Articles | Volume 21, issue 10
https://doi.org/10.5194/acp-21-8357-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-8357-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
01 Jun 2021
Research article |
| 01 Jun 2021
| 01 Jun 2021
Isotopic constraints on atmospheric sulfate formation pathways in the Mt. Everest region, southern Tibetan Plateau
Kun Wang
State Key Laboratory of Cryospheric Science, Northwest Institute of Eco-Environment and Resources, Chinese Academy of Sciences (CAS), Lanzhou 730000, China
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
University of Chinese Academy of Sciences, Beijing 100049, China
Shohei Hattori
CORRESPONDING AUTHOR
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
State Key Laboratory of Isotope Geochemistry, Guangzhou Institute of Geochemistry, CAS, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China
Sakiko Ishino
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
National Institute of Polar Research, Research Organization of Information and Systems, Tokyo 190-8518, Japan
Becky Alexander
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
Kazuki Kamezaki
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
Faculty of Science and Technology, Sophia University, 7-1 Kioi-cho, Chiyoda-ku, Tokyo 102-8554, Japan
Naohiro Yoshida
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8502, Japan
Earth-Life Science Institute, Tokyo Institute of Technology, Meguro-ku, Tokyo 152-8551, Japan
National Institute of Information and Communications Technology, Koganei, Tokyo 184-8795, Japan
Shichang Kang
CORRESPONDING AUTHOR
State Key Laboratory of Cryospheric Science, Northwest Institute of Eco-Environment and Resources, Chinese Academy of Sciences (CAS), Lanzhou 730000, China
CAS Center for Excellence in Tibetan Plateau Earth Sciences, Beijing 100101, China
University of Chinese Academy of Sciences, Beijing 100049, China
Related authors
No articles found.
Jakob Pernov, William Aeberhard, Michele Volpi, Eliza Harris, Benjamin Hohermuth, Sakiko Ishino, Ragnhild Bieltvedt Skeie, Stephan Henne, Ulas Im, Patricia Quinn, Lucia Upchurch, and Julia Schmale
EGUsphere, https://doi.org/10.5194/egusphere-2024-3379, https://doi.org/10.5194/egusphere-2024-3379, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
MSAp is a vital part of the Arctic climate system. Numerical models struggle to reproduce the seasonal cycle of MSAp. We evaluate three numerical models and one reanalysis product’s ability to simulate MSAp. We develop data-driven models for MSAp at four High Arctic stations. The data-driven models outperform the numerical models and reanalysis product and identified precursor source, chemical processing, and removal-related features as being important for modeling MSAp.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
Short summary
Short summary
Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
Short summary
Short summary
Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
Atmos. Chem. Phys., 24, 4895–4914, https://doi.org/10.5194/acp-24-4895-2024, https://doi.org/10.5194/acp-24-4895-2024, 2024
Short summary
Short summary
Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
Chaman Gul, Shichang Kang, Yuanjian Yang, Xinlei Ge, and Dong Guo
EGUsphere, https://doi.org/10.5194/egusphere-2024-1144, https://doi.org/10.5194/egusphere-2024-1144, 2024
Preprint archived
Short summary
Short summary
Long-term variations in upper atmospheric temperature and water vapor in the selected domains of time and space are presented. The temperature during the past two decades showed a cooling trend and water vapor showed an increasing trend and had an inverse relation with temperature in selected domains of space and time. Seasonal temperature variations are distinct, with a summer minimum and a winter maximum. Our results can be an early warning indication for future climate change.
Jianzhong Xu, Xinghua Zhang, Wenhui Zhao, Lixiang Zhai, Miao Zhong, Jinsen Shi, Junying Sun, Yanmei Liu, Conghui Xie, Yulong Tan, Kemei Li, Xinlei Ge, Qi Zhang, and Shichang Kang
Earth Syst. Sci. Data, 16, 1875–1900, https://doi.org/10.5194/essd-16-1875-2024, https://doi.org/10.5194/essd-16-1875-2024, 2024
Short summary
Short summary
A comprehensive aerosol observation project was carried out in the Tibetan Plateau (TP) and its surroundings in recent years to investigate the properties and sources of atmospheric aerosols as well as their regional differences by performing multiple intensive field observations. The release of this dataset can provide basic and systematic data for related research in the atmospheric, cryospheric, and environmental sciences in this unique region.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
Short summary
Short summary
Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Yuling Hu, Haipeng Yu, Shichang Kang, Junhua Yang, Mukesh Rai, Xiufeng Yin, Xintong Chen, and Pengfei Chen
Atmos. Chem. Phys., 24, 85–107, https://doi.org/10.5194/acp-24-85-2024, https://doi.org/10.5194/acp-24-85-2024, 2024
Short summary
Short summary
The Tibetan Plateau (TP) saw a record-breaking aerosol pollution event from April 20 to May 10, 2016. We studied the impact of aerosol–meteorology feedback on the transboundary transport flux of black carbon (BC) during this severe pollution event. It was found that the aerosol–meteorology feedback decreases the transboundary transport flux of BC from the central and western Himalayas towards the TP. This study is of great significance for the protection of the ecological environment of the TP.
Kazuki Kamezaki, Sebastian O. Danielache, Shigeyuki Ishidoya, Takahisa Maeda, and Shohei Murayama
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-209, https://doi.org/10.5194/amt-2023-209, 2023
Revised manuscript not accepted
Short summary
Short summary
Recently, MIRA Pico, a portable continuous carbonyl sulfide (COS) concentration analyzer using mid-infrared absorption, has been released. MIRA Pico has a lower cost and is smaller than conventional laser COS analyzers. However, actual COS atmospheric measurement results using MIRA Pico have not yet been reported. In this study, we modified and tested the MIRA Pico for atmospheric COS concentration measurements. We used the modified MIRA Pico for observations at Tsukuba, Japan.
Xiufeng Yin, Dipesh Rupakheti, Guoshuai Zhang, Jiali Luo, Shichang Kang, Benjamin de Foy, Junhua Yang, Zhenming Ji, Zhiyuan Cong, Maheswar Rupakheti, Ping Li, Yuling Hu, and Qianggong Zhang
Atmos. Chem. Phys., 23, 10137–10143, https://doi.org/10.5194/acp-23-10137-2023, https://doi.org/10.5194/acp-23-10137-2023, 2023
Short summary
Short summary
The monthly mean surface ozone concentrations peaked earlier in the south in April and May and later in the north in June and July over the Tibetan Plateau. The migration of monthly surface ozone peaks was coupled with the synchronous movement of tropopause folds and the westerly jet that created conditions conducive to stratospheric ozone intrusion. Stratospheric ozone intrusion significantly contributed to surface ozone across the Tibetan Plateau.
Huiming Lin, Yindong Tong, Long Chen, Chenghao Yu, Zhaohan Chu, Qianru Zhang, Xiufeng Yin, Qianggong Zhang, Shichang Kang, Junfeng Liu, James Schauer, Benjamin de Foy, and Xuejun Wang
Atmos. Chem. Phys., 23, 3937–3953, https://doi.org/10.5194/acp-23-3937-2023, https://doi.org/10.5194/acp-23-3937-2023, 2023
Short summary
Short summary
Lhasa is the largest city in the Tibetan Plateau, and its atmospheric mercury concentrations represent the highest level of pollution in this region. Unexpectedly high concentrations of atmospheric mercury species were found. Combined with the trajectory analysis, the high atmospheric mercury concentrations may have originated from external long-range transport. Local sources, especially special mercury-related sources, are important factors influencing the variability of atmospheric mercury.
Shaoyong Wang, Xiaobo He, Shichang Kang, Hui Fu, and Xiaofeng Hong
The Cryosphere, 16, 5023–5040, https://doi.org/10.5194/tc-16-5023-2022, https://doi.org/10.5194/tc-16-5023-2022, 2022
Short summary
Short summary
This study used the sine-wave exponential model and long-term water stable isotopic data to estimate water mean residence time (MRT) and its influencing factors in a high-altitude permafrost catchment (5300 m a.s.l.) in the central Tibetan Plateau (TP). MRT for stream and supra-permafrost water was estimated at 100 and 255 d, respectively. Climate and vegetation factors affected the MRT of stream and supra-permafrost water mainly by changing the thickness of the permafrost active layer.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
Short summary
Short summary
Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
Short summary
Short summary
We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Jizu Chen, Wentao Du, Shichang Kang, Xiang Qin, Weijun Sun, Yang Li, Yushuo Liu, Lihui Luo, and Youyan Jiang
The Cryosphere Discuss., https://doi.org/10.5194/tc-2022-179, https://doi.org/10.5194/tc-2022-179, 2022
Preprint withdrawn
Short summary
Short summary
This study developed a dynamic deposition model of light absorbing particles (LAPs), which coupled with a surface energy and mass balance model. Based on the coupled model, we assessed atmospheric deposited BC effect on glacier melting, and quantified global warming and increment of emitted black carbon respective contributions to current accelerated glacier melting.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
Short summary
Short summary
A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
Chaman Gul, Shichang Kang, Siva Praveen Puppala, Xiaokang Wu, Cenlin He, Yangyang Xu, Inka Koch, Sher Muhammad, Rajesh Kumar, and Getachew Dubache
Atmos. Chem. Phys., 22, 8725–8737, https://doi.org/10.5194/acp-22-8725-2022, https://doi.org/10.5194/acp-22-8725-2022, 2022
Short summary
Short summary
This work aims to understand concentrations, spatial variability, and potential source regions of light-absorbing impurities (black carbon aerosols, dust particles, and organic carbon) in the surface snow of central and western Himalayan glaciers and their impact on snow albedo and radiative forcing.
Xinghua Zhang, Wenhui Zhao, Lixiang Zhai, Miao Zhong, Jinsen Shi, Junying Sun, Yanmei Liu, Conghui Xie, Yulong Tan, Kemei Li, Xinlei Ge, Qi Zhang, Shichang Kang, and Jianzhong Xu
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-211, https://doi.org/10.5194/essd-2022-211, 2022
Manuscript not accepted for further review
Short summary
Short summary
A comprehensive aerosol observation project was carried out in the Tibetan Plateau (TP) in recent years to investigate the properties and sources of atmospheric aerosols as well as their regional differences by performing multiple short-term intensive field observations. The real-time online high-time-resolution (hourly) data of aerosol properties in the different TP region are integrated in a new dataset and can provide supporting for related studies in in the TP.
Yongqin Liu, Pengcheng Fang, Bixi Guo, Mukan Ji, Pengfei Liu, Guannan Mao, Baiqing Xu, Shichang Kang, and Junzhi Liu
Earth Syst. Sci. Data, 14, 2303–2314, https://doi.org/10.5194/essd-14-2303-2022, https://doi.org/10.5194/essd-14-2303-2022, 2022
Short summary
Short summary
Glaciers are an important pool of microorganisms, organic carbon, and nitrogen. This study constructed the first dataset of microbial abundance and total nitrogen in Tibetan Plateau (TP) glaciers and the first dataset of dissolved organic carbon in ice cores on the TP. These new data could provide valuable information for research on the glacier carbon and nitrogen cycle and help in assessing the potential impacts of glacier retreat due to global warming on downstream ecosystems.
Mukesh Rai, Shichang Kang, Junhua Yang, Maheswar Rupakheti, Dipesh Rupakheti, Lekhendra Tripathee, Yuling Hu, and Xintong Chen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-199, https://doi.org/10.5194/acp-2022-199, 2022
Revised manuscript not accepted
Short summary
Short summary
Our study revealed distinctive seasonality with the maximum and minimum aerosol concentrations during the winter and summer seasons respectively. However, interestingly summer high (AOD > 0.8) was observed over South Asia. The highest aerosols are laden over South Asia and East China within 1–2 km, however, aerosol overshooting found up to 10 km due to the deep convection process. Whereas, integrated aerosol transport for OC during spring was found to be 5 times higher than the annual mean.
Huiming Lin, Yindong Tong, Chenghao Yu, Long Chen, Xiufeng Yin, Qianggong Zhang, Shichang Kang, Lun Luo, James Schauer, Benjamin de Foy, and Xuejun Wang
Atmos. Chem. Phys., 22, 2651–2668, https://doi.org/10.5194/acp-22-2651-2022, https://doi.org/10.5194/acp-22-2651-2022, 2022
Short summary
Short summary
The Tibetan Plateau is known as
The Third Poleand is generally considered to be a clean area owing to its high altitude. However, it may receive be impacted by air pollutants transported from the Indian subcontinent. Pollutants generally enter the Tibetan Plateau in several ways. Among them is the Yarlung Zangbu–Brahmaputra Grand Canyon. In this study, we identified the influence of the Indian summer monsoon on the origin, transport, and behavior of mercury in this area.
