. Parts of the valleys with a steep valley floor inclination (2–5°) are associated with weaker and shallower daytime up-valley winds compared with the parts that have nearly flat valley floors (< 1°).
Edward Groot and Holger Tost
Atmos. Chem. Phys., 23, 565–585, https://doi.org/10.5194/acp-23-565-2023, https://doi.org/10.5194/acp-23-565-2023, 2023
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Thunderstorm systems play an important role in the dynamics of the Earth’s atmosphere, and some of them form a well-organised line: squall lines. Simulations of such squall lines with very small initial perturbations are compared to a reference simulation. The evolution of perturbations and processes amplifying them are analysed. It is shown that the formation of new secondary thunderstorm cells (after the initial primary cells) directly ahead of the line affects the spread strongly.
Matthias Nützel, Sabine Brinkop, Martin Dameris, Hella Garny, Patrick Jöckel, Laura L. Pan, and Mijeong Park
Atmos. Chem. Phys., 22, 15659–15683, https://doi.org/10.5194/acp-22-15659-2022, https://doi.org/10.5194/acp-22-15659-2022, 2022
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During the Asian summer monsoon season, a large high-pressure system is present at levels close to the tropopause above Asia. We analyse how air masses are transported from surface levels to this high-pressure system, which shows distinct features from the surrounding air masses. To this end, we employ multiannual data from two complementary models that allow us to analyse the climatology as well as the interannual and intraseasonal variability of these transport pathways.
Alice Crawford, Tianfeng Chai, Binyu Wang, Allison Ring, Barbara Stunder, Christopher P. Loughner, Michael Pavolonis, and Justin Sieglaff
Atmos. Chem. Phys., 22, 13967–13996, https://doi.org/10.5194/acp-22-13967-2022, https://doi.org/10.5194/acp-22-13967-2022, 2022
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This study describes the development of a workflow which produces probabilistic and quantitative forecasts of volcanic ash in the atmosphere. The workflow includes methods of incorporating satellite observations of the ash cloud into a modeling framework as well as verification statistics that can be used to guide further model development and provide information for risk-based approaches to flight planning.
Alessandro Carlo Maria Savazzi, Louise Nuijens, Irina Sandu, Geet George, and Peter Bechtold
Atmos. Chem. Phys., 22, 13049–13066, https://doi.org/10.5194/acp-22-13049-2022, https://doi.org/10.5194/acp-22-13049-2022, 2022
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Winds are of great importance for the transport of energy and moisture in the atmosphere. In this study we use measurements from the EUREC4A field campaign and several model experiments to understand the wind bias in the forecasts produced by the European Centre for Medium-Range Weather Forecasts. We are able to link the model errors to heights above 2 km and to the representation of the diurnal cycle of winds: the model makes the winds too slow in the morning and too strong in the evening.
Ivo Neefjes, Roope Halonen, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 22, 11155–11172, https://doi.org/10.5194/acp-22-11155-2022, https://doi.org/10.5194/acp-22-11155-2022, 2022
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Collisions between ionic and dipolar molecules and clusters facilitate the formation of atmospheric aerosol particles, which affect global climate and air quality. We compared often-used classical approaches for calculating ion–dipole collision rates with robust atomistic computer simulations. While classical approaches work for simple ions and dipoles only, our modeling approach can also efficiently calculate reasonable collision properties for more complex systems.
Alice Maison, Cédric Flageul, Bertrand Carissimo, Yunyi Wang, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 22, 9369–9388, https://doi.org/10.5194/acp-22-9369-2022, https://doi.org/10.5194/acp-22-9369-2022, 2022
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This paper presents a parameterization of the tree crown effect on air flow and pollutant dispersion in a street network model used to simulate air quality at the street level. The new parameterization is built using a finer-scale model (computational fluid dynamics). The tree effect increases with the leaf area index and the crown volume fraction of the trees; the street horizontal velocity is reduced by up to 68 % and the vertical transfer into or out of the street by up to 23 %.
