Articles | Volume 21, issue 24
Atmos. Chem. Phys., 21, 18351–18374, 2021
https://doi.org/10.5194/acp-21-18351-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 21, 18351–18374, 2021
https://doi.org/10.5194/acp-21-18351-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
17 Dec 2021
Research article
| 17 Dec 2021
Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models
Kelvin H. Bates et al.
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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.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
T. B. Nguyen, M. M. Coggon, K. H. Bates, X. Zhang, R. H. Schwantes, K. A. Schilling, C. L. Loza, R. C. Flagan, P. O. Wennberg, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 3497–3510, https://doi.org/10.5194/acp-14-3497-2014, https://doi.org/10.5194/acp-14-3497-2014, 2014
Yi Cheng, Shaofei Kong, Liquan Yao, Huang Zheng, Jian Wu, Qin Yan, Shurui Zheng, Yao Hu, Zhenzhen Niu, Yingying Yan, Zhenxing Shen, Guofeng Shen, Dantong Liu, Shuxiao Wang, and Shihua Qi
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-154, https://doi.org/10.5194/essd-2022-154, 2022
Preprint under review for ESSD
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We present an emission inventory from 2000 to 2018 with a high spatial-temporal resolution for five missing sources that are related to people’s daily life. The emission factors of carbonaceous aerosol were tested in our laboratory, and activity data were obtained from the combination of multiple proxy data.
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.
Zichong Chen, Daniel Jacob, Hannah Nesser, Melissa Sulprizio, Alba Lorente, Daniel Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-303, https://doi.org/10.5194/acp-2022-303, 2022
Preprint under review for ACP
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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-gas’ energy transition in China. However, this small loss rate can be misleading given China’s high gas imports.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2022-226, https://doi.org/10.5194/egusphere-2022-226, 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 ESM and allows two strong but currently separate research communities to benefit from each other’s advances.
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. Discuss., https://doi.org/10.5194/acp-2022-246, https://doi.org/10.5194/acp-2022-246, 2022
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We review the capability of current and planned satellite observations of atmospheric methane to quantify methane emissions from the global scale down to point sources.
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.
Daniel C. Anderson, Melanie B. Follette-Cook, Sarah A. Strode, Julie M. Nicely, Junhua Liu, Peter D. Ivatt, and Bryan N. Duncan
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-44, https://doi.org/10.5194/gmd-2022-44, 2022
Revised manuscript under review for GMD
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The hydroxyl radical (OH) is the most important chemical in the atmosphere for removing certain pollutants, including methane, the second most important greenhouse gas. We present a methodology to create an easily modifiable parameterization that can calculate OH concentrations in a computationally efficient way. The parameterization, which predicts OH within 5 %, can be integrated into larger climate models to allow for calculation of the interactions between OH, methane, and other chemicals.
Lu Shen, Ritesh Gautam, Mark Omara, Daniel Zavala-Araiza, Joannes Maasakkers, Tia Scarpelli, Alba Lorente, David Lyon, Jianxiong Sheng, Daniel Varon, Hannah Nesser, Zhen Qu, Xiao Lu, Melissa Sulprizio, Steven Hamburg, and Daniel Jacob
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-155, https://doi.org/10.5194/acp-2022-155, 2022
Revised manuscript under review for ACP
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We use 22 months of TROPOMI satellite observations to quantity methane emissions from the oil and natural gas 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 5 O/G basins, including Permian, Haynesville, Anadarko, Eagle Ford and Barnett.
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.
Daniel J. Varon, Daniel J. Jacob, Melissa Sulprizio, Lucas 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. Discuss., https://doi.org/10.5194/gmd-2022-45, https://doi.org/10.5194/gmd-2022-45, 2022
Revised manuscript accepted for GMD
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Reducing atmospheric methane emissions is critical to abating near-term climate change. Global-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 easily map methane emissions across user-selected regions of interest using TROPOMI satellite observations.
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
Short summary
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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.
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. Discuss., https://doi.org/10.5194/gmd-2022-42, https://doi.org/10.5194/gmd-2022-42, 2022
Preprint under review for GMD
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as stand-alone 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 off-line high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores including on the cloud with improved access, performance, and accuracy.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
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.