Shichang Kang, Yulan Zhang, Pengfei Chen, Junming Guo, Qianggong Zhang, Zhiyuan Cong, Susan Kaspari, Lekhendra Tripathee, Tanguang Gao, Hewen Niu, Xinyue Zhong, Xintong Chen, Zhaofu Hu, Xiaofei Li, Yang Li, Bigyan Neupane, Fangping Yan, Dipesh Rupakheti, Chaman Gul, Wei Zhang, Guangming Wu, Ling Yang, Zhaoqing Wang, and Chaoliu Li
Earth Syst. Sci. Data, 14, 683–707, https://doi.org/10.5194/essd-14-683-2022, https://doi.org/10.5194/essd-14-683-2022, 2022
Short summary
Short summary
The Tibetan Plateau is important to the Earth’s climate. However, systematically observed data here are scarce. To perform more integrated and in-depth investigations of the origins and distributions of atmospheric pollutants and their impacts on cryospheric change, systematic data of black carbon and organic carbon from the atmosphere, glaciers, snow cover, precipitation, and lake sediment cores over the plateau based on the Atmospheric Pollution and Cryospheric Change program are provided.
Jinlei Chen, Shichang Kang, Wentao Du, Junming Guo, Min Xu, Yulan Zhang, Xinyue Zhong, Wei Zhang, and Jizu Chen
The Cryosphere, 15, 5473–5482, https://doi.org/10.5194/tc-15-5473-2021, https://doi.org/10.5194/tc-15-5473-2021, 2021
Short summary
Short summary
Sea ice is retreating with rapid warming in the Arctic. It will continue and approach the worst predicted pathway released by the IPCC. The irreversible tipping point might show around 2060 when the oldest ice will have completely disappeared. It has a huge impact on human production. Ordinary merchant ships will be able to pass the Northeast Passage and Northwest Passage by the midcentury, and the opening time will advance to the next 10 years for icebreakers with moderate ice strengthening.
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
Short summary
Short summary
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 %.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
Short summary
Short summary
Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
Short summary
Short summary
We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Yongkang Xue, Tandong Yao, Aaron A. Boone, Ismaila Diallo, Ye Liu, Xubin Zeng, William K. M. Lau, Shiori Sugimoto, Qi Tang, Xiaoduo Pan, Peter J. van Oevelen, Daniel Klocke, Myung-Seo Koo, Tomonori Sato, Zhaohui Lin, Yuhei Takaya, Constantin Ardilouze, Stefano Materia, Subodh K. Saha, Retish Senan, Tetsu Nakamura, Hailan Wang, Jing Yang, Hongliang Zhang, Mei Zhao, Xin-Zhong Liang, J. David Neelin, Frederic Vitart, Xin Li, Ping Zhao, Chunxiang Shi, Weidong Guo, Jianping Tang, Miao Yu, Yun Qian, Samuel S. P. Shen, Yang Zhang, Kun Yang, Ruby Leung, Yuan Qiu, Daniele Peano, Xin Qi, Yanling Zhan, Michael A. Brunke, Sin Chan Chou, Michael Ek, Tianyi Fan, Hong Guan, Hai Lin, Shunlin Liang, Helin Wei, Shaocheng Xie, Haoran Xu, Weiping Li, Xueli Shi, Paulo Nobre, Yan Pan, Yi Qin, Jeff Dozier, Craig R. Ferguson, Gianpaolo Balsamo, Qing Bao, Jinming Feng, Jinkyu Hong, Songyou Hong, Huilin Huang, Duoying Ji, Zhenming Ji, Shichang Kang, Yanluan Lin, Weiguang Liu, Ryan Muncaster, Patricia de Rosnay, Hiroshi G. Takahashi, Guiling Wang, Shuyu Wang, Weicai Wang, Xu Zhou, and Yuejian Zhu
Geosci. Model Dev., 14, 4465–4494, https://doi.org/10.5194/gmd-14-4465-2021, https://doi.org/10.5194/gmd-14-4465-2021, 2021
Short summary
Short summary
The subseasonal prediction of extreme hydroclimate events such as droughts/floods has remained stubbornly low for years. This paper presents a new international initiative which, for the first time, introduces spring land surface temperature anomalies over high mountains to improve precipitation prediction through remote effects of land–atmosphere interactions. More than 40 institutions worldwide are participating in this effort. The experimental protocol and preliminary results are presented.
Shuang Yi, Chunqiao Song, Kosuke Heki, Shichang Kang, Qiuyu Wang, and Le Chang
The Cryosphere, 14, 2267–2281, https://doi.org/10.5194/tc-14-2267-2020, https://doi.org/10.5194/tc-14-2267-2020, 2020
Short summary
Short summary
High-Asia glaciers have been observed to be retreating the fastest in the southeastern Tibeten Plateau, where vast amounts of glacier and snow feed the streamflow of the Brahmaputra. Here, we provide the first monthly glacier and snow mass balance during 2002–2017 based on satellite gravimetry. The results confirm previous long-term decreases but reveal strong seasonal variations. This work helps resolve previous divergent model estimates and underlines the importance of meltwater.
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
Short summary
Short summary
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.
Meixin Zhang, Chun Zhao, Zhiyuan Cong, Qiuyan Du, Mingyue Xu, Yu Chen, Ming Chen, Rui Li, Yunfei Fu, Lei Zhong, Shichang Kang, Delong Zhao, and Yan Yang
Atmos. Chem. Phys., 20, 5923–5943, https://doi.org/10.5194/acp-20-5923-2020, https://doi.org/10.5194/acp-20-5923-2020, 2020
Short summary
Short summary
Analysis of multiple numerical experiments over the Himalayas and Tibetan Plateau (TP) shows that the complex topography results in 50 % stronger overall cross-Himalayan transport during the pre-monsoon season primarily due to the strengthened efficiency of near-surface meridional transport towards the TP, enhanced wind speed in some valleys and deeper valley channels associated with larger transported BC mass volume, which leads to 30–50 % stronger BC radiative heating over the TP.
Tamaki Fujinawa, Tomohiro O. Sato, Takayoshi Yamada, Seidai Nara, Yuki Uchiyama, Kodai Takahashi, Naohiro Yoshida, and Yasuko Kasai
Atmos. Meas. Tech., 13, 2119–2129, https://doi.org/10.5194/amt-13-2119-2020, https://doi.org/10.5194/amt-13-2119-2020, 2020
Short summary
Short summary
We performed an error analysis of SMILES observations for acetonitrile and a validation using the MLS observations by extracting the coincident points between SMILES and MLS data. The major error sources for the SMILES observations were quantitatively estimated. At upper pressure levels the difference between the two datasets increased because of an uncertainty in MLS observations. The results showed that SMILES has an advantage in measuring acetonitrile in the upper stratosphere and mesosphere.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
Short summary
Short summary
Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
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
Short summary
Short summary
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.
Xinghua Zhang, Jianzhong Xu, Shichang Kang, Qi Zhang, and Junying Sun
Atmos. Chem. Phys., 19, 7897–7911, https://doi.org/10.5194/acp-19-7897-2019, https://doi.org/10.5194/acp-19-7897-2019, 2019
Short summary
Short summary
Highly time resolved chemistry and sources of PM1 were measured by an Aerodyne HR-ToF-AMS at Waliguan Baseline Observatory, a high-altitude background station at the northeastern edge of Qinghai–Tibet Plateau (QTP), during summer 2017. Relatively higher mass concentration of PM1 and dominant sulfate contribution were observed in this site compared to those at other high-elevation sites in the southern or central QTP, indicating the different aerosol sources between them.
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
Short summary
Short summary
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.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
Short summary
Short summary
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
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
Short summary
Short summary
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.
Xin Wan, Shichang Kang, Maheswar Rupakheti, Qianggong Zhang, Lekhendra Tripathee, Junming Guo, Pengfei Chen, Dipesh Rupakheti, Arnico K. Panday, Mark G. Lawrence, Kimitaka Kawamura, and Zhiyuan Cong
Atmos. Chem. Phys., 19, 2725–2747, https://doi.org/10.5194/acp-19-2725-2019, https://doi.org/10.5194/acp-19-2725-2019, 2019
Short summary
Short summary
The sources of primary and secondary aerosols in the Hindu Kush–Himalayan–Tibetan Plateau region are not well known. Organic molecular tracers are useful for aerosol source apportionment. The characterization of molecular tracers were first systemically investigated and the contribution from primary and secondary sources to carbonaceous aerosols was estimated in the Kathmandu Valley. Our results demonstrate that biomass burning contributed a significant fraction to OC in the Kathmandu Valley.
Kazuki Kamezaki, Shohei Hattori, Enno Bahlmann, and Naohiro Yoshida
Atmos. Meas. Tech., 12, 1141–1154, https://doi.org/10.5194/amt-12-1141-2019, https://doi.org/10.5194/amt-12-1141-2019, 2019
Short summary
Short summary
Knowledge related to sulfur isotopic composition of carbonyl sulfide (OCS or COS), the most abundant atmospheric sulfur species, remains scarce. We present a new sampling system for collecting approx. 10 nmol of OCS from ambient air coupled with a purification system. The system presented herein is useful for application of sulfur isotopic compositions for investigation of OCS sources and sinks in the troposphere to elucidate its cycle and its contribution to background stratospheric sulfate.
Yanqing An, Jianzhong Xu, Lin Feng, Xinghua Zhang, Yanmei Liu, Shichang Kang, Bin Jiang, and Yuhong Liao
Atmos. Chem. Phys., 19, 1115–1128, https://doi.org/10.5194/acp-19-1115-2019, https://doi.org/10.5194/acp-19-1115-2019, 2019
Short summary
Short summary
Detailed molecular chemical composition of water-soluble organic matter in the Himalayas was characterized by positive electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry for the first time. Many products formed from biogenic volatile organic compounds and biomass-burning-emitted compounds were found in the organic compounds, suggesting the important contribution of these two sources in the Himalayas.
Zhiwen Dong, Shichang Kang, Dahe Qin, Yaping Shao, Sven Ulbrich, and Xiang Qin
The Cryosphere, 12, 3877–3890, https://doi.org/10.5194/tc-12-3877-2018, https://doi.org/10.5194/tc-12-3877-2018, 2018
Short summary
Short summary
This study aimed to provide a first and unique record of physicochemical properties and mixing states of LAPs at the glacier and atmosphere interface over the northeastern Tibetan Plateau to determine the individual LAPs' structure aging and mixing state changes through the atmospheric deposition process from atmosphere to glacier–snowpack surface, thereby helping to characterize the LAPs' radiative forcing and climate effects in the cryosphere region.
Zhiyuan Cong, Shaopeng Gao, Wancang Zhao, Xin Wang, Guangming Wu, Yulan Zhang, Shichang Kang, Yongqin Liu, and Junfeng Ji
The Cryosphere, 12, 3177–3186, https://doi.org/10.5194/tc-12-3177-2018, https://doi.org/10.5194/tc-12-3177-2018, 2018
Short summary
Short summary
Cryoconites from glaciers on the Tibetan Plateau and surrounding area were studied for iron oxides. We found that goethite is the predominant iron oxide form. Using the abundance, speciation and optical properties of iron oxides, the total light absorption was quantitatively attributed to goethite, hematite, black carbon and organic matter. Such findings are essential to understand the relative significance of anthropogenic and natural impacts.
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
Short summary
Short summary
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.
Xintong Chen, Shichang Kang, Zhiyuan Cong, Junhua Yang, and Yaoming Ma
Atmos. Chem. Phys., 18, 12859–12875, https://doi.org/10.5194/acp-18-12859-2018, https://doi.org/10.5194/acp-18-12859-2018, 2018
Short summary
Short summary
To understand the impact of transboundary atmospheric black carbon on the Mt. Everest region and depict the transport pathways in different spatiotemporal scales, we first investigated the concentration level, temporal variation, and sources of black carbon based on high-resolution (2-year) measurements at Qomolangma (Mt. Everest) Station (4276 m a.s.l.). Next, the WRF-Chem simulations were used to reveal the transport mechanisms of black carbon from southern Asia to the Mt. Everest region.
