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

Ono, Shuhei·2017·Annual Review of Earth and Planetary Sciences

DOI 10.1146/annurev-earth-060115-012324

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Abstract

Archean sulfide and sulfate minerals commonly exhibit anomalous ratios among four stable sulfur isotopes,32 S,33 S,34 S, and 36 S. 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 (δ 33 S, δ 34 S, and δ 36 S) 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 (SO 2). Photolysis of SO 2 at wavelengths <220 nm and photoexcitation at 240–340 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.

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Authors: Ono, S.
Affiliations: Massachusetts Institute of Technology (US)
Corresponding author: Ono, Shuhei
ORCID: Ono, Shuhei
Venue: Annual Review of Earth and Planetary Sciences
Publisher: Annual Reviews
Published: 2017-08-30
Volume: 45
Issue: 1
Pages: 301-329
ISSN: 0084-6597 (ISSN-L)
1545-4495
DOI: 10.1146/annurev-earth-060115-012324
OpenAlex: W2620153389
Cited by: 119
References: 122
Citations by year: 2026: 8 · 2025: 11 · 2024: 15 · 2023: 14 · 2022: 12 · 2021: 13 · 2020: 22 · 2019: 13 · 2018: 9 · 2017: 2
FWCI: 1.58
Type: journal article
Language: en
Open access: closed
Licence: www.annualreviews.org/licenses/tdm (tdm)
Locations: Annual Review of Earth and Planetary Sciences (publishedVersion)
Funders: National Science Foundation
National Aeronautics and Space Administration
Topics: Physical Sciences › Earth and Planetary Sciences › Paleontology › Paleontology and Stratigraphy of Fossils
Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
Physical Sciences › Earth and Planetary Sciences › Geochemistry and Petrology › Geological and Geochemical Analysis
Keywords: sulfur dioxide, photochemistry, Archean atmosphere, early Earth atmosphere, anoxic atmosphere, sulfur isotopes, photolysis, photoexcitation, self-shielding, cross sections, vibronic coupling, intersystem crossing, sulfide minerals, sulfate minerals

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

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