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

H. Bian; H. Bian; M. Chin; P. R. Colarco; E. C. Apel; D. R. Blake; K. Froyd; R. S. Hornbrook; J. Jimenez; J. Jimenez; P. C. Jost; P. C. Jost; M. Lawler; M. Lawler; M. Liu; M. T. Lund; H. Matsui; B. A. Nault; B. A. Nault; B. A. Nault; B. A. Nault; J. E. Penner; A. W. Rollins; A. W. Rollins; G. Schill; R. B. Skeie; H. Wang; L. Xu; L. Xu; K. Zhang; J. Zhu

doi:10.5194/acp-24-1717-2024

Atmospheric Chemistry and Physics (Feb 2024)

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

H. Bian,
H. Bian,
M. Chin,
P. R. Colarco,
E. C. Apel,
D. R. Blake,
K. Froyd,
R. S. Hornbrook,
J. Jimenez,
J. Jimenez,
P. C. Jost,
P. C. Jost,
M. Lawler,
M. Lawler,
M. Liu,
M. T. Lund,
H. Matsui,
B. A. Nault,
B. A. Nault,
B. A. Nault,
B. A. Nault,
J. E. Penner,
A. W. Rollins,
A. W. Rollins,
G. Schill,
R. B. Skeie,
H. Wang,
L. Xu,
L. Xu,
K. Zhang,
J. Zhu

Affiliations

H. Bian: Goddard Earth Sciences Technology and Research (GESTAR) II, University of Maryland at Baltimore County, Baltimore, MD, USA
H. Bian: Chemistry and Dynamic Branch, NASA Goddard Space Flight Center, Greenbelt, MD, USA
M. Chin: Chemistry and Dynamic Branch, NASA Goddard Space Flight Center, Greenbelt, MD, USA
P. R. Colarco: Chemistry and Dynamic Branch, NASA Goddard Space Flight Center, Greenbelt, MD, USA
E. C. Apel: Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
D. R. Blake: Department of Chemistry, University of California Irvine, CA, USA
K. Froyd: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
R. S. Hornbrook: Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
J. Jimenez: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
J. Jimenez: Department of Chemistry, University of Colorado, Boulder, CO, USA
P. C. Jost: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
P. C. Jost: Department of Chemistry, University of Colorado, Boulder, CO, USA
M. Lawler: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
M. Lawler: Chemical Sciences Laboratory, NOAA Earth System Research Laboratories, Boulder, CO, USA
M. Liu: Graduate School of Environmental Studies, Nagoya University, Nagoya, Japan
M. T. Lund: Center for International Climate and Environmental Research – Oslo (CICERO), Oslo, Norway
H. Matsui: Graduate School of Environmental Studies, Nagoya University, Nagoya, Japan
B. A. Nault: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
B. A. Nault: Department of Chemistry, University of Colorado, Boulder, CO, USA
B. A. Nault: now at: Department of Environmental Health and Engineering, Whiting School of Engineering, The Johns Hopkins University, Baltimore, MD, USA
B. A. Nault: now at: Center for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., Billerica, MA, USA
J. E. Penner: Dept. of Atmospheric, Oceanic and Space Sciences, University of Michigan, Ann Arbor, MI, USA
A. W. Rollins: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
A. W. Rollins: Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, CO, USA
G. Schill: Chemical Sciences Laboratory, NOAA Earth System Research Laboratories, Boulder, CO, USA
R. B. Skeie: Center for International Climate and Environmental Research – Oslo (CICERO), Oslo, Norway
H. Wang: Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
L. Xu: Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
L. Xu: now at: Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
K. Zhang: Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
J. Zhu: Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin, China

DOI: https://doi.org/10.5194/acp-24-1717-2024
Journal volume & issue: Vol. 24
pp. 1717 – 1741

Abstract

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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.

Published in Atmospheric Chemistry and Physics

ISSN: 1680-7316 (Print); 1680-7324 (Online)
Publisher: Copernicus Publications
Country of publisher: Germany
LCC subjects: Science: Physics; Science: Chemistry
Website: http://www.atmospheric-chemistry-and-physics.net/

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