Cenlin He, Mark G. Flanner, Fei Chen, Michael Barlage, Kuo-Nan Liou, Shichang Kang, Jing Ming, and Yun Qian
Atmos. Chem. Phys., 18, 11507–11527, https://doi.org/10.5194/acp-18-11507-2018, https://doi.org/10.5194/acp-18-11507-2018, 2018
Short summary
Short summary
Snow albedo plays a key role in the Earth and climate system. It can be affected by impurities and snow properties. This study implements new parameterizations into a widely used snow model to account for effects of snow shape and black carbon–snow mixing state on snow albedo reduction in the Tibetan Plateau. This study points toward an imperative need for extensive measurements and improved model characterization of snow grain shape and aerosol–snow mixing state in Tibet and elsewhere.
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
Short summary
Short summary
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.
Xiufeng Yin, Shichang Kang, Benjamin de Foy, Yaoming Ma, Yindong Tong, Wei Zhang, Xuejun Wang, Guoshuai Zhang, and Qianggong Zhang
Atmos. Chem. Phys., 18, 10557–10574, https://doi.org/10.5194/acp-18-10557-2018, https://doi.org/10.5194/acp-18-10557-2018, 2018
Short summary
Short summary
Total gaseous mercury concentrations were measured at Nam Co Station on the inland Tibetan Plateau for ~ 3 years. The mean concentration of TGM during the entire monitoring period was 1.33 ± 0.24 ngm-3, ranking it the lowest in China and indicating the pristine atmospheric environment of the inland Tibetan Plateau. Variation of TGM at Nam Co was affected by regional surface reemission, vertical mixing and long-range transported atmospheric mercury, which was associated with the Indian monsoon.
Hewen Niu, Shichang Kang, Hailong Wang, Rudong Zhang, Xixi Lu, Yun Qian, Rukumesh Paudyal, Shijin Wang, Xiaofei Shi, and Xingguo Yan
Atmos. Chem. Phys., 18, 6441–6460, https://doi.org/10.5194/acp-18-6441-2018, https://doi.org/10.5194/acp-18-6441-2018, 2018
Short summary
Short summary
Deposition of light-absorbing carbonaceous aerosol on the surface of glaciers can greatly alter the energy fluxes of glaciers. Two years of continuous observations of carbonaceous aerosols in a glacierized region are analyzed. We mainly studied the light absorption properties of carbonaceous aerosol and have employed a global aerosol–climate model to estimate source attributions of atmospheric black carbon.
D. Rupakheti, S. Kang, Z. Cong, M. Rupakheti, L. Tripathee, A. K. Panday, and B. Holben
Int. Arch. Photogramm. Remote Sens. Spatial Inf. Sci., XLII-3, 1493–1497, https://doi.org/10.5194/isprs-archives-XLII-3-1493-2018, https://doi.org/10.5194/isprs-archives-XLII-3-1493-2018, 2018
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
Short summary
Short summary
We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Chaman Gul, Siva Praveen Puppala, Shichang Kang, Bhupesh Adhikary, Yulan Zhang, Shaukat Ali, Yang Li, and Xiaofei Li
Atmos. Chem. Phys., 18, 4981–5000, https://doi.org/10.5194/acp-18-4981-2018, https://doi.org/10.5194/acp-18-4981-2018, 2018
Short summary
Short summary
Snow and ice samples were collected from six glaciers and multiple mountain valleys from northern Pakistan. Samples were analyzed for black carbon and water-insoluble organic carbon. Relatively high concentrations of black carbon, organic carbon, and dust were reported. Snow albedo and radiative forcing were estimated for the snow samples. Possible source regions of pollutants were identified through various techniques.
Xinghua Zhang, Jianzhong Xu, Shichang Kang, Yanmei Liu, and Qi Zhang
Atmos. Chem. Phys., 18, 4617–4638, https://doi.org/10.5194/acp-18-4617-2018, https://doi.org/10.5194/acp-18-4617-2018, 2018
Short summary
Short summary
Highly time and chemically resolved submicron aerosol properties were characterized online for the first time in a high-altitude site (Qomolangma station, 4276 m a.s.l.) in the northern Himalayas by using the Aerodyne HR-ToF-AMS. Biomass burning plumes were frequently observed and the dynamic processes (emissions, transport, and chemical processing) were characterized. The source and chemical composition of organic aerosol were further elucidated using positive matrix factorization analysis.
Haipeng Wang, Jianhui Chen, Shengda Zhang, David D. Zhang, Zongli Wang, Qinghai Xu, Shengqian Chen, Shijin Wang, Shichang Kang, and Fahu Chen
Clim. Past, 14, 383–396, https://doi.org/10.5194/cp-14-383-2018, https://doi.org/10.5194/cp-14-383-2018, 2018
Short summary
Short summary
The chironomid-inferred temperature record from Gonghai Lake exhibits a stepwise decreasing trend since 4 ka. A cold event in the Era of Disunity, the Sui-Tang Warm Period, the Medieval Warm Period and the Little Ice Age can all be recognized in our record, as well as in many other temperature reconstructions in China. Local wars in Shanxi Province, documented in the historical literature during the past 2700 years, are statistically significantly correlated with changes in temperature.
Yulan Zhang, Shichang Kang, Michael Sprenger, Zhiyuan Cong, Tanguang Gao, Chaoliu Li, Shu Tao, Xiaofei Li, Xinyue Zhong, Min Xu, Wenjun Meng, Bigyan Neupane, Xiang Qin, and Mika Sillanpää
The Cryosphere, 12, 413–431, https://doi.org/10.5194/tc-12-413-2018, https://doi.org/10.5194/tc-12-413-2018, 2018
Short summary
Short summary
Light-absorbing impurities deposited on snow can reduce surface albedo and contribute to the near-worldwide melting of snowpack and ice. This study focused on the black carbon and mineral dust in snow cover on the Tibetan Plateau. We discussed their concentrations, distributions, possible sources, and albedo reduction and radiative forcing. Findings indicated that the impacts of black carbon and mineral dust need to be properly accounted for in future regional climate projections.
Sakae Toyoda, Naohiro Yoshida, Shinji Morimoto, Shuji Aoki, Takakiyo Nakazawa, Satoshi Sugawara, Shigeyuki Ishidoya, Mitsuo Uematsu, Yoichi Inai, Fumio Hasebe, Chusaku Ikeda, Hideyuki Honda, and Kentaro Ishijima
Atmos. Chem. Phys., 18, 833–844, https://doi.org/10.5194/acp-18-833-2018, https://doi.org/10.5194/acp-18-833-2018, 2018
Short summary
Short summary
By analysis of whole air samples collected by balloon-borne compact cryogenic samplers, we found that apparent isotope effect for stratospheric N2O between 25 and 30 km over the Equator is larger than that observed in other latitudes and that it is almost equal to the effect predicted by laboratory simulation experiments. These results suggest that equatorial middle stratosphere can be treated as an isolated region when we consider the decomposition of N2O by photochemical processes.
Xinyue Zhong, Tingjun Zhang, Shichang Kang, Kang Wang, Lei Zheng, Yuantao Hu, and Huijuan Wang
The Cryosphere, 12, 227–245, https://doi.org/10.5194/tc-12-227-2018, https://doi.org/10.5194/tc-12-227-2018, 2018
Jianzhong Xu, Qi Zhang, Jinsen Shi, Xinlei Ge, Conghui Xie, Junfeng Wang, Shichang Kang, Ruixiong Zhang, and Yuhang Wang
Atmos. Chem. Phys., 18, 427–443, https://doi.org/10.5194/acp-18-427-2018, https://doi.org/10.5194/acp-18-427-2018, 2018
Short summary
Short summary
This manuscript presents results from a comprehensive field study using an HR-AMS coupled with a suite of other instruments in central Tibetan Plateau. The study discusses the chemical composition, sources, and processes of submicron aerosol during the transition from pre-monsoon to monsoon. Organic aerosol was overall highly oxidized during the entire study with higher O / C ratios during the pre-monsoon period. Sensitivity of air pollution transport with synoptic process was also evaluated.
Lin Feng, Yanqing An, Jianzhong Xu, Shichang Kang, Xiaofei Li, Yongqiang Zhou, Yunlin Zhang, Bin Jiang, and Yuhong Liao
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-507, https://doi.org/10.5194/bg-2017-507, 2017
Revised manuscript not accepted
Chaoliu Li, Fangping Yan, Shichang Kang, Pengfei Chen, Xiaowen Han, Zhaofu Hu, Guoshuai Zhang, Ye Hong, Shaopeng Gao, Bin Qu, Zhejing Zhu, Jiwei Li, Bing Chen, and Mika Sillanpää
Atmos. Chem. Phys., 17, 11899–11912, https://doi.org/10.5194/acp-17-11899-2017, https://doi.org/10.5194/acp-17-11899-2017, 2017
Short summary
Short summary
In this study, we found, due to contribution of carbonates, previously reported BC concentration in atmosphere of the Himalayas and Tibetan Plateau (HTP) were overestimated by around 39–52 %. Meanwhile, we found BC deposition of lake cores overestimated the atmospheric deposition of BC in the HTP; BC depositions of glacier region reflected actual values of 17.9 ± 5.3 mg m−2 a−1. The above results are critical for studying atmospheric distribution and chemical transport of BC in and around the HTP.
Xiufeng Yin, Shichang Kang, Benjamin de Foy, Zhiyuan Cong, Jiali Luo, Lang Zhang, Yaoming Ma, Guoshuai Zhang, Dipesh Rupakheti, and Qianggong Zhang
Atmos. Chem. Phys., 17, 11293–11311, https://doi.org/10.5194/acp-17-11293-2017, https://doi.org/10.5194/acp-17-11293-2017, 2017
Short summary
Short summary
We presented 5-year surface ozone measurements at Nam Co in the inland Tibetan Plateau and made a synthesis comparison of diurnal and seasonal patterns on regional and hemispheric scales. Surface ozone at Nam Co is mainly dominated by natural processes and is less influenced by stratospheric intrusions and human activities than on the rim of the Tibetan Plateau. Ozone at Nam Co is representative of background that is valuable for studying ozone-related effects on large scales.
Dipesh Rupakheti, Bhupesh Adhikary, Puppala Siva Praveen, Maheswar Rupakheti, Shichang Kang, Khadak Singh Mahata, Manish Naja, Qianggong Zhang, Arnico Kumar Panday, and Mark G. Lawrence
Atmos. Chem. Phys., 17, 11041–11063, https://doi.org/10.5194/acp-17-11041-2017, https://doi.org/10.5194/acp-17-11041-2017, 2017
Short summary
Short summary
For the first time, atmospheric composition was monitored during pre-monsoon season of 2013 at Lumbini (UNESCO world heritage site as birthplace of the Buddha). PM and O3 frequently exceeded WHO guidelines. Pollution concentration, diurnal characteristics and influence of open burning on air quality in Lumbini were investigated. Potential source regions were also identified. Results show that air pollution at this site is of a great concern, requiring prompt attention for mitigation.
Xin Wan, Shichang Kang, Quanlian Li, Dipesh Rupakheti, Qianggong Zhang, Junming Guo, Pengfei Chen, Lekhendra Tripathee, Maheswar Rupakheti, Arnico K. Panday, Wu Wang, Kimitaka Kawamura, Shaopeng Gao, Guangming Wu, and Zhiyuan Cong
Atmos. Chem. Phys., 17, 8867–8885, https://doi.org/10.5194/acp-17-8867-2017, https://doi.org/10.5194/acp-17-8867-2017, 2017
Short summary
Short summary
Biomass burning (BB) tracers in the aerosols in Lumbini, northern IGP, were studied for the first time. The levoglucosan was the predominant tracer and BB significantly contributed to the air quality in Lumbini. Mixed crop residues and hardwood were main burning materials. BB emissions constituted large fraction of OC, especially during the post-monsoon season. The sources of BB aerosols in Lumbini varies seasonally due to the influence of local emissions and long-range transport.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
Short summary
Short summary
We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Bin Liu, Zhiyuan Cong, Yuesi Wang, Jinyuan Xin, Xin Wan, Yuepeng Pan, Zirui Liu, Yonghong Wang, Guoshuai Zhang, Zhongyan Wang, Yongjie Wang, and Shichang Kang
Atmos. Chem. Phys., 17, 449–463, https://doi.org/10.5194/acp-17-449-2017, https://doi.org/10.5194/acp-17-449-2017, 2017
Short summary
Short summary
The first observation net of background atmospheric aerosols of the Himalayas and Tibetan Plateau were conducted in 2011–2013, and the aerosol mass loadings were especially illustrated in this paper. Consequently, these terrestrial aerosol masses were strongly ecosystem-dependent, with various seasonality and diurnal cycles at these sites. These findings implicate that regional characteristics and fine-particle emissions need to be treated sensitively when assessing their climatic effects.
