Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations

Creators: Bian, Huisheng^{1, 2}; Chin, Mian²; Colarco, Peter R.²; Apel, Eric C.³; Blake, Donald R.⁴; Froyd, Karl⁵; Hornbrook, Rebecca S.³; Jimenez, Jose^{5, 6}; Jost, Pedro Campuzano^{5, 6}; Lawler, Michael^{5, 7}; Liu, Mingxu⁸; Lund, Marianne Tronstad⁹; Matsui, Hitoshi⁸; Nault, Benjamin A.^{5, 6, 10, 11}; Penner, Joyce E.¹²; Rollins, Andrew W.^{5, 13}; Schill, Gregory⁷; Skeie, Ragnhild B.⁹; Wang, Hailong¹⁴; Xu, Lu^{15, 16}; Zhang, Kai¹⁴; Zhu, Jialei¹⁷

1. University of Maryland, Baltimore County
2. Goddard Space Flight Center
3. National Center for Atmospheric Research
4. University of California, Irvine
5. Cooperative Institute for Research in Environmental Sciences
6. University of Colorado Boulder
7. Chemical Sciences Laboratory, NOAA Earth System Research Laboratories, Boulder, CO, USA
8. Nagoya University
9. Center for International Climate and Environmental Research
10. Johns Hopkins University
11. Aerodyne Research
12. University of Michigan–Ann Arbor
13. Earth System Research Laboratory
14. Pacific Northwest National Laboratory
15. California Institute of Technology
16. Washington University in St. Louis
17. Tianjin University

Abstract

The atmospheric sulfur cycle plays a key role in air quality, climate, and ecosystems, such as pollution, radiative forcing, new particle formation, and acid rain. In this study, we compare the spatially and temporally resolved measurements from the NASA Atmospheric Tomography (ATom) mission with simulations from five AeroCom III models for four sulfur species (dimethyl sulfide (DMS), sulfur dioxide (SO₂), particulate methanesulfonate (MSA), and particulate sulfate (SO₄)). We focus on remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ∼ 12 km altitude range covering all four seasons. In general, the differences among model results can be greater than 1 order of magnitude. Comparing with observations, model-simulated SO₂ is generally low, whereas SO₄ is generally high. Simulated DMS concentrations near the sea surface exceed observed levels by a factor of 5 in most cases, suggesting potential overestimation of DMS emissions in all models. With GEOS model simulations of tagging emission from anthropogenic, biomass burning, volcanic, and oceanic sources, we find that anthropogenic emissions are the dominant source of sulfate aerosol (40 %–60 % of the total amount) in the ATom measurements at almost all altitudes, followed by volcanic emissions (18 %–32 %) and oceanic sources (16 %–32 %). Similar source contributions can also be derived at broad ocean basins and on monthly scales, indicating the representativeness of ATom measurements for global ocean. Our work presents the first assessment of AeroCom sulfur study using ATom measurements, providing directions for improving sulfate simulations, which remain the largest uncertainty in radiative forcing estimates in aerosol climate models.

Copyright and License

Published by Copernicus Publications on behalf of the European Geosciences Union.

Acknowledgement

Huisheng Bian, Mian Chin, and Peter R. Colarco acknowledge the GEOS model developmental efforts at the Global Modeling and Assimilation Office (GMAO). This work was supported by NASA's MAP, Aura STM, ISFM, and ACMAP programs. The computing resources supporting this work were provided by the NASA High-End Computing (HEC) program through the NASA Center for Climate Simulation (NCCS).

Eric C. Apel and Rebecca S. Hornbrook acknowledge the support of the National Center for Atmospheric Research, which is a major facility sponsored by the National Science Foundation under Cooperative Agreement No. 1852977.

Mingxu Liu acknowledges the support of JSPS Postdoctoral Fellowships for Research in Japan (Standard).

Hitoshi Matsui was supported by the Ministry of Education, Culture, Sports, Science, and Technology and the Japan Society for the Promotion of Science (MEXT/JSPS) KAKENHI grants (JP19H05699, JP19KK0265, JP20H00196, JP20H00638, JP22H03722, JP22F22092, JP23H00515, JP23H00523, and JP23K18519); by the MEXT Arctic Challenge for Sustainability II (ArCS II) project (JPMXD1420318865); and by the Environment Research and Technology Development Fund 2-2003 (JPMEERF20202003) and 2-2301 (JPMEERF20232001) of the Environmental Restoration and Conservation Agency.

Kai Zhang and Hailong Wang acknowledge support by the U.S. Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research, Earth and Environmental Systems Modeling program. The Pacific Northwest National Laboratory (PNNL) is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RLO1830.

Lu Xu thanks Michelle Kim, Hannah Allen, John Crounse, and Paul Wennberg for operating the Caltech CIMS instrument during ATom. Lu Xu acknowledges NASA grant NNX15AG61A.

Marianne Tronstad Lund thanks Marit Sandstad (CICERO) for assistance with the model postprocessing and acknowledges the National Infrastructure for High Performance Computing and Data Storage in Norway (UNINETT) resources (grant NN9188K).

Ragnhild B. Skeie acknowledges funding from the Research Council of Norway (grant number 314997).

Funding

This research has been supported by the NASA's Earth Sciences Division (grant no. 80NSSC23K1000).

Code Availability

The GEOS Earth System Model source code and the instructions for model build are available at https://github.com/GEOS-ESM/GEOSgcm/ (The NASA GMAO group, 2024).

Data Availability

The AeroCom model outputs needed to reproduce the results described in this paper are publicly available for download at https://acd-ext.gsfc.nasa.gov/anonftp/acd/tropo/bian/ATom-AeroCom-Sulfur/ (Bian, 2024). The ATom data were obtained from their ESPO Data Archive: https://espo.nasa.gov/atom/content/ATom (Padhi and Vasques, 2024).

Supplemental Material

The supplement related to this article is available online at: https://doi.org/10.5194/acp-24-1717-2024-supplement.

Contributions

HB and MC conceptualized the ATom-AeroCom experiment. HB performed analysis and wrote the manuscript. HB, PRC, MLi, MTL, RBS, HM, JEP, HW, KZ, and JZ provided AeroCom model results, and ECA, KF, DRB, RSH, JJ, PCJ, MLa, BAN, AWR, GS, and LX contributed to ATom measurements. All authors contributed to the editing of the manuscript.

Conflict of Interest

At least one of the (co-)authors is a member of the editorial board of Atmospheric Chemistry and Physics. The peer-review process was guided by an independent editor, and the authors also have no other competing interests to declare.

Additional Information

This paper was edited by Barbara Ervens and reviewed by three anonymous referees.

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