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.
Yulu Qiu, Zhiqiang Ma, Ke Li, Mengyu Huang, Jiujiang Sheng, Ping Tian, Jia Zhu, Weiwei Pu, Yingxiao Tang, Tingting Han, Huaigang Zhou, and Hong Liao
Atmos. Chem. Phys., 21, 17995–18010, https://doi.org/10.5194/acp-21-17995-2021, https://doi.org/10.5194/acp-21-17995-2021, 2021
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Photochemical pollution over the North China Plain (NCP) is attracting much concern. Our observations at a rural site in the NCP identified high peroxyacetyl nitrate (PAN) concentrations, even on cold days. Increased acetaldehyde concentration and hydroxyl radical production rates drive fast PAN formation. Moreover, our study emphasizes the importance of formaldehyde photolysis in PAN formation and calls for implementing strict volatile organic compound controls after summer over the NCP.
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.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
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.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
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.
Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy
Atmos. Chem. Phys., 21, 457–481, https://doi.org/10.5194/acp-21-457-2021, https://doi.org/10.5194/acp-21-457-2021, 2021
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We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
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.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
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.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
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.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
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.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
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.
Hao Kong, Jintai Lin, Ruixiong Zhang, Mengyao Liu, Hongjian Weng, Ruijing Ni, Lulu Chen, Jingxu Wang, Yingying Yan, and Qiang Zhang
Atmos. Chem. Phys., 19, 12835–12856, https://doi.org/10.5194/acp-19-12835-2019, https://doi.org/10.5194/acp-19-12835-2019, 2019
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We develop a computationally efficient space-based top-down method to inverting NOx emissions in major urban areas at high resolution. The inversion method uses long-term OMI NO2 data to enhance the horizontal resolution, and it accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition on NOx. The inversion results reveal fine-scale spatial information of emissions which is hardly captured by bottom-up inventories.
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.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
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.
Xiao Lu, Lin Zhang, Youfan Chen, Mi Zhou, Bo Zheng, Ke Li, Yiming Liu, Jintai Lin, Tzung-May Fu, and Qiang Zhang
Atmos. Chem. Phys., 19, 8339–8361, https://doi.org/10.5194/acp-19-8339-2019, https://doi.org/10.5194/acp-19-8339-2019, 2019
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Severe and deteriorating surface ozone pollution over major Chinese cities has become an emerging environmental concern in China. This study assesses the source contributions (including anthropogenic, background, and individual natural sources) and meteorological influences of surface ozone over China in 2016–2017 using the GEOS-Chem chemical transport model at high horizontal resolution with the most up-to-date Chinese anthropogenic emission inventory.
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.
Huang Zheng, Shaofei Kong, Fangqi Wu, Yi Cheng, Zhenzhen Niu, Shurui Zheng, Guowei Yang, Liquan Yao, Qin Yan, Jian Wu, Mingming Zheng, Nan Chen, Ke Xu, Yingying Yan, Dantong Liu, Delong Zhao, Tianliang Zhao, Yongqing Bai, Shuanglin Li, and Shihua Qi
Atmos. Chem. Phys., 19, 4499–4516, https://doi.org/10.5194/acp-19-4499-2019, https://doi.org/10.5194/acp-19-4499-2019, 2019
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This study simultaneously observed black carbon (BC) at five sites in central China and on the south edge of North China Plain, which have the most serious air pollution issues in China. The differences in BC properties between different air quality conditions and the property changes during transportation were studied. The main findings of this study were that during the downwind transportation of air, the BC mass concentration increased, whereas the absorption Ångström exponent decreased.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
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.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Lei Sun, Likun Xue, Yuhang Wang, Longlei Li, Jintai Lin, Ruijing Ni, Yingying Yan, Lulu Chen, Juan Li, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 19, 1455–1469, https://doi.org/10.5194/acp-19-1455-2019, https://doi.org/10.5194/acp-19-1455-2019, 2019
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We quantified the detailed impacts of meteorology and anthropogenic emissions on surface O3 increase in central eastern China between 2003 and 2015 using GEOS-Chem. The emission change plays a more important role than the meteorological change, while the regions with a larger O3 increase are more sensitive to meteorology. NMVOC emission change dominated the O3 increase in eastern CEC, while NOx emission change led to an O3 increase in western and central CEC and O3 decrease in urban areas.