Jianzhong Xu, Jinsen Shi, Qi Zhang, Xinlei Ge, Francesco Canonaco, André S. H. Prévôt, Matthias Vonwiller, Sönke Szidat, Jinming Ge, Jianmin Ma, Yanqing An, Shichang Kang, and Dahe Qin
Atmos. Chem. Phys., 16, 14937–14957, https://doi.org/10.5194/acp-16-14937-2016, https://doi.org/10.5194/acp-16-14937-2016, 2016
Short summary
Short summary
This study deployed an AMS field study in Lanzhou, a city in northwestern China, evaluating the chemical composition, sources, and processes of urban aerosols during wintertime. In comparison with the results during summer in Lanzhou, the air pollution during winter was more severe and the sources were more complex. In addition, this paper estimates the contributions of fossil and non-fossil sources of organic carbon to primary and secondary organic carbon using the carbon isotopic method.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
Short summary
Short summary
This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Fangping Yan, Shichang Kang, Chaoliu Li, Yulan Zhang, Xiang Qin, Yang Li, Xiaopeng Zhang, Zhaofu Hu, Pengfei Chen, Xiaofei Li, Bin Qu, and Mika Sillanpää
The Cryosphere, 10, 2611–2621, https://doi.org/10.5194/tc-10-2611-2016, https://doi.org/10.5194/tc-10-2611-2016, 2016
Short summary
Short summary
DOC release of Laohugou Glacier No. 12 was 192 kg km−2 yr−1, of which 43.2 % could be decomposed and return to atmosphere as CO2 within 28 days, producing positive feedback in the warming process and influencing downstream ecosystems. Radiative forcing of snow pit DOC was calculated to be 0.43 W m−2, accounting for about 10 % of the radiative forcing caused by BC. Therefore, DOC is also a light-absorbing agent in glacierized regions, influencing the albedo of glacier surface and glacier melting.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
Short summary
Short summary
The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Shengyun Chen, Wenjie Liu, Qian Zhao, Lin Zhao, Qingbai Wu, Xingjie Lu, Shichang Kang, Xiang Qin, Shilong Chen, Jiawen Ren, and Dahe Qin
The Cryosphere Discuss., https://doi.org/10.5194/tc-2016-80, https://doi.org/10.5194/tc-2016-80, 2016
Revised manuscript not accepted
Short summary
Short summary
Experimental warming was manipulated using open top chambers in alpine grassland ecosystem in the permafrost regions of the Qinghai-Tibet Plateau. The results revealed variations of earlier thawing, later freezing and longer freezing-thawing periods in shallow soil. Further, the estimated permafrost table declined under the warming scenarios. The work will be helpful to evaluate the stability of Qinghai-Tibet Railway/Highway and estimate the release of carbon under the future climate warming.
Sakae Toyoda and Naohiro Yoshida
Atmos. Meas. Tech., 9, 2093–2101, https://doi.org/10.5194/amt-9-2093-2016, https://doi.org/10.5194/amt-9-2093-2016, 2016
Short summary
Short summary
Tiny variation in natural abundance ratios of stable isotopes of nitrogen and oxygen in nitrous oxide (N2O) can be used as a fingerprint of this trace gas that causes greenhouse effect and stratospheric ozone depletion. Toward the understanding of the global budget of N2O and its temporal change, we developed an automated sample preparation system that can be used to measure the stable isotope ratios in N2O in various air samples collected into flasks with high precision and less labor.
Yang Li, Jizu Chen, Shichang Kang, Chaoliu Li, Bin Qu, Lekhendra Tripathee, Fangping Yan, Yulan Zhang, Junmin Guo, Chaman Gul, and Xiang Qin
The Cryosphere Discuss., https://doi.org/10.5194/tc-2016-32, https://doi.org/10.5194/tc-2016-32, 2016
Preprint withdrawn
Short summary
Short summary
To our knowledge, this study constitutes the first quantitative dataset of the impacts of light absorbing particles (LAPs) on glacier ablation estimated directly from the northeastern edge of the Tibetan Plateau (TP).The average concentrations of black carbon (BC) and mineral dust (MD) in surface snow and ice at Laohugou Glacier No. 12 (LHG) were much higher than those detected in snow pits and ice cores in TP and Tien Shan mountains.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
Short summary
Short summary
We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
Koki Maeda, Sakae Toyoda, Midori Yano, Shohei Hattori, Makoto Fukasawa, Keiichi Nakajima, and Naohiro Yoshida
Biogeosciences, 13, 1341–1349, https://doi.org/10.5194/bg-13-1341-2016, https://doi.org/10.5194/bg-13-1341-2016, 2016
Short summary
Short summary
Nitrogen isotope ratios (δ15N) of NH4+ in dairy manure compost piles were studied. The δ15N–NH4+ values in different pile zones (top, side and core) show that extremely high nitrogen conversion, nitrification–denitrification activity of the microbes and NH3 volatilization occurred in pile top zone, which has very high NH4+ concentrations and significantly high 15N (δ15N: 12.7–29.8 ‰) values.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
Short summary
Short summary
We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
Short summary
Short summary
The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
S. Song, N. E. Selin, A. L. Soerensen, H. Angot, R. Artz, S. Brooks, E.-G. Brunke, G. Conley, A. Dommergue, R. Ebinghaus, T. M. Holsen, D. A. Jaffe, S. Kang, P. Kelley, W. T. Luke, O. Magand, K. Marumoto, K. A. Pfaffhuber, X. Ren, G.-R. Sheu, F. Slemr, T. Warneke, A. Weigelt, P. Weiss-Penzias, D. C. Wip, and Q. Zhang
Atmos. Chem. Phys., 15, 7103–7125, https://doi.org/10.5194/acp-15-7103-2015, https://doi.org/10.5194/acp-15-7103-2015, 2015
Short summary
Short summary
A better knowledge of mercury (Hg) emission fluxes into the global atmosphere is important for assessing its human health impacts and evaluating the effectiveness of corresponding policy actions. We for the first time apply a top-down approach at a global scale to quantitatively estimate present-day mercury emission sources as well as key parameters in a chemical transport model, in order to better constrain the global biogeochemical cycle of mercury.
S. Kang, F. Wang, U. Morgenstern, Y. Zhang, B. Grigholm, S. Kaspari, M. Schwikowski, J. Ren, T. Yao, D. Qin, and P. A. Mayewski
The Cryosphere, 9, 1213–1222, https://doi.org/10.5194/tc-9-1213-2015, https://doi.org/10.5194/tc-9-1213-2015, 2015
Short summary
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
Short summary
Short summary
Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
N. Zhang, K. Yamada, N. Suzuki, and N. Yoshida
Biogeosciences, 11, 5335–5348, https://doi.org/10.5194/bg-11-5335-2014, https://doi.org/10.5194/bg-11-5335-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
T. Yamazaki, T. Hozuki, K. Arai, S. Toyoda, K. Koba, T. Fujiwara, and N. Yoshida
Biogeosciences, 11, 2679–2689, https://doi.org/10.5194/bg-11-2679-2014, https://doi.org/10.5194/bg-11-2679-2014, 2014
T. O. Sato, H. Sagawa, N. Yoshida, and Y. Kasai
Atmos. Meas. Tech., 7, 941–958, https://doi.org/10.5194/amt-7-941-2014, https://doi.org/10.5194/amt-7-941-2014, 2014
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
J. A. Schmidt, M. S. Johnson, S. Hattori, N. Yoshida, S. Nanbu, and R. Schinke
Atmos. Chem. Phys., 13, 1511–1520, https://doi.org/10.5194/acp-13-1511-2013, https://doi.org/10.5194/acp-13-1511-2013, 2013
Related subject area
Subject: Isotopes | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
A seasonal analysis of aerosol NO3− sources and NOx oxidation pathways in the Southern Ocean marine boundary layer
Nitrate chemistry in the northeast US – Part 1: Nitrogen isotope seasonality tracks nitrate formation chemistry
Nitrate chemistry in the northeast US – Part 2: Oxygen isotopes reveal differences in particulate and gas-phase formation
Photolytic modification of seasonal nitrate isotope cycles in East Antarctica
Atmospheric methane isotopes identify inventory knowledge gaps in the Surat Basin, Australia, coal seam gas and agricultural regions
Methane (CH4) sources in Krakow, Poland: insights from isotope analysis
Isotopic signatures of major methane sources in the coal seam gas fields and adjacent agricultural districts, Queensland, Australia
Measurement report: Nitrogen isotopes (δ15N) and first quantification of oxygen isotope anomalies (Δ17O, δ18O) in atmospheric nitrogen dioxide
Measurement report: Spatial variability of northern Iberian rainfall stable isotope values – investigating atmospheric controls on daily and monthly timescales
Baffin Bay sea ice extent and synoptic moisture transport drive water vapor isotope (δ18O, δ2H, and deuterium excess) variability in coastal northwest Greenland
New evidence for atmospheric mercury transformations in the marine boundary layer from stable mercury isotopes
The isotopic composition of atmospheric nitrous oxide observed at the high-altitude research station Jungfraujoch, Switzerland
Deposition, recycling, and archival of nitrate stable isotopes between the air–snow interface: comparison between Dronning Maud Land and Dome C, Antarctica
Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33S reservoir of sulfate aerosols?
Atmospheric radiocarbon measurements to quantify CO2 emissions in the UK from 2014 to 2015
An improved estimate for the δ13C and δ18O signatures of carbon monoxide produced from atmospheric oxidation of volatile organic compounds
Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2
The Δ17O and δ18O values of atmospheric nitrates simultaneously collected downwind of anthropogenic sources – implications for polluted air masses
A very limited role of tropospheric chlorine as a sink of the greenhouse gas methane
Detection and variability of combustion-derived vapor in an urban basin
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region
Triple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric deposition
Isotopic constraints on heterogeneous sulfate production in Beijing haze
Estimation of the fossil fuel component in atmospheric CO2 based on radiocarbon measurements at the Beromünster tall tower, Switzerland
Constraining N2O emissions since 1940 using firn air isotope measurements in both hemispheres
Seasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica
Carbon isotopic signature of coal-derived methane emissions to the atmosphere: from coalification to alteration
Isotopic composition for source identification of mercury in atmospheric fine particles
Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer
In situ observations of the isotopic composition of methane at the Cabauw tall tower site
Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign
Isotopic effects of nitrate photochemistry in snow: a field study at Dome C, Antarctica
Stable carbon isotope ratios of ambient secondary organic aerosols in Toronto
WAIS Divide ice core suggests sustained changes in the atmospheric formation pathways of sulfate and nitrate since the 19th century in the extratropical Southern Hemisphere
Stable carbon isotope ratios of toluene in the boundary layer and the lower free troposphere
Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning
Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?
Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summer
Chemical characterization and stable carbon isotopic composition of particulate Polycyclic Aromatic Hydrocarbons issued from combustion of 10 Mediterranean woods
Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis
Temporal and spatial variability of the stable isotopic composition of atmospheric molecular hydrogen: observations at six EUROHYDROS stations
Continuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution events
Anthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern China
Analysis of 13C and 18O isotope data of CO2 in CARIBIC aircraft samples as tracers of upper troposphere/lower stratosphere mixing and the global carbon cycle
Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17O
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
Sources and transport of Δ14C in CO2 within the Mexico City Basin and vicinity
Jessica M. Burger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 23, 5605–5622, https://doi.org/10.5194/acp-23-5605-2023, https://doi.org/10.5194/acp-23-5605-2023, 2023
Short summary
Short summary
A seasonal analysis of the nitrogen isotopes of atmospheric nitrate over the remote Southern Ocean reveals that similar natural NOx sources dominate in spring and summer, while winter is representative of background-level conditions. The oxygen isotopes suggest that similar oxidation pathways involving more ozone occur in spring and winter, while the hydroxyl radical is the main oxidant in summer. This work helps to constrain NOx cycling and oxidant budgets in a data-sparse remote marine region.
