28 Aug 2023
 | 28 Aug 2023
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Analysis of the global atmospheric background sulfur budget in a multi-model framework

Christina V. Brodowsky, Timofei Sukhodolov, Gabriel Chiodo, Valentina Aquila, Slimane Bekki, Sandip S. Dhomse, Anton Laakso, Graham W. Mann, Ulrike Niemeier, Ilaria Quaglia, Eugene Rozanov, Anja Schmidt, Takashi Sekiya, Simone Tilmes, Claudia Timmreck, Sandro Vattioni, Daniele Visioni, Pengfei Yu, Yunqian Zhu, and Thomas Peter

Abstract. Sulfate aerosol in the stratosphere is an important climate driver, causing solar dimming in the years after major volcanic eruptions. Hence, a growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant chemical processes and associated feedbacks. However, uncertainties of these schemes are not well constrained. Stratospheric sulfate is modulated by natural emissions of sulfur-containing species, including volcanic eruptive, and anthropogenic emissions. Model intercomparisons have examined the effects of volcanic eruptions, whereas the background conditions of the sulfur cycle have not been addressed in a global model intercomparison project. Assessing background conditions in global models allows us to identify model discrepancies as they are masked by large perturbations such as volcanic eruptions, yet may still matter in the aftermath of such a disturbance.

Here, we analyze the atmospheric burden, seasonal cycle, and vertical and meridional distribution of the main sulfur species among nine global atmospheric aerosol models that are widely used in the stratospheric aerosol research community. We use observational and reanalysis data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO2) make up about 98 % of stratospheric sulfur and 95 % of tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO2 strongly affects the sulfate aerosol burden in the Northern Hemispheric troposphere, while its importance is very uncertain in other regions. The total deposition of sulfur varies among models, deviating by a factor of two, but models agree that sulfate aerosol is the main form in which sulfur is deposited. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. We investigate the areas of greatest variability in the sulfur species burdens and find that inter-model variability is low in the tropics and increases towards the poles. Seasonality in the southern hemisphere is depicted very similar among models. Differences are largest in the dynamically active northern hemispheric extratropical region, hence some of the differences could be attributed to the differences in the representation of the stratospheric circulation among underlying general circulation models. This study highlights that the differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed focusing on the clarification of the reasons for biases, given also the importance of this topic for the stratospheric aerosol injection studies.

Christina V. Brodowsky et al.

Status: open (until 09 Oct 2023)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-1655', Anonymous Referee #1, 03 Sep 2023 reply
  • RC2: 'Comment on egusphere-2023-1655, observations missing', Anonymous Referee #2, 21 Sep 2023 reply

Christina V. Brodowsky et al.

Christina V. Brodowsky et al.


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Short summary
The aerosol layer is an essential part of the climate system. We characterize the sulfur budget in a volcanically quiescent (background) setting, with a special focus on the sulfate aerosol layer, for the first time using a multi-model approach. The aim is to identify weak points in the representation of the atmospheric sulfur budget in an intercomparison of nine state-of-the-art coupled global circulation models.