Photochemical and thermochemical pathways to S<sub>2</sub> and polysulfur formation in the atmosphere of Venus.

Francés-Monerris, Antonio; Carmona-García, Javier; Trabelsi, Tarek; Saiz-Lopez, Alfonso; Lyons, James R; Francisco, Joseph S; Roca-Sanjuán, Daniel · Nat Commun · 2022

basic_science · Level V

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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)<sub>2</sub> isomers, cis-OSSO, directly yields S<sub>2</sub> 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 S<sub>3</sub>, S<sub>4</sub>, and S<sub>8</sub>. We report here the results of high-level ab-initio quantum-chemistry computations that demonstrate that S<sub>2</sub> is not a product in cis-OSSO photolysis. Instead, we establish a novel mechanism in which S<sub>2</sub> is formed in a two-step process. Firstly, the intermediate S<sub>2</sub>O 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, S<sub>2</sub>O reacts with SO. This modified chemistry yields S<sub>2</sub> 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.