Claire Bekker, Wendell W. Walters, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4185–4201, https://doi.org/10.5194/acp-23-4185-2023, https://doi.org/10.5194/acp-23-4185-2023, 2023
Short summary
Short summary
Nitrate is a critical component of the atmosphere that degrades air quality and ecosystem health. We have investigated the nitrogen isotope compositions of nitrate from deposition samples collected across the northeastern United States. Spatiotemporal variability in the nitrogen isotope compositions was found to track with nitrate formation chemistry. Our results highlight that nitrogen isotope compositions may be a robust tool for improving model representation of nitrate chemistry.
Heejeong Kim, Wendell W. Walters, Claire Bekker, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
Short summary
Short summary
Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
Pete D. Akers, Joël Savarino, Nicolas Caillon, Olivier Magand, and Emmanuel Le Meur
Atmos. Chem. Phys., 22, 15637–15657, https://doi.org/10.5194/acp-22-15637-2022, https://doi.org/10.5194/acp-22-15637-2022, 2022
Short summary
Short summary
Nitrate isotopes in Antarctic ice do not preserve the seasonal isotopic cycles of the atmosphere, which limits their use to study the past. We studied nitrate along an 850 km Antarctic transect to learn how these cycles are changed by sunlight-driven chemistry in the snow. Our findings suggest that the snow accumulation rate and other environmental signals can be extracted from nitrate with the right sampling and analytical approaches.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
Short summary
Short summary
This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
Short summary
Short summary
Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
Short summary
Short summary
Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497, https://doi.org/10.5194/acp-21-10477-2021, https://doi.org/10.5194/acp-21-10477-2021, 2021
Short summary
Short summary
We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Ana Moreno, Miguel Iglesias, Cesar Azorin-Molina, Carlos Pérez-Mejías, Miguel Bartolomé, Carlos Sancho, Heather Stoll, Isabel Cacho, Jaime Frigola, Cinta Osácar, Arsenio Muñoz, Antonio Delgado-Huertas, Ileana Bladé, and Françoise Vimeux
Atmos. Chem. Phys., 21, 10159–10177, https://doi.org/10.5194/acp-21-10159-2021, https://doi.org/10.5194/acp-21-10159-2021, 2021
Short summary
Short summary
We present a large and unique dataset of the rainfall isotopic composition at seven sites from northern Iberia to characterize their variability at daily and monthly timescales and to assess the role of climate and geographic factors in the modulation of δ18O values. We found that the origin, moisture uptake along the trajectory and type of precipitation play a key role. These results will help to improve the interpretation of δ18O paleorecords from lacustrine carbonates or speleothems.
Pete D. Akers, Ben G. Kopec, Kyle S. Mattingly, Eric S. Klein, Douglas Causey, and Jeffrey M. Welker
Atmos. Chem. Phys., 20, 13929–13955, https://doi.org/10.5194/acp-20-13929-2020, https://doi.org/10.5194/acp-20-13929-2020, 2020
Short summary
Short summary
Water vapor isotopes recorded for 2 years in coastal northern Greenland largely reflect changes in sea ice cover, with distinct values when Baffin Bay is ice covered in winter vs. open in summer. Resulting changes in moisture transport, surface winds, and air temperature also modify the isotopes. Local glacial ice may thus preserve past changes in the Baffin Bay sea ice extent, and this will help us better understand how the Arctic environment and water cycle responds to global climate change.
Ben Yu, Lin Yang, Linlin Wang, Hongwei Liu, Cailing Xiao, Yong Liang, Qian Liu, Yongguang Yin, Ligang Hu, Jianbo Shi, and Guibin Jiang
Atmos. Chem. Phys., 20, 9713–9723, https://doi.org/10.5194/acp-20-9713-2020, https://doi.org/10.5194/acp-20-9713-2020, 2020
Short summary
Short summary
We found that Br atoms in the marine boundary layer are the most probable oxidizer that transform gaseous elemental mercury into gaseous oxidized mercury, according to the mercury isotopes in the total gaseous mercury. On the other hand, Br or Cl atoms are not the primary oxidizers that produced oxidized mercury on particles. This study showed that mercury isotopes can provide new evidence that help us to fully understand the transformations of atmospheric mercury.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
Short summary
Short summary
We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
Short summary
Short summary
The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Isabelle Genot, David Au Yang, Erwan Martin, Pierre Cartigny, Erwann Legendre, and Marc De Rafelis
Atmos. Chem. Phys., 20, 4255–4273, https://doi.org/10.5194/acp-20-4255-2020, https://doi.org/10.5194/acp-20-4255-2020, 2020
Short summary
Short summary
Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using their isotope signatures (δ34S, ∆33S, ∆36S, δ18O, and ∆17O). A striking observation is that ∆33S > 0 ‰, implying a missing reservoir in the sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crust sulfates (i.e., formed on carbonate walls) that must therefore result from distinct chemical pathway(s) compared to sulfate aerosols, and they may well represent this complementary reservoir.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070, https://doi.org/10.5194/acp-19-14057-2019, https://doi.org/10.5194/acp-19-14057-2019, 2019
Short summary
Short summary
We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
Short summary
Short summary
Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
David Au Yang, Pierre Cartigny, Karine Desboeufs, and David Widory
Atmos. Chem. Phys., 19, 3779–3796, https://doi.org/10.5194/acp-19-3779-2019, https://doi.org/10.5194/acp-19-3779-2019, 2019
Short summary
Short summary
Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays, which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two other possible oxidation pathways.
Martine M. Savard, Amanda S. Cole, Robert Vet, and Anna Smirnoff
Atmos. Chem. Phys., 18, 10373–10389, https://doi.org/10.5194/acp-18-10373-2018, https://doi.org/10.5194/acp-18-10373-2018, 2018
Short summary
Short summary
Improving air quality requires understanding of the atmospheric processes transforming nitrous oxides emitted by human activities into nitrates, an N form that may degrade natural ecosystems. Isotopes (∆17O, δ18O) are characterized in separate wet, particulate and gaseous nitrates for the first time. The gas ranges are distinct from those of the other nitrates, and the plume dynamics emerge as crucial in interpreting the results, which unravel key processes behind the distribution of nitrates.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, https://doi.org/10.5194/acp-18-9831-2018, 2018
Short summary
Short summary
Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
Richard P. Fiorella, Ryan Bares, John C. Lin, James R. Ehleringer, and Gabriel J. Bowen
Atmos. Chem. Phys., 18, 8529–8547, https://doi.org/10.5194/acp-18-8529-2018, https://doi.org/10.5194/acp-18-8529-2018, 2018
Short summary
Short summary
Fossil fuel combustion produces water; where fossil fuel combustion is concentrated in urban areas, this humidity source may represent ~ 10 % of total humidity. In turn, this water vapor addition may alter urban meteorology, though the contribution of combustion vapor is difficult to measure. Using stable water isotopes, we estimate that up to 16 % of urban humidity may arise from combustion when the atmosphere is stable during winter, and develop recommendations for application in other cities.
Neda Amiri, Roya Ghahreman, Ofelia Rempillo, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, and Ann-Lise Norman
Atmos. Chem. Phys., 18, 7757–7780, https://doi.org/10.5194/acp-18-7757-2018, https://doi.org/10.5194/acp-18-7757-2018, 2018
David M. Nelson, Urumu Tsunogai, Dong Ding, Takuya Ohyama, Daisuke D. Komatsu, Fumiko Nakagawa, Izumi Noguchi, and Takashi Yamaguchi
Atmos. Chem. Phys., 18, 6381–6392, https://doi.org/10.5194/acp-18-6381-2018, https://doi.org/10.5194/acp-18-6381-2018, 2018
Short summary
Short summary
Atmospheric nitrate may be produced locally and/or come from upwind regions. To address this issue we measured oxygen and nitrogen isotopes of wet and dry nitrate deposition at nearby urban and rural sites. Our results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments results from local NOx emissions more so than wet deposition, which is transported longer distances.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
Short summary
Short summary
We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766, https://doi.org/10.5194/acp-17-10753-2017, https://doi.org/10.5194/acp-17-10753-2017, 2017
Short summary
Short summary
Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
Short summary
Short summary
Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
Short summary
Short summary
We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680, https://doi.org/10.5194/acp-16-13669-2016, https://doi.org/10.5194/acp-16-13669-2016, 2016
Short summary
Short summary
Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Qiang Huang, Jiubin Chen, Weilin Huang, Pingqing Fu, Benjamin Guinot, Xinbin Feng, Lihai Shang, Zhuhong Wang, Zhongwei Wang, Shengliu Yuan, Hongming Cai, Lianfang Wei, and Ben Yu
Atmos. Chem. Phys., 16, 11773–11786, https://doi.org/10.5194/acp-16-11773-2016, https://doi.org/10.5194/acp-16-11773-2016, 2016
Short summary
Short summary
Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its vectors might have adverse effects on human beings. In this study, we attempted to identify the sources of PM2.5-Hg in Beijing, China, using Hg isotopic composition. Large range and seasonal variations in both mass-dependent and mass-independent fractionations of Hg isotopes in haze particles demonstrate the usefulness of Hg isotopes for directly tracing the sources and its vectors in the atmosphere.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
Short summary
Short summary
The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
Short summary
Short summary
A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673, https://doi.org/10.5194/acp-16-2659-2016, https://doi.org/10.5194/acp-16-2659-2016, 2016
Short summary
Short summary
Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
Short summary
Short summary
In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. Saccon, A. Kornilova, L. Huang, S. Moukhtar, and J. Rudolph
Atmos. Chem. Phys., 15, 10825–10838, https://doi.org/10.5194/acp-15-10825-2015, https://doi.org/10.5194/acp-15-10825-2015, 2015
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
J. Wintel, E. Hösen, R. Koppmann, M. Krebsbach, A. Hofzumahaus, and F. Rohrer
Atmos. Chem. Phys., 13, 11059–11071, https://doi.org/10.5194/acp-13-11059-2013, https://doi.org/10.5194/acp-13-11059-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
C. J. Sapart, P. Martinerie, E. Witrant, J. Chappellaz, R. S. W. van de Wal, P. Sperlich, C. van der Veen, S. Bernard, W. T. Sturges, T. Blunier, J. Schwander, D. Etheridge, and T. Röckmann
Atmos. Chem. Phys., 13, 6993–7005, https://doi.org/10.5194/acp-13-6993-2013, https://doi.org/10.5194/acp-13-6993-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
A. Guillon, K. Le Ménach, P.-M. Flaud, N. Marchand, H. Budzinski, and E. Villenave
Atmos. Chem. Phys., 13, 2703–2719, https://doi.org/10.5194/acp-13-2703-2013, https://doi.org/10.5194/acp-13-2703-2013, 2013
D. Ceburnis, A. Garbaras, S. Szidat, M. Rinaldi, S. Fahrni, N. Perron, L. Wacker, S. Leinert, V. Remeikis, M. C. Facchini, A. S. H. Prevot, S. G. Jennings, M. Ramonet, and C. D. O'Dowd
Atmos. Chem. Phys., 11, 8593–8606, https://doi.org/10.5194/acp-11-8593-2011, https://doi.org/10.5194/acp-11-8593-2011, 2011
A. M. Batenburg, S. Walter, G. Pieterse, I. Levin, M. Schmidt, A. Jordan, S. Hammer, C. Yver, and T. Röckmann
Atmos. Chem. Phys., 11, 6985–6999, https://doi.org/10.5194/acp-11-6985-2011, https://doi.org/10.5194/acp-11-6985-2011, 2011
B. Tuzson, S. Henne, D. Brunner, M. Steinbacher, J. Mohn, B. Buchmann, and L. Emmenegger
Atmos. Chem. Phys., 11, 1685–1696, https://doi.org/10.5194/acp-11-1685-2011, https://doi.org/10.5194/acp-11-1685-2011, 2011
Y. T. Fang, K. Koba, X. M. Wang, D. Z. Wen, J. Li, Y. Takebayashi, X. Y. Liu, and M. Yoh
Atmos. Chem. Phys., 11, 1313–1325, https://doi.org/10.5194/acp-11-1313-2011, https://doi.org/10.5194/acp-11-1313-2011, 2011
S. S. Assonov, C. A. M. Brenninkmeijer, T. J. Schuck, and P. Taylor
Atmos. Chem. Phys., 10, 8575–8599, https://doi.org/10.5194/acp-10-8575-2010, https://doi.org/10.5194/acp-10-8575-2010, 2010
U. Tsunogai, D. D. Komatsu, S. Daita, G. A. Kazemi, F. Nakagawa, I. Noguchi, and J. Zhang
Atmos. Chem. Phys., 10, 1809–1820, https://doi.org/10.5194/acp-10-1809-2010, https://doi.org/10.5194/acp-10-1809-2010, 2010
M. M. Frey, J. Savarino, S. Morin, J. Erbland, and J. M. F. Martins
Atmos. Chem. Phys., 9, 8681–8696, https://doi.org/10.5194/acp-9-8681-2009, https://doi.org/10.5194/acp-9-8681-2009, 2009
S. A. Vay, S. C. Tyler, Y. Choi, D. R. Blake, N. J. Blake, G. W. Sachse, G. S. Diskin, and H. B. Singh
Atmos. Chem. Phys., 9, 4973–4985, https://doi.org/10.5194/acp-9-4973-2009, https://doi.org/10.5194/acp-9-4973-2009, 2009
Cited articles
Alexander, B., Savarino, J., Barkov, N., Delmas, R., and Thiemens, M.: Climate driven changes in the oxidation pathways of atmospheric sulfur, Geophys. Res. Lett., 29, 1685, https://doi.org/10.1029/2002GL014879, 2002.
