Photochemistry of Sulfur Dioxide and the Origin of Mass-Independent Isotope Fractionation in Earth's Atmosphere

Photochemistry of Sulfur Dioxide and the Origin of Mass-Independent Isotope Fractionation in... Archean sulfide and sulfate minerals commonly exhibit anomalous ratios among four stable sulfur isotopes, 32S, 33S, 34S, and 36S. These anomalous relationships, referred to as sulfur mass-independent fractionation (S-MIF), provide strong evidence for an early anoxic atmosphere. Correlated variations among three isotope ratios (33S, 34S, and 36S) can be observed in rocks throughout the Archean and are a key clue toward identifying the source reaction of S-MIF. Studies to investigate the origin of Archean S-MIF so far have primarily focused on the photochemistry of sulfur dioxide (SO2). Photolysis of SO2 at wavelengths <220 nm and photoexcitation at 240340 nm both yield large-magnitude S-MIF. Proposed mechanisms of S-MIF include isotopologue-dependent self-shielding, cross-sectional amplitudes, and vibronic coupling during intersystem crossing. This review discusses the emerging picture of the physical origins of S-MIF and their implications for the chemistry of the early Earth's atmosphere. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Annual Review of Earth and Planetary Sciences Annual Reviews

Photochemistry of Sulfur Dioxide and the Origin of Mass-Independent Isotope Fractionation in Earth's Atmosphere

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Publisher
Annual Reviews
Copyright
Copyright 2017 by Annual Reviews. All rights reserved
ISSN
0084-6597
eISSN
1545-4495
D.O.I.
10.1146/annurev-earth-060115-012324
Publisher site
See Article on Publisher Site

Abstract

Archean sulfide and sulfate minerals commonly exhibit anomalous ratios among four stable sulfur isotopes, 32S, 33S, 34S, and 36S. These anomalous relationships, referred to as sulfur mass-independent fractionation (S-MIF), provide strong evidence for an early anoxic atmosphere. Correlated variations among three isotope ratios (33S, 34S, and 36S) can be observed in rocks throughout the Archean and are a key clue toward identifying the source reaction of S-MIF. Studies to investigate the origin of Archean S-MIF so far have primarily focused on the photochemistry of sulfur dioxide (SO2). Photolysis of SO2 at wavelengths <220 nm and photoexcitation at 240340 nm both yield large-magnitude S-MIF. Proposed mechanisms of S-MIF include isotopologue-dependent self-shielding, cross-sectional amplitudes, and vibronic coupling during intersystem crossing. This review discusses the emerging picture of the physical origins of S-MIF and their implications for the chemistry of the early Earth's atmosphere.

Journal

Annual Review of Earth and Planetary SciencesAnnual Reviews

Published: Aug 30, 2017

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