12 Sep 2023
 | 12 Sep 2023
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

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

Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu

Abstract. The sulfur cycle plays a key role in atmospheric air quality, climate, and ecosystems. In this study, we compare the spatial and temporal distribution of four sulfur-containing species, dimethyl sulfide (DMS), sulfur dioxide (SO2), particulate methanesulfonate (MSA), and particulate sulfate (SO4), that were measured during the airborne NASA Atmospheric Tomography (ATom) mission and simulated by five AeroCom-III models to analyze the budget of sulfur cycle from the models. This study focuses on remote regions over the Pacific, Atlantic, and Southern Oceans from near the ocean surface to ~12-km altitude range, and covers all four seasons. These regions provide us with highly heterogeneous natural and anthropogenic source environments, which is not usually the case for traditional continental studies. We examine the vertical and seasonal variations of these sulfur species over tropical, mid-, and high-latitude regions in both hemispheres. We identify their origins from land versus ocean and from anthropogenic versus natural sources with sensitivity studies by applying tagged tracers linking to emission types and regions. In general, the differences among model results can be greater than one-order of magnitude. Comparing with observations, simulated SO2 is generally low while SO4 is high, and the model-observation agreement is much better in ATom-4 (April–May, 2018). There are much larger DMS concentrations simulated close to the sea surface than observed, indicating that the DMS emissions may be too high from all models. Anthropogenic emissions are the dominant source (40–60 % of the total amount) for atmospheric sulfate simulated at locations and times along the ATom flight tracks at almost every altitude, followed by volcanic emissions (18–32 %) and oceanic sources (16–32 %). Similar source contributions can also be derived at broad ocean basin and monthly scales, indicating that any reductions of anthropogenic sulfur emissions would have global impacts in modern times.

Huisheng Bian et al.

Status: open (until 24 Oct 2023)

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Huisheng Bian et al.


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Short summary
This work studies sulfur in remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, the spread of model simulations, and the observation-model discrepancies. Such understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulation and improve our understanding of sulfur cycle in atmospheric air quality, climate, and ecosystems.