Natalie J. Harvey, Helen F. Dacre, Cameron Saint, Andrew T. Prata, Helen N. Webster, and Roy G. Grainger
Atmos. Chem. Phys., 22, 8529–8545, https://doi.org/10.5194/acp-22-8529-2022, https://doi.org/10.5194/acp-22-8529-2022, 2022
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In the event of a volcanic eruption, airlines need to make decisions about which routes are safe to operate and ensure that airborne aircraft land safely. The aim of this paper is to demonstrate the application of a statistical technique that best combines ash information from satellites and a suite of computer forecasts of ash concentration to provide a range of plausible estimates of how much volcanic ash emitted from a volcano is available to undergo long-range transport.
Jean-Pierre Chaboureau, Laurent Labbouz, Cyrille Flamant, and Alma Hodzic
Atmos. Chem. Phys., 22, 8639–8658, https://doi.org/10.5194/acp-22-8639-2022, https://doi.org/10.5194/acp-22-8639-2022, 2022
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Ground-based, spaceborne and rare airborne observations of biomass burning aerosols (BBAs) during the AEROCLO-sA field campaign in 2017 are complemented with convection-permitting simulations with online trajectories. The results show that the radiative effect of the BBA accelerates the southern African easterly jet and generates upward motions that transport the BBAs to higher altitudes and farther southwest.
Annika Drews, Wenjuan Huo, Katja Matthes, Kunihiko Kodera, and Tim Kruschke
Atmos. Chem. Phys., 22, 7893–7904, https://doi.org/10.5194/acp-22-7893-2022, https://doi.org/10.5194/acp-22-7893-2022, 2022
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Solar irradiance varies with a period of approximately 11 years. Using a unique large chemistry–climate model dataset, we investigate the solar surface signal in the North Atlantic and European region and find that it changes over time, depending on the strength of the solar cycle. For the first time, we estimate the potential predictability associated with including realistic solar forcing in a model. These results may improve seasonal to decadal predictions of European climate.
Shipra Jain, Ruth M. Doherty, David Sexton, Steven Turnock, Chaofan Li, Zixuan Jia, Zongbo Shi, and Lin Pei
Atmos. Chem. Phys., 22, 7443–7460, https://doi.org/10.5194/acp-22-7443-2022, https://doi.org/10.5194/acp-22-7443-2022, 2022
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We provide a range of future projections of winter haze and clear conditions over the North China Plain (NCP) using multiple simulations from a climate model for the high-emission scenario (RCP8.5). The frequency of haze conducive weather is likely to increase whereas the frequency of clear weather is likely to decrease in future. The total number of hazy days for a given winter can be as much as ˜3.5 times higher than the number of clear days over the NCP.
Antonio Capponi, Natalie J. Harvey, Helen F. Dacre, Keith Beven, Cameron Saint, Cathie Wells, and Mike R. James
Atmos. Chem. Phys., 22, 6115–6134, https://doi.org/10.5194/acp-22-6115-2022, https://doi.org/10.5194/acp-22-6115-2022, 2022
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Forecasts of the dispersal of volcanic ash in the atmosphere are hampered by uncertainties in parameters describing the characteristics of volcanic plumes. Uncertainty quantification is vital for making robust flight-planning decisions. We present a method using satellite data to refine a series of volcanic ash dispersion forecasts and quantify these uncertainties. We show how we can improve forecast accuracy and potentially reduce the regions of high risk of volcanic ash relevant to aviation.
Piyush Srivastava, Ian M. Brooks, John Prytherch, Dominic J. Salisbury, Andrew D. Elvidge, Ian A. Renfrew, and Margaret J. Yelland
Atmos. Chem. Phys., 22, 4763–4778, https://doi.org/10.5194/acp-22-4763-2022, https://doi.org/10.5194/acp-22-4763-2022, 2022
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The parameterization of surface turbulent fluxes over sea ice remains a weak point in weather forecast and climate models. Recent theoretical developments have introduced more extensive physics but these descriptions are poorly constrained due to a lack of observation data. Here we utilize a large dataset of measurements of turbulent fluxes over sea ice to tune the state-of-the-art parameterization of wind stress, and compare it with a previous scheme.