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).
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
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China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
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.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952, https://doi.org/10.5194/acp-18-12933-2018, https://doi.org/10.5194/acp-18-12933-2018, 2018
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Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
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.
Ruijing Ni, Jintai Lin, Yingying Yan, and Weili Lin
Atmos. Chem. Phys., 18, 11447–11469, https://doi.org/10.5194/acp-18-11447-2018, https://doi.org/10.5194/acp-18-11447-2018, 2018
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By integrating several modeling methods, we find considerable contributions of foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For anthropogenic ozone over China, the foreign contribution is 40–50 % below 2 km and 85 % in the upper troposphere. For total foreign anthropogenic ozone over China, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
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.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
Jiawei Zhuang, Daniel J. Jacob, and Sebastian D. Eastham
Atmos. Chem. Phys., 18, 6039–6055, https://doi.org/10.5194/acp-18-6039-2018, https://doi.org/10.5194/acp-18-6039-2018, 2018
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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.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
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.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Yingying Yan, Jintai Lin, and Cenlin He
Atmos. Chem. Phys., 18, 1185–1202, https://doi.org/10.5194/acp-18-1185-2018, https://doi.org/10.5194/acp-18-1185-2018, 2018
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Examining observed and simulated ozone at about 1000 sites during 1990–2014, we find a clear diurnal cycle both in the magnitude of ozone trends and in the relative importance of climate variability versus anthropogenic emissions to ozone changes, which has policy implications to mitigate ozone at night and other non-peak hours.
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.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Hongyan Zhao, Xin Li, Qiang Zhang, Xujia Jiang, Jintai Lin, Glen P. Peters, Meng Li, Guannan Geng, Bo Zheng, Hong Huo, Lin Zhang, Haikun Wang, Steven J. Davis, and Kebin He
Atmos. Chem. Phys., 17, 10367–10381, https://doi.org/10.5194/acp-17-10367-2017, https://doi.org/10.5194/acp-17-10367-2017, 2017
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Effective and efficient control of air pollution relies upon an understanding of the pollution sources. We conduct an interdisciplinary study and find that 33 % of China’s PM2.5-related premature mortality in 2010 were caused by production emission in other regions; 56 % of the mortality was related to consumption in other regions. Multilateral and multi-stage cooperation under a regional sustainable development framework is in urgent need to mitigate air pollution and related health impacts.
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.
Guannan Geng, Qiang Zhang, Randall V. Martin, Jintai Lin, Hong Huo, Bo Zheng, Siwen Wang, and Kebin He
Atmos. Chem. Phys., 17, 4131–4145, https://doi.org/10.5194/acp-17-4131-2017, https://doi.org/10.5194/acp-17-4131-2017, 2017
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We investigated the impact of spatial proxies on the representation of gridded emissions by comparing six gridded NOx emission datasets over China developed from the same magnitude of emissions and different spatial proxies. GEOS-Chem-modeled NO2 columns from the six gridded emissions are compared with satellite-based columns from OMI. Results show that differences between modeled and satellite-based NO2 columns are sensitive to the spatial proxies used in the gridded emission inventories.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Alba Lorente, K. Folkert Boersma, Huan Yu, Steffen Dörner, Andreas Hilboll, Andreas Richter, Mengyao Liu, Lok N. Lamsal, Michael Barkley, Isabelle De Smedt, Michel Van Roozendael, Yang Wang, Thomas Wagner, Steffen Beirle, Jin-Tai Lin, Nickolay Krotkov, Piet Stammes, Ping Wang, Henk J. Eskes, and Maarten Krol
Atmos. Meas. Tech., 10, 759–782, https://doi.org/10.5194/amt-10-759-2017, https://doi.org/10.5194/amt-10-759-2017, 2017
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Choices and assumptions made to represent the state of the atmosphere introduce an uncertainty of 42 % in the air mass factor calculation in trace gas satellite retrievals in polluted regions. The AMF strongly depends on the choice of a priori trace gas profile, surface albedo data set and the correction method to account for clouds and aerosols. We call for well-designed validation exercises focusing on situations when AMF structural uncertainty has the highest impact on satellite retrievals.