Alexander, B., Park, R. J., Jacob, D. J., Li, Q., Yantosca, R. M., Savarino, J., Lee, C., and Thiemens, M.: Sulfate formation in sea-salt aerosols: Constraints from oxygen isotopes, J. Geophys. Res.-Atmos., 110, D10307, https://doi.org/10.1029/2004JD005659, 2005.
Alexander, B., Park, R. J., Jacob, D. J., and Gong, S.: Transition metal-catalyzed oxidation of atmospheric sulfur: Global implications for the sulfur budget, J. Geophys. Res., 114, D02309, https://doi.org/10.1029/2008JD010486, 2009.
Alexander, B., Allman, D., Amos, H., Fairlie, T., Dachs, J., Hegg, D. A., and Sletten, R. S.: Isotopic constraints on the formation pathways of sulfate aerosol in the marine boundary layer of the subtropical northeast Atlantic Ocean, J. Geophys. Res.-Atmos., 117, D06304, https://doi.org/10.1029/2011JD016773, 2012.
Banzhaf, S., Schaap, M., Kerschbaumer, A., Reimer, E., Stern, R., Van Der Swaluw, E., and Builtjes, P.: Implementation and evaluation of pH-dependent cloud chemistry and wet deposition in the chemical transport model REM-Calgrid, Atmos. Environ., 49, 378–390, https://doi.org/10.1016/j.atmosenv.2011.10.069, 2012.
Bao, H., Campbell, D. A., Bockheim, J. G., and Thiemens, M. H.: Origins of sulphate in Antarctic dry-valley soils as deduced from anomalous 17O compositions, Nature, 407, 499–502, https://doi.org/10.1038/35035054, 2000a.
Bao, H., Thiemens, M. H., Farquhar, J., Campbell, D. A., Lee, C. C.-W., Heine, K., and Loope, D. B.: Anomalous 17O compositions in massive sulphate deposits on the Earth, Nature, 406, 176–178, https://doi.org/10.1038/35018052, 2000b.
Bao, H., Michalski, G. M., and Thiemens, M. H.: Sulfate oxygen-17 anomalies in desert varnishes, Geochim. Cosmochim. Ac., 65, 2029–2036, https://doi.org/10.1016/S0016-7037(00)00490-7, 2001.
Bao, H. and Reheis, M. C.: Multiple oxygen and sulfur isotopic analyses on water-soluble sulfate in bulk atmospheric deposition from the southwestern United States, J. Geophys. Res.-Atmos., 108, 4430, https://doi.org/10.1029/2002JD003022, 2003.
Bauer, S. E. and Koch, D.: Impact of heterogeneous sulfate formation at mineral dust surfaces on aerosol loads and radiative forcing in the Goddard Institute for Space Studies general circulation model, J. Geophys. Res.-Atmos., 110, D17202, https://doi.org/10.1029/2005jd005870, 2005.
Berresheim, H., Wine, P., and Davis, D.: Sulfur in the atmosphere, in: Composition, chemistry, and climate of the atmosphere, edited by: Singh, H. B., Van Nostrand Reinhold, New York, 251–307, 1995.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res.-Atmos., 106, 23073–23095, https://doi.org/10.1029/2001jd000807, 2001.
Calvert, J. G., Lazrus, A., Kok, G. L., Heikes, B. G., Walega, J. G., Lind, J., and Cantrell, C. A.: Chemical mechanisms of acid generation in the troposphere, Nature, 317, 27–35, https://doi.org/10.1038/317027a0, 1985.
Cerqueira, M., Pio, C., Legrand, M., Puxbaum, H., Kasper-Giebl, A., Afonso, J., Preunkert, S., Gelencsér, A., and Fialho, P.: Particulate carbon in precipitation at European background sites, J. Aerosol Sci., 41, 51–61, https://doi.org/10.1016/j.jaerosci.2009.08.002, 2010.
Chang, J., Brost, R., Isaksen, I., Madronich, S., Middleton, P., Stockwell, W., and Walcek, C.: A three-dimensional Eulerian acid deposition model: Physical concepts and formulation, J. Geophys. Res.-Atmos., 92, 14681–14700, https://doi.org/10.1029/jd092id12p14681, 1987.
Charlson, R. J., Schwartz, S., Hales, J., Cess, R. D., Coakley, J. J., Hansen, J., and Hofmann, D.: Climate forcing by anthropogenic aerosols, Science, 255, 423–430, https://doi.org/10.1126/science.255.5043.423, 1992.
Chen, Q., Geng, L., Schmidt, J. A., Xie, Z., Kang, H., Dachs, J., Cole-Dai, J., Schauer, A. J., Camp, M. G., and Alexander, B.: Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer, Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, 2016.
Chen, Q., Schmidt, J. A., Shah, V., Jaeglé, L., Sherwen, T., and Alexander, B.: Sulfate production by reactive bromine: Implications for the global sulfur and reactive bromine budgets, Geophys. Res. Lett., 44, 7069–7078, https://doi.org/10.1002/2017gl073812, 2017.
Chen, X., Kang, S., Cong, Z., Yang, J., and Ma, Y.: Concentration, temporal variation, and sources of black carbon in the Mt. Everest region retrieved by real-time observation and simulation, Atmos. Chem. Phys., 18, 12859–12875, https://doi.org/10.5194/acp-18-12859-2018, 2018.
Chin, M., Jacob, D. J., Gardner, G. M., Foreman-Fowler, M. S., Spiro, P. A., and Savoie, D. L.: A global three-dimensional model of tropospheric sulfate, J. Geophys. Res.-Atmos., 101, 18667–18690, https://doi.org/10.1029/96jd01221, 1996.
Cong, Z., Kang, S., Kawamura, K., Liu, B., Wan, X., Wang, Z., Gao, S., and Fu, P.: Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources, Atmos. Chem. Phys., 15, 1573–1584, https://doi.org/10.5194/acp-15-1573-2015, 2015a.
Cong, Z., Kawamura, K., Kang, S., and Fu, P.: Penetration of biomass-burning emissions from South Asia through the Himalayas: new insights from atmospheric organic acids, Sci. Rep., 5, 9580, https://doi.org/10.1038/srep09580, 2015b.
Cristofanelli, P., Bracci, A., Sprenger, M., Marinoni, A., Bonafè, U., Calzolari, F., Duchi, R., Laj, P., Pichon, J. M., Roccato, F., Venzac, H., Vuillermoz, E., and Bonasoni, P.: Tropospheric ozone variations at the Nepal Climate Observatory-Pyramid (Himalayas, 5079 m a.s.l.) and influence of deep stratospheric intrusion events, Atmos. Chem. Phys., 10, 6537–6549, https://doi.org/10.5194/acp-10-6537-2010, 2010.
Dee, D. P., Uppala, S. M., Simmons, A., Berrisford, P., Poli, P., Kobayashi, S., Andrae, U., Balmaseda, M., Balsamo, G., and Bauer, D. P.: The ERA-Interim reanalysis: Configuration and performance of the data assimilation system, Q. J. Roy. Meteor. Soc., 137, 553–597, https://doi.org/10.1002/qj.828, 2011.
Dentener, F., Williams, J., and Metzger, S.: Aqueous phase reaction of HNO4: The impact on tropospheric chemistry, J. Atmos. Chem., 41, 109–133, https://doi.org/10.1023/A:1014233910126, 2002.
Dominguez, G., Jackson, T., Brothers, L., Barnett, B., Nguyen, B., and Thiemens, M. H.: Discovery and measurement of an isotopically distinct source of sulfate in Earth's atmosphere, Proc. Natl. Acad. Sci. USA., 105, 12769–12773, https://doi.org/10.1073/pnas.0805255105, 2008.
Duan, J., Esper, J., Buntgen, U., Li, L., Xoplaki, E., Zhang, H., Wang, L., Fang, Y., and Luterbacher, J.: Weakening of annual temperature cycle over the Tibetan Plateau since the 1870s, Nat. Commun., 8, 14008–14008, https://doi.org/10.1038/ncomms14008, 2017.
Fairlie, T. D., Jacob, D. J., and Park, R. J.: The impact of transpacific transport of mineral dust in the United States, Atmos. Environ., 41, 1251–1266, https://doi.org/10.1016/j.atmosenv.2006.09.048, 2007.
Fairlie, T. D., Jacob, D. J., Dibb, J. E., Alexander, B., Avery, M. A., van Donkelaar, A., and Zhang, L.: Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes, Atmos. Chem. Phys., 10, 3999–4012, https://doi.org/10.5194/acp-10-3999-2010, 2010.
Feingold, G., Frost, G. J., and Ravishankara, A.: Role of NO3 in sulfate production in the wintertime northern latitudes, J. Geophys. Res.-Atmos., 107, 4640, https://doi.org/10.1029/2002jd002288, 2002.
Gautier, E., Savarino, J., Hoek, J., Erbland, J., Caillon, N., Hattori, S., Yoshida, N., Albalat, E., Albarede, F., and Farquhar, J.: 2600 years of stratospheric volcanism through sulfate isotopes, Nat. Commun., 10, 1–7, https://doi.org/10.1038/s41467-019-08357-0, 2019.
Geng, L., Schauer, A. J., Kunasek, S. A., Sofen, E. D., Erbland, J., Savarino, J., Allman, D. J., Sletten, R. S., and Alexander, B.: Analysis of oxygen-17 excess of nitrate and sulfate at sub-micromole levels using the pyrolysis method, Rapid Commun. Mass Sp., 27, 2411–2419, https://doi.org/10.1002/rcm.6703, 2013.
Goto-Azuma, K., Hirabayashi, M., Motoyama, H., Miyake, T., Kuramoto, T., Uemura, R., Igarashi, M., Iizuka, Y., Sakurai, T., and Horikawa, S.: Reduced marine phytoplankton sulphur emissions in the Southern Ocean during the past seven glacials, Nat. Commun., 10, 1–7, https://doi.org/10.1038/s41467-019-11128-6, 2019.
Guha, T., Lin, C., Bhattacharya, S., Mahajan, A., Ou Yang, C., Lan, Y., Hsu, S., and Liang, M.: Isotopic ratios of nitrate in aerosol samples from Mt. Lulin, a high-altitude station in Central Taiwan, Atmos. Environ., 154, 53–69, https://doi.org/10.1016/j.atmosenv.2017.01.036, 2017.
Harris, E., Sinha, B., Van Pinxteren, D., Tilgner, A., Fomba, K. W., Schneider, J., Roth, A., Gnauk, T., Fahlbusch, B., and Mertes, S.: Enhanced role of transition metal ion catalysis during in-cloud oxidation of SO2, Science, 340, 727–730, https://doi.org/10.1126/science.1230911, 2013.
Hattori, S., Iizuka, Y., Alexander, B., Ishino, S., Fujita, K., Zhai, S., Sherwen, T., Oshima, N., Uemura, R., Yamada, A., Suzuki, N., Matoba, S., Tsuruta, A., Savarino, J., and Yoshida, N.: Isotopic evidence for acidity-driven enhancement of sulfate formation after SO2 emission control, Sci. Adv., 7, eabd4610, https://doi.org/10.1126/sciadv.abd4610, 2021.