Yiqing Liu, Zhiwen Luo, and Sue Grimmond
Atmos. Chem. Phys., 22, 4721–4735, https://doi.org/10.5194/acp-22-4721-2022, https://doi.org/10.5194/acp-22-4721-2022, 2022
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Anthropogenic heat emission from buildings is important for atmospheric modelling in cities. The current building anthropogenic heat flux is simplified by building energy consumption. Our research proposes a novel approach to determine ‘real’ building anthropogenic heat emission from the changes in energy balance fluxes between occupied and unoccupied buildings. We hope to provide new insights into future parameterisations of building anthropogenic heat flux in urban climate models.
Lars Hoffmann and Reinhold Spang
Atmos. Chem. Phys., 22, 4019–4046, https://doi.org/10.5194/acp-22-4019-2022, https://doi.org/10.5194/acp-22-4019-2022, 2022
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We present an intercomparison of 2009–2018 lapse rate tropopause characteristics as derived from ECMWF's ERA5 and ERA-Interim reanalyses. Large-scale features are similar, but ERA5 shows notably larger variability, which we mainly attribute to UTLS temperature fluctuations due to gravity waves being better resolved by ECMWF's IFS forecast model. Following evaluation with radiosondes and GPS data, we conclude ERA5 will be a more suitable asset for tropopause-related studies in future work.
Linye Song, Shangfeng Chen, Wen Chen, Jianping Guo, Conglan Cheng, and Yong Wang
Atmos. Chem. Phys., 22, 1669–1688, https://doi.org/10.5194/acp-22-1669-2022, https://doi.org/10.5194/acp-22-1669-2022, 2022
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This study shows that in most years when haze pollution (HP) over the North China Plain (NCP) is more (less) serious in winter, air conditions in the following spring are also worse (better) than normal. Conversely, there are some years when HP in the following spring is opposed to that in winter. It is found that North Atlantic sea surface temperature (SST) anomalies play important roles in HP evolution over the NCP. Thus North Atlantic SST is an important preceding signal for NCP HP evolution.
Anna A. Shestakova, Dmitry G. Chechin, Christof Lüpkes, Jörg Hartmann, and Marion Maturilli
Atmos. Chem. Phys., 22, 1529–1548, https://doi.org/10.5194/acp-22-1529-2022, https://doi.org/10.5194/acp-22-1529-2022, 2022
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This article presents a comprehensive analysis of the easterly orographic wind episode which occurred over Svalbard on 30–31 May 2017. This wind caused a significant temperature rise on the lee side of the mountains and greatly intensified the snowmelt. This episode was investigated on the basis of measurements collected during the ACLOUD/PASCAL field campaigns with the help of numerical modeling.
Xiadong An, Lifang Sheng, Chun Li, Wen Chen, Yulian Tang, and Jingliang Huangfu
Atmos. Chem. Phys., 22, 725–738, https://doi.org/10.5194/acp-22-725-2022, https://doi.org/10.5194/acp-22-725-2022, 2022
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The North China Plain (NCP) suffered many periods of haze in winter during 1985–2015, related to the rainfall-induced diabatic heating over southern China. The haze over the NCP is modulated by an anomalous anticyclone caused by the Rossby wave and a north–south circulation (NSC) induced mainly by diabatic heating. As a Rossby wave source, rainfall-induced diabatic heating supports waves and finally strengthens the anticyclone over the NCP. These changes favor haze over the NCP.
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Short summary
Our work explains why current model simulations are unable to capture the intercontinental influences of pollution plumes that are often observed over some regions like California. Due to inadequate vertical grid resolution in these models, the plumes get diffused too rapidly during intercontinental transport. Increasing the vertical grid resolution greatly improves the simulation of plumes and considerably increases the estimate of local surface pollution influence.
Our work explains why current model simulations are unable to capture the intercontinental...
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