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.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
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.
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.
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.
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.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Yuanzheng Cui, Jintai Lin, Chunqiao Song, Mengyao Liu, Yingying Yan, Yuan Xu, and Bo Huang
Atmos. Chem. Phys., 16, 6207–6221, https://doi.org/10.5194/acp-16-6207-2016, https://doi.org/10.5194/acp-16-6207-2016, 2016
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We find rapid NO2 growth over Western China over 2005–2013 at a rate which exceeds the rates over the well-known polluted regions in the east. A nested GEOS-Chem simulation and Chinese official emission data confirm that anthropogenic emissions are the main driver of NO2 variations. Additional socioeconomic analysis suggests that this rapid NO2 growth is likely related to the fast industrialization and urbanization along with the "Go West" movement as well as relatively weak emission controls.
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.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
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.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
Yingying Yan, Jintai Lin, Jinxuan Chen, and Lu Hu
Atmos. Chem. Phys., 16, 2381–2400, https://doi.org/10.5194/acp-16-2381-2016, https://doi.org/10.5194/acp-16-2381-2016, 2016
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We use a newly built two-way coupling system of the GEOS-Chem CTM to simulate the global tropospheric O3 in 2009. It significantly improves the simulation upon the global model by comparisons with a suite of ground, aircraft, and satellite measurements, also reduces the global OH by 5 % with enhancements by 5 % in the lifetimes of MCF and methane. Therefore, improving model representations of small-scale processes is a critical step forward to understanding the global tropospheric chemistry.
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.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
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.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
J.-T. Lin, M.-Y. Liu, J.-Y. Xin, K. F. Boersma, R. Spurr, R. Martin, and Q. Zhang
Atmos. Chem. Phys., 15, 11217–11241, https://doi.org/10.5194/acp-15-11217-2015, https://doi.org/10.5194/acp-15-11217-2015, 2015
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We conduct an improved OMI-based retrieval of tropospheric NO2 VCDs (POMINO) over China by explicitly accounting for aerosol optical effects and surface reflectance anisotropy. Compared to the traditional implicit aerosol treatment, an explicit treatment greatly lowers NO2 VCDs and subsequently estimated NOx emissions over eastern China, but with large spatiotemporal dependence. An explicit treatment also better captures high-pollution days. Effects of surface reflectance treatments are smaller.
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
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 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
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 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.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
Y.-Y. Yan, J.-T. Lin, Y. Kuang, D. Yang, and L. Zhang
Atmos. Chem. Phys., 14, 12649–12663, https://doi.org/10.5194/acp-14-12649-2014, https://doi.org/10.5194/acp-14-12649-2014, 2014
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Limited by coarse resolutions, global chemical transport models cannot well capture small-scale nonlinear processes. To alleviate the problem, we develop a two-way coupled system to integrate the global GEOS-Chem model and its three high-resolution nested models covering Asia, Europe and North America. Confirmed by comparisons with observations, the coupled system improves upon the global model with a 10% increase in global tropospheric CO, a 4% decrease in OH and a 4% increase in MCF lifetime.