He, P., Alexander, B., Geng, L., Chi, X., Fan, S., Zhan, H., Kang, H., Zheng, G., Cheng, Y., Su, H., Liu, C., and Xie, Z.: Isotopic constraints on heterogeneous sulfate production in Beijing haze, Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, 2018.
Hill-Falkenthal, J., Priyadarshi, A., Savarino, J., and Thiemens, M.: Seasonal variations in 35S and Δ17O of sulfate aerosols on the Antarctic plateau, J. Geophys. Res.-Atmos., 118, 9444–9455, https://doi.org/10.1002/jgrd.50716, 2013.
Hoesly, R. M., Smith, S. J., Feng, L., Klimont, Z., Janssens-Maenhout, G., Pitkanen, T., Seibert, J. J., Vu, L., Andres, R. J., Bolt, R. M., Bond, T. C., Dawidowski, L., Kholod, N., Kurokawa, J.-I., Li, M., Liu, L., Lu, Z., Moura, M. C. P., O'Rourke, P. R., and Zhang, Q.: Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS), Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, 2018.
Holt, B., Kumar, R., and Cunningham, P.: Oxygen-18 study of the aqueous-phase oxidation of sulfur dioxide, Atmos. Environ., 15, 557–566, https://doi.org/10.1016/0004-6981(81)90186-4, 1981.
Immerzeel, W. W., Van Beek, L. P., and Bierkens, M. F.: Climate change will affect the Asian water towers, Science, 328, 1382–1385, https://doi.org/10.1126/science.1183188, 2010.
Ishino, S., Hattori, S., Savarino, J., Jourdain, B., Preunkert, S., Legrand, M., Caillon, N., Barbero, A., Kuribayashi, K., and Yoshida, N.: Seasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica, Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, 2017.
Ishino, S., Hattori, S., Legrand, M., Chen, Q., Alexander, B., Shao, J., Huang, J., Jaegle, L., Jourdain, B., and Preunkert, S.: Regional characteristics of atmospheric sulfate formation in East Antarctica imprinted on 17O-excess signature, J. Geophys. Res.-Atmos., 126, e2020JD033583, https://doi.org/10.1029/2020JD033583, 2021.
Jenkins, K. A. and Bao, H.: Multiple oxygen and sulfur isotope compositions of atmospheric sulfate in Baton Rouge, LA, USA, Atmos. Environ., 40, 4528–4537, https://doi.org/10.1016/j.atmosenv.2006.04.010, 2006.
Kang, S., Wake, C. P., Qin, D., Mayewski, P. A., and Yao, T.: Monsoon and dust signals recorded in Dasuopu glacier, Tibetan Plateau, J. Glaciol., 46, 222–226, https://doi.org/10.3189/172756500781832864, 2000.
Kang, S., Qin, D., Mayewski, P. A., Sneed, S. B., and Yao, T.: Chemical composition of fresh snow on Xixabangma peak, central Himalaya, during the summer monsoon season, J. Glaciol., 48, 337–339, https://doi.org/10.3189/172756502781831467, 2002.
Kang, S., You, Q., Flügel, W. A., Pepin, N., and Yao, T.: Review of climate and cryospheric change in the Tibetan Plateau, Environ. Res. Lett., 5, 015101, https://doi.org/10.1088/1748-9326/5/1/015101, 2010.
Kang, S., Zhang, Q., Qian, Y., Ji, Z., Li, C., Cong, Z., Zhang, Y., Guo, J., Du, W., and Huang, J.: Linking Atmospheric Pollution to Cryospheric Change in the Third Pole Region: Current Progresses and Future Prospects, Natl. Sci. Rev., 6, 796–809, https://doi.org/10.1093/nsr/nwz031, 2019.
Kang, S., Zhang, Y., Qian, Y., and Wang, H.: A review of black carbon in snow and ice and its impact on the cryosphere, Earth Sci. Rev., 210, 103346, https://doi.org/10.1016/j.earscirev.2020.103346, 2020.
Kaufman, Y. J. and Tanre, D.: Effect of variations in super-saturation on the formation of cloud condensation nuclei, Nature, 369, 45–48, https://doi.org/10.1038/369045a0, 1994.
Kaufmann, P., Fundel, F., Fischer, H., Bigler, M., Ruth, U., Udisti, R., Hansson, M., De Angelis, M., Barbante, C., and Wolff, E. W.: Ammonium and non-sea salt sulfate in the EPICA ice cores as indicator of biological activity in the Southern Ocean, Quaternary Sci. Rev., 29, 313–323, https://doi.org/10.1016/j.quascirev.2009.11.009, 2010.
Koch, D., Jacob, D., Tegen, I., Rind, D., and Chin, M.: Tropospheric sulfur simulation and sulfate direct radiative forcing in the Goddard Institute for Space Studies general circulation model, J. Geophys. Res.-Atmos., 104, 23799–23822, https://doi.org/10.1029/1999jd900248, 1999.
Krankowsky, D., Lämmerzahl, P., and Mauersberger, K.: Isotopic measurements of stratospheric ozone, Geophys. Res. Lett., 27, 2593–2595, https://doi.org/10.1029/2000gl011812, 2000.
Kulmala, M., Pirjola, L., and Mäkelä, J. M.: Stable sulphate clusters as a source of new atmospheric particles, Nature, 404, 66–69, https://doi.org/10.1038/35003550, 2000.
Kunasek, S., Alexander, B., Steig, E., Sofen, E., Jackson, T., Thiemens, M., McConnell, J., Gleason, D., and Amos, H.: Sulfate sources and oxidation chemistry over the past 230 years from sulfur and oxygen isotopes of sulfate in a West Antarctic ice core, J. Geophys. Res.-Atmos., 115, D18313, https://doi.org/10.1029/2010jd013846, 2010.
Lee, C. W. and Thiemens, M. H.: The δ17O and δ18O measurements of atmospheric sulfate from a coastal and high alpine region: A mass-independent isotopic anomaly, J. Geophys. Res.-Atmos., 106, 17359–17374, https://doi.org/10.1029/2000jd900805, 2001.
Lee, Y. and Schwartz, S. E.: Kinetics of oxidation of aqueous sulfur (IV) by nitrogen dioxide, in: Precipitation Scavenging, Dry Deposition and Resuspension, edited by: Pruppacher, H. R., Semonin, R. G., and Slinn, W. G. N., Elsevier, New York, 453–470, 1983.
Li, C., Bosch, C., Kang, S., Andersson, A., Chen, P., Zhang, Q., Cong, Z., Chen, B., Qin, D., and Gustafsson, Ö.: Sources of black carbon to the Himalayan-Tibetan Plateau glaciers, Nat. Commun., 7, 1–7, https://doi.org/10.1038/ncomms12574, 2016.
Li, L., Chen, Z. M., Zhang, Y. H., Zhu, T., Li, J. L., and Ding, J.: Kinetics and mechanism of heterogeneous oxidation of sulfur dioxide by ozone on surface of calcium carbonate, Atmos. Chem. Phys., 6, 2453–2464, https://doi.org/10.5194/acp-6-2453-2006, 2006.
Li, X., Bao, H., Gan, Y., Zhou, A., and Liu, Y.: Multiple oxygen and sulfur isotope compositions of secondary atmospheric sulfate in a mega-city in central China, Atmos. Environ., 81, 591–599, https://doi.org/10.1016/j.atmosenv.2013.09.051, 2013.
Liang, J. and Jacobson, M. Z.: A study of sulfur dioxide oxidation pathways over a range of liquid water contents, pH values, and temperatures, J. Geophys. Res.-Atmos., 104, 13749–13769, https://doi.org/10.1029/1999jd900097, 1999.
Lim, S., Lee, M., Kim, S.-W., and Laj, P.: Sulfate alters aerosol absorption properties in East Asian outflow, Sci. Rep., 8, 1–7, https://doi.org/10.1038/s41598-018-23021-1, 2018.
Lin, M., Zhang, Z., Su, L., Hill-Falkenthal, J., Priyadarshi, A., Zhang, Q., Zhang, G., Kang, S., Chan, C. Y., and Thiemens, M. H.: Resolving the impact of stratosphere-to-troposphere transport on the sulfur cycle and surface ozone over the Tibetan Plateau using a cosmogenic 35S tracer, J. Geophys. Res.-Atmos., 121, 439–456, https://doi.org/10.1002/2015jd023801, 2016.
Lin, M., Biglari, S., Zhang, Z., Crocker, D., Tao, J., Su, B., Liu, L., and Thiemens, M. H.: Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes, Geophys. Res. Lett., 44, 5187–5196, https://doi.org/10.1002/2017gl073637, 2017.
Lin, M., Wang, K., Kang, S., Li, Y., Fan, Z., and Thiemens, M. H.: Isotopic signatures of stratospheric air at the himalayas and beyond, Sci. Bull., 66, 323–326, https://doi.org/10.1016/j.scib.2020.11.005, 2021.
Liu, X. and Chen, B.: Climatic warming in the Tibetan Plateau during recent decades, Int. J. Climatol., 20, 1729–1742, https://doi.org/10.1002/1097-0088(20001130)20:14<1729::aid-joc556>3.0.co;2-y, 2000.
Lyons, J. R.: Transfer of mass-independent fractionation in ozone to other oxygen-containing radicals in the atmosphere, Geophys. Res. Lett., 28, 3231–3234, https://doi.org/10.1029/2000gl012791, 2001.
Ma, Y., Wang, Y., Zhong, L., Wu, R., Wang, S., and Li, M.: The characteristics of atmospheric turbulence and radiation energy transfer and the structure of atmospheric boundary layer over the northern slope area of Himalaya, J. Meteorol. Soc. Jpn., 89, 345–353, https://doi.org/10.2151/jmsj.2011-a24, 2011.
Massling, A., Nielsen, I. E., Kristensen, D., Christensen, J. H., Sørensen, L. L., Jensen, B., Nguyen, Q. T., Nøjgaard, J. K., Glasius, M., and Skov, H.: Atmospheric black carbon and sulfate concentrations in Northeast Greenland, Atmos. Chem. Phys., 15, 9681–9692, https://doi.org/10.5194/acp-15-9681-2015, 2015.
McCabe, J. R., Savarino, J., Alexander, B., Gong, S., and Thiemens, M. H.: Isotopic constraints on non-photochemical sulfate production in the Arctic winter, Geophys. Res. Lett., 33, L05810, https://doi.org/10.1029/2005gl025164, 2006.
Mchenry, J. N. and Dennis, R. L.: The relative importance of oxidation pathways and clouds to atmospheric ambient sulfate production as predicted by the regional acid deposition model, J. Appl. Meteorol., 33, 890–905, https://doi.org/10.1175/1520-0450(1994)033<0890:trioop>2.0.co;2, 1994.
Michalski, G., Scott, Z., Kabiling, M., and Thiemens, M. H.: First measurements and modeling of Δ17O in atmospheric nitrate, Geophys. Res. Lett., 30, 1870, https://doi.org/10.1029/2003gl017015, 2003.
Patris, N., Delmas, R., Legrand, M., De Angelis, M., Ferron, F. A., Stiévenard, M., and Jouzel, J.: First sulfur isotope measurements in central Greenland ice cores along the preindustrial and industrial periods, J. Geophys. Res.-Atmos., 107, ACH 6-1–ACH 6-11, https://doi.org/10.1029/2001jd000672, 2002.
Paulot, F., Jacob, D. J., Pinder, R., Bash, J., Travis, K., and Henze, D.: Ammonia emissions in the United States, European Union, and China derived by high-resolution inversion of ammonium wet deposition data: Interpretation with a new agricultural emissions inventory (MASAGE_NH3), J. Geophys. Res.-Atmos., 119, 4343–4364, https://doi.org/10.1002/2013jd021130, 2014.
Priyadarshi, A., Hill-Falkenthal, J., Thiemens, M., Zhang, Z., Lin, M., Chan, C.-y., and Kang, S.: Cosmogenic 35S measurements in the Tibetan Plateau to quantify glacier snowmelt, J. Geophys. Res.-Atmos., 119, 4125–4135, https://doi.org/10.1002/2013jd019801, 2014.
Prospero, J. M., Ginoux, P., Torres, O., Nicholson, S. E., and Gill, T. E.: Environmental characterization of global sources of atmospheric soil dust identified with the Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) absorbing aerosol product, Rev. Geophys., 40, 2-1–2-31, https://doi.org/10.1029/2000rg000095, 2002.
