Articles | Volume 25, issue 7
https://doi.org/10.5194/acp-25-4083-2025
© Author(s) 2025. 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-25-4083-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
10 Apr 2025
Research article |
| 10 Apr 2025
| 10 Apr 2025
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Department of Atmospheric and Climate Science, University of Washington, Seattle, WA 98195, USA
Jacob I. Chalif
Department of Earth Sciences, Dartmouth College, Hanover, NH 03755, USA
Linia Tashmim
Department of Environmental Sciences, University of California, Riverside, CA 92521, USA
William C. Porter
Department of Environmental Sciences, University of California, Riverside, CA 92521, USA
Kelvin H. Bates
Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, USA
Qianjie Chen
Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hong Kong SAR 999077, China
Erich C. Osterberg
Department of Earth Sciences, Dartmouth College, Hanover, NH 03755, USA
Bess G. Koffman
Department of Geology, Colby College, Waterville, ME 04901, USA
Jihong Cole-Dai
Department of Chemistry and Biochemistry, South Dakota State University, Brookings, SD 57006, USA
Dominic A. Winski
Climate Change Institute and School of Earth and Climate Science, University of Maine, Orono, ME 04469, USA
David G. Ferris
Department of Earth Sciences, Dartmouth College, Hanover, NH 03755, USA
Karl J. Kreutz
Climate Change Institute and School of Earth and Climate Science, University of Maine, Orono, ME 04469, USA
Cameron P. Wake
The Center for North Atlantic Studies, University of New England, Portland, ME 04103, USA
Department of Atmospheric and Climate Science, University of Washington, Seattle, WA 98195, USA
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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.
Michael Sigl, Matthew Toohey, Joseph R. McConnell, Jihong Cole-Dai, and Mirko Severi
Earth Syst. Sci. Data, 14, 3167–3196, https://doi.org/10.5194/essd-14-3167-2022, https://doi.org/10.5194/essd-14-3167-2022, 2022
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Volcanism is a key driver of climate. Based on ice cores from Greenland and Antarctica, we reconstruct its climate impact potential over the Holocene. By aligning records on a well-dated chronology from Antarctica, we resolve long-standing inconsistencies in the dating of past volcanic eruptions. We reconstruct 850 eruptions (which, in total, injected 7410 Tg of sulfur in the stratosphere) and estimate how they changed the opacity of the atmosphere, a prerequisite for climate model simulations.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Kathryn D. Kulju, Stephen M. McNamara, Qianjie Chen, Hannah S. Kenagy, Jacinta Edebeli, Jose D. Fuentes, Steven B. Bertman, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 2553–2568, https://doi.org/10.5194/acp-22-2553-2022, https://doi.org/10.5194/acp-22-2553-2022, 2022
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N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and highly reactive Cl radicals that impact air quality. In the inland urban atmosphere, ClNO2 was elevated during lower air turbulence and over snow-covered ground, from snowpack ClNO2 production. N2O5 and ClNO2 levels were lowest, on average, during rainfall and fog because of scavenging, with N2O5 scavenging by fog droplets likely contributing to observed increased particulate nitrate concentrations.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
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
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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
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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.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
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We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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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.
Jenna A. Epifanio, Edward J. Brook, Christo Buizert, Jon S. Edwards, Todd A. Sowers, Emma C. Kahle, Jeffrey P. Severinghaus, Eric J. Steig, Dominic A. Winski, Erich C. Osterberg, Tyler J. Fudge, Murat Aydin, Ekaterina Hood, Michael Kalk, Karl J. Kreutz, David G. Ferris, and Joshua A. Kennedy
Clim. Past, 16, 2431–2444, https://doi.org/10.5194/cp-16-2431-2020, https://doi.org/10.5194/cp-16-2431-2020, 2020
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A new ice core drilled at the South Pole provides a 54 000-year paleo-environmental record including the composition of the past atmosphere. This paper describes the gas chronology for the South Pole ice core, based on a high-resolution methane record. The new gas chronology, in combination with the existing ice age scale from Winski et al. (2019), allows a model-independent reconstruction of the delta age record.
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Hopkins, F. E., Archer, S. D., Bell, T. G., Suntharalingam, P., and Todd, J. D.: The biogeochemistry of marine dimethylsulfide, Nat. Rev. Earth Environ., 4, 361–376, https://doi.org/10.1038/s43017-023-00428-7, 2023. a
Hulswar, S., Simó, R., Galí, M., Bell, T. G., Lana, A., Inamdar, S., Halloran, P. R., Manville, G., and Mahajan, A. S.: Third revision of the global surface seawater dimethyl sulfide climatology (DMS-Rev3), Earth Syst. Sci. Data, 14, 2963–2987, https://doi.org/10.5194/essd-14-2963-2022, 2022. a, b
Jernigan, C. M., Fite, C. H., Vereecken, L., Berkelhammer, M. B., Rollins, A. W., Rickly, P. S., Novelli, A., Taraborrelli, D., Holmes, C. D., and Bertram, T. H.: Efficient Production of Carbonyl Sulfide in the Low-NOx Oxidation of Dimethyl Sulfide, Geophys. Res. Lett., 49, e2021GL096838, https://doi.org/10.1029/2021GL096838, 2022. a
Jin, Q., Grandey, B. S., Rothenberg, D., Avramov, A., and Wang, C.: Impacts on cloud radiative effects induced by coexisting aerosols converted from international shipping and maritime DMS emissions, Atmos. Chem. Phys., 18, 16793–16808, https://doi.org/10.5194/acp-18-16793-2018, 2018. a
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Jongebloed, U., Alexander, B., Cole-Dai, J., Schauer, A., Larrick, C., Wood, R., Fischer, T., Carn, S., Salimi, S., Edouard, S., Zhai, S., and Geng, L.: Sulfur isotopes of sulfate measurements from a Greenland ice core (1200–1850) and volcanic gas measurements from various volcanoes and hot springs in Iceland, Arctic Data Center [data set], https://doi.org/10.18739/A2N873162, 2022. a
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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 model 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.
Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and...
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