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
T. B. Nguyen, M. M. Coggon, K. H. Bates, X. Zhang, R. H. Schwantes, K. A. Schilling, C. L. Loza, R. C. Flagan, P. O. Wennberg, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 3497–3510, https://doi.org/10.5194/acp-14-3497-2014, https://doi.org/10.5194/acp-14-3497-2014, 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
J.-T. Lin, R. V. Martin, K. F. Boersma, M. Sneep, P. Stammes, R. Spurr, P. Wang, M. Van Roozendael, K. Clémer, and H. Irie
Atmos. Chem. Phys., 14, 1441–1461, https://doi.org/10.5194/acp-14-1441-2014, https://doi.org/10.5194/acp-14-1441-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
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. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 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
J.-T. Lin, Z. Liu, Q. Zhang, H. Liu, J. Mao, and G. Zhuang
Atmos. Chem. Phys., 12, 12255–12275, https://doi.org/10.5194/acp-12-12255-2012, https://doi.org/10.5194/acp-12-12255-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurements
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizations
The impacts of marine-emitted halogens on OH radicals in East Asia during summer
Impact of eastern and central Pacific El Niño on lower tropospheric ozone in China
Contribution of Asian emissions to upper tropospheric CO over the remote Pacific
An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018
Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism construction
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Quantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversion
Model evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model study
Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products
A model for simultaneous evaluation of NO2, O3 and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysis
Influence of photochemical loss of volatile organic compounds on understanding ozone formation mechanism
North China Plain as a hot spot of ozone pollution exacerbated by extreme high temperatures
Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants
Impact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphere
Influence of total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODEs) in the Antarctic
Changes in anthropogenic precursor emissions drive shifts in the ozone seasonal cycle throughout the northern midlatitude troposphere
Amplified role of potential HONO sources in O3 formation in North China Plain during autumn haze aggravating processes
Improving NOX emissions in Beijing using network observations and a novel perturbed emissions ensemble
Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017
Surface ozone impacts on major crop production in China from 2010 to 2017
Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in China
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
A machine learning approach to quantify meteorological drivers of recent ozone pollution in China
Tropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathways
An integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulations
Observation-based Analysis of Ozone Production Sensitivity for Two Persistent Ozone Episodes in Guangdong, China
An assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonyls
Methane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observations
Evaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System Model
Ozone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescales
Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Improving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaign
Atmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)
Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2
Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mapping
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Impact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model results
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
Opinion: The germicidal effect of ambient air (open-air factor) revisited
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Study of different Carbon Bond 6 (CB6) mechanisms by using a concentration sensitivity analysis
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285, https://doi.org/10.5194/acp-22-7273-2022, https://doi.org/10.5194/acp-22-7273-2022, 2022
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This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981, https://doi.org/10.5194/acp-22-5961-2022, https://doi.org/10.5194/acp-22-5961-2022, 2022
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Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
EGUsphere, https://doi.org/10.5194/egusphere-2022-117, https://doi.org/10.5194/egusphere-2022-117, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easy interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants even when having missing data.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Le Yuan, Olalekan Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-161, https://doi.org/10.5194/acp-2022-161, 2022
Revised manuscript accepted for ACP
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Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing emissions inventories using air quality models and routine in situ observations. Using this approach, we derived estimates of NOX emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Xiang Weng, Grant Forster, and Peer Nowack
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1075, https://doi.org/10.5194/acp-2021-1075, 2022
Revised manuscript accepted for ACP
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We compare two machine learning approaches to quantify meteorological drivers behind recent surface ozone across China. Our novel approaches show an overall better agreement between predicted and observed ozone than commonly used methods such as multiple linear regression, and we highlight several key implications of our analysis. For example, we find that almost half of the observed ozone trend between 2015 and 2019 on average might have been driven by meteorological factors.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-50, https://doi.org/10.5194/acp-2022-50, 2022
Revised manuscript accepted for ACP
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station-days exhibit ozone formation sensitivity to NOx, 20 % of the station-days are in the transitional regime sensitive to both NOx and VOC, only 13 % of the station-days are sensitive to VOC.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949, https://doi.org/10.5194/acp-22-929-2022, https://doi.org/10.5194/acp-22-929-2022, 2022
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Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys., 21, 16093–16120, https://doi.org/10.5194/acp-21-16093-2021, https://doi.org/10.5194/acp-21-16093-2021, 2021
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Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661, https://doi.org/10.5194/acp-21-15647-2021, https://doi.org/10.5194/acp-21-15647-2021, 2021
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
Le Cao, Simeng Li, and Luhang Sun
Atmos. Chem. Phys., 21, 12687–12714, https://doi.org/10.5194/acp-21-12687-2021, https://doi.org/10.5194/acp-21-12687-2021, 2021
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Gas-phase chemical reaction mechanisms, e.g., CB6 mechanism, are essential parts of the atmospheric transport model. In order to better understand the changes caused by the updates between different versions of the CB6 mechanism, in this study, the behavior of three different CB6 mechanisms in simulating ozone, nitrogen oxides and formaldehyde under two different emission conditions was analyzed using a concentration sensitivity analysis, and the reasons causing the deviations were figured out.
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Short summary
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.
Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is...
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