Putero, D., Marinoni, A., Bonasoni, P., Calzolari, F., Rupakheti, M., and Cristofanelli, P.: Black carbon and ozone variability at the Kathmandu Valley and at the southern Himalayas: a comparison between a “hot spot” and a downwind high-altitude site, Aerosol Air Qual. Res., 18, 623–635, ap621, https://doi.org/10.4209/aaqr.2017.04.0138, 2018.
Pye, H., Liao, H., Wu, S., Mickley, L. J., Jacob, D. J., Henze, D. K., and Seinfeld, J.: Effect of changes in climate and emissions on future sulfate-nitrate-ammonium aerosol levels in the United States, J. Geophys. Res.-Atmos., 114, D01205, https://doi.org/10.1029/2008jd010701, 2009.
Pye, H. O. T., Nenes, A., Alexander, B., Ault, A. P., Barth, M. C., Clegg, S. L., Collett Jr., J. L., Fahey, K. M., Hennigan, C. J., Herrmann, H., Kanakidou, M., Kelly, J. T., Ku, I.-T., McNeill, V. F., Riemer, N., Schaefer, T., Shi, G., Tilgner, A., Walker, J. T., Wang, T., Weber, R., Xing, J., Zaveri, R. A., and Zuend, A.: The acidity of atmospheric particles and clouds, Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, 2020.
Ram, K., Sarin, M. M., and Hegde, P.: Long-term record of aerosol optical properties and chemical composition from a high-altitude site (Manora Peak) in Central Himalaya, Atmos. Chem. Phys., 10, 11791–11803, https://doi.org/10.5194/acp-10-11791-2010, 2010.
Ramanathan, V., Chung, C., Kim, D., Bettge, T., Buja, L., Kiehl, J., Washington, W., Fu, Q., Sikka, D., and Wild, M.: Atmospheric brown clouds: Impacts on South Asian climate and hydrological cycle, Proc. Natl. Acad. Sci. USA, 102, 5326–5333, https://doi.org/10.1073/pnas.0500656102, 2005.
Savarino, J. and Thiemens, M. H.: Analytical procedure to determine both δ18O and δ17O of H2O2 in natural water and first measurements, Atmos. Environ., 33, 3683–3690, https://doi.org/10.1016/s1352-2310(99)00122-3, 1999.
Savarino, J., Lee, C. C., and Thiemens, M. H.: Laboratory oxygen isotopic study of sulfur (IV) oxidation: Origin of the mass-independent oxygen isotopic anomaly in atmospheric sulfates and sulfate mineral deposits on Earth, J. Geophys. Res.-Atmos., 105, 29079–29088, https://doi.org/10.1029/2000jd900456, 2000.
Savarino, J., Alexander, B., Darmohusodo, V., and Thiemens, M. H.: Sulfur and oxygen isotope analysis of sulfate at micromole levels using a pyrolysis technique in a continuous flow system, Anal. Chem., 73, 4457–4462, https://doi.org/10.1021/ac010017f, 2001.
Savarino, J., Kaiser, J., Morin, S., Sigman, D. M., and Thiemens, M. H.: Nitrogen and oxygen isotopic constraints on the origin of atmospheric nitrate in coastal Antarctica, Atmos. Chem. Phys., 7, 1925–1945, https://doi.org/10.5194/acp-7-1925-2007, 2007.
Schauer, A. J., Kunasek, S. A., Sofen, E. D., Erbland, J., Savarino, J., Johnson, B. W., Amos, H. M., Shaheen, R., Abaunza, M., and Jackson, T. L.: Oxygen isotope exchange with quartz during pyrolysis of silver sulfate and silver nitrate, Rapid Commun. Mass Sp., 26, 2151–2157, https://doi.org/10.1002/rcm.6332, 2012.
Schwartz, S. E.: Aqueous-phase reactions in clouds, in: The Chemistry of Acid Rain: Sources and Atmospheric Processes, edited by: Johnson, R. W. and Gordon, G. E., ACS Publications, United States, Washington, DC, 93–108, 1987.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, edited by: Seinfeld, J. and Pandis, S., John Wiley & Sons, New York, 2016.
Shah, V., Jacob, D. J., Moch, J. M., Wang, X., and Zhai, S.: Global modeling of cloud water acidity, precipitation acidity, and acid inputs to ecosystems, Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, 2020.
Sherwen, T., Schmidt, J. A., Evans, M. J., Carpenter, L. J., Großmann, K., Eastham, S. D., Jacob, D. J., Dix, B., Koenig, T. K., Sinreich, R., Ortega, I., Volkamer, R., Saiz-Lopez, A., Prados-Roman, C., Mahajan, A. S., and Ordóñez, C.: Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem, Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, 2016.
Škerlak, B., Sprenger, M., and Wernli, H.: A global climatology of stratosphere–troposphere exchange using the ERA-Interim data set from 1979 to 2011, Atmos. Chem. Phys., 14, 913–937, https://doi.org/10.5194/acp-14-913-2014, 2014.
Sofen, E. D., Alexander, B., and Kunasek, S. A.: The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core
Stein, A., Draxler, R. R., Rolph, G. D., Stunder, B. J., Cohen, M., and Ngan, F.: NOAA's HYSPLIT atmospheric transport and dispersion modeling system, B. Am. Meteorol. Soc., 96, 2059–2077, https://doi.org/10.1175/bams-d-14-00110.1, 2015.
Stockwell, W. R. and Calvert, J. G.: The mechanism of the HO-SO2 reaction, Atmos. Environ., 17, 2231–2235, https://doi.org/10.1016/0004-6981(83)90220-2, 1983.
Thiemens, M. H. and Heidenreich, J. E.: The mass-independent fractionation of oxygen: A novel isotope effect and its possible cosmochemical implications, Science, 219, 1073–1075, https://doi.org/10.1126/science.219.4588.1073, 1983.
Thiemens, M. H.: Mass-independent isotope effects in planetary atmospheres and the early solar system, Science, 283, 341–345, https://doi.org/10.1126/science.283.5400.341, 1999.
Turnock, S., Mann, G., Woodhouse, M., Dalvi, M., O'Connor, F., Carslaw, K., and Spracklen, D.: The impact of changes in cloud water pH on aerosol radiative forcing, Geophys. Res. Lett., 46, 4039–4048, https://doi.org/10.1029/2019gl082067, 2019.
Ullerstam, M., Vogt, R., Langer, S., and Ljungström, E.: The kinetics and mechanism of SO2 oxidation by O3 on mineral dust, Phys. Chem. Chem. Phys., 4, 4694–4699, https://doi.org/10.1039/b203529b, 2002.
van Marle, M. J. E., Kloster, S., Magi, B. I., Marlon, J. R., Daniau, A.-L., Field, R. D., Arneth, A., Forrest, M., Hantson, S., Kehrwald, N. M., Knorr, W., Lasslop, G., Li, F., Mangeon, S., Yue, C., Kaiser, J. W., and van der Werf, G. R.: Historic global biomass burning emissions for CMIP6 (BB4CMIP) based on merging satellite observations with proxies and fire models (1750–2015), Geosci. Model Dev., 10, 3329–3357, https://doi.org/10.5194/gmd-10-3329-2017, 2017.
Vicars, W. C. and Savarino, J.: Quantitative constraints on the 17O-excess (Δ17O) signature of surface ozone: Ambient measurements from 50∘ N to 50∘ S using the nitrite-coated filter technique, Geochim. Cosmochim. Ac., 135, 270–287, https://doi.org/10.1016/j.gca.2014.03.023, 2014.
Vogt, R., Crutzen, P. J., and Sander, R.: A mechanism for halogen release from sea-salt aerosol in the remote marine boundary layer, Nature, 383, 327–330, https://doi.org/10.1038/383327a0, 1996.
Walters, W. W., Michalski, G., Böhlke, J. K., Alexander, B., Savarino, J., and Thiemens, M. H.: Assessing the seasonal dynamics of nitrate and sulfate aerosols at the South Pole utilizing stable isotopes, J. Geophys. Res.-Atmos., 124, 8161–8177, https://doi.org/10.1029/2019jd030517, 2019.
Wang, K., Hattori, S., Kang, S., Lin, M., and Yoshida, N.: Isotopic constraints on the formation pathways and sources of atmospheric nitrate in the Mt. Everest region, Environ. Pollut., 115274, https://doi.org/10.1016/j.envpol.2020.115274, 2020.
Wang, R., Tao, S., Balkanski, Y., Ciais, P., Boucher, O., Liu, J., Piao, S., Shen, H., Vuolo, M. R., and Valari, M.: Exposure to ambient black carbon derived from a unique inventory and high-resolution model, Proc. Natl. Acad. Sci. USA, 111, 2459–2463, https://doi.org/10.1073/pnas.1318763111, 2014.
Wang, T., Tang, J., Sun, M., Liu, X., Huang, Y., Huang, J., Han, Y., Cheng, Y., Huang, Z., and Li, J.: Identifying a transport mechanism of dust aerosols over South Asia to the Tibetan Plateau: A case study, Sci. Total Environ., 143714, https://doi.org/10.1016/j.scitotenv.2020.143714, 2020.
Wang, W., Xu, W., Collett Jr., J. L., Liu, D., Zheng, A., Dore, A. J., and Liu, X.: Chemical compositions of fog and precipitation at Sejila Mountain in the southeast Tibetan Plateau, China, Environ. Pollut., 253, 560–568, https://doi.org/10.1016/j.envpol.2019.07.055, 2019.
Wang, Y., Zhang, X., and Draxler, R. R.: TrajStat: GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data, Environ. Modell. Softw., 24, 938–939, https://doi.org/10.1016/j.envsoft.2009.01.004, 2009.
Wang, Y. L., Song, W., Yang, W., Sun, X. C., Tong, Y. D., Wang, X. M., Liu, C. Q., Bai, Z. P., and Liu, X. Y.: Influences of atmospheric pollution on the contributions of major oxidation pathways to PM2.5 nitrate formation in Beijing, J. Geophys. Res.-Atmos., 124, 4174–4185, https://doi.org/10.1029/2019jd030284, 2019.
Xia, X., Zong, X., Cong, Z., Chen, H., Kang, S., and Wang, P.: Baseline continental aerosol over the central Tibetan plateau and a case study of aerosol transport from South Asia, Atmos. Environ., 45, 7370–7378, https://doi.org/10.1016/j.atmosenv.2011.07.067, 2011.
Xie, L., Spiro, B., and Wei, G.: Purification of BaSO4 precipitate contaminated with organic matter for oxygen isotope measurements (δ18O and Δ17O), Rapid Commun. Mass Sp., 30, 1727–1733, https://doi.org/10.1002/rcm.7610, 2016.
Yang, Y., Zhou, R., Yan, Y., Yu, Y., Liu, J., Du, Z., and Wu, D.: Seasonal variations and size distributions of water-soluble ions of atmospheric particulate matter at Shigatse, Tibetan Plateau, Chemosphere, 145, 560–567, https://doi.org/10.1016/j.chemosphere.2015.11.065, 2016.
Yao, T., Thompson, L. G., Mosbrugger, V., Zhang, F., Ma, Y., Luo, T., Xu, B., Yang, X., Joswiak, D. R., and Wang, W.: Third pole environment (TPE), Environ. Dev., 3, 52–64, https://doi.org/10.1016/j.envdev.2012.04.002, 2012.
Yin, X., Kang, S., de Foy, B., Cong, Z., Luo, J., Zhang, L., Ma, Y., Zhang, G., Rupakheti, D., and Zhang, Q.: Surface ozone at Nam Co in the inland Tibetan Plateau: variation, synthesis comparison and regional representativeness, Atmos. Chem. Phys., 17, 11293–11311, https://doi.org/10.5194/acp-17-11293-2017, 2017.
Yuen, P.-F., Hegg, D. A., Larson, T. V., and Barth, M. C.: Parameterization of heterogeneous droplet chemistry for use in bulk cloud models, J. Appl. Meteorol., 35, 679–689, https://doi.org/10.1175/1520-0450(1996)035<0679:POHDCF>2.0.CO;2, 1996.
Zheng, X., Shen, C., Wan, G., Liu, K., Tang, J., and Xu, X.:
Short summary
Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Sulfate aerosols play an important climatic role and exert adverse effects on the ecological...
Altmetrics
Final-revised paper
Preprint