Photochemical and thermochemical pathways to S2 and polysulfur formation in the atmosphere of Venus

Antonio Francés-Monerris (), Javier Carmona-García, Tarek Trabelsi, Alfonso Saiz-Lopez, James R. Lyons (), Joseph S. Francisco () and Daniel Roca-Sanjuán ()
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Antonio Francés-Monerris: Universitat de València
Javier Carmona-García: Universitat de València
Tarek Trabelsi: University of Pennsylvania
Alfonso Saiz-Lopez: Institute of Physical Chemistry Rocasolano, CSIC
James R. Lyons: Planetary Science Institute
Joseph S. Francisco: University of Pennsylvania
Daniel Roca-Sanjuán: Universitat de València

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Polysulfur species have been proposed to be the unknown near-UV absorber in the atmosphere of Venus. Recent work argues that photolysis of one of the (SO)2 isomers, cis-OSSO, directly yields S2 with a branching ratio of about 10%. If correct, this pathway dominates polysulfur formation by several orders of magnitude, and by addition reactions yields significant quantities of S3, S4, and S8. We report here the results of high-level ab-initio quantum-chemistry computations that demonstrate that S2 is not a product in cis-OSSO photolysis. Instead, we establish a novel mechanism in which S2 is formed in a two-step process. Firstly, the intermediate S2O is produced by the coupling between the S and Cl atmospheric chemistries (in particular, SO reaction with ClS) and in a lesser extension by O-abstraction reactions from cis-OSSO. Secondly, S2O reacts with SO. This modified chemistry yields S2 and subsequent polysulfur abundances comparable to the photolytic cis-OSSO mechanism through a more plausible pathway. Ab initio quantification of the photodissociations at play fills a critical data void in current atmospheric models of Venus.

Date: 2022
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DOI: 10.1038/s41467-022-32170-x

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