2013
DOI: 10.1073/pnas.1213153110
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SO2photoexcitation mechanism links mass-independent sulfur isotopic fractionation in cryospheric sulfate to climate impacting volcanism

Abstract: Natural climate variation, such as that caused by volcanoes, is the basis for identifying anthropogenic climate change. However, knowledge of the history of volcanic activity is inadequate, particularly concerning the explosivity of specific events. Some material is deposited in ice cores, but the concentration of glacial sulfate does not distinguish between tropospheric and stratospheric eruptions. Stable sulfur isotope abundances contain additional information, and recent studies show a correlation between v… Show more

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Cited by 53 publications
(65 citation statements)
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“…A recent model that considers SO 2 photoexcitation rather than photolysis and volcanic plume chemistry (including heterogeneous stratospheric chemistry) suggests that UV photo excitation of SO 2 is another route to the observed S-MIF in volcanic sulfate. This new mechanism may also provide information about the ozone-depletion chemistry in the plume (30) and is relevant for the present data. Laboratory experiments indicate that SO 2 photodissociation is wavelength-dependent (Δ 36 S/Δ 33 S slopes vary from −1 at λ = 193 nm to −4 at λ = 248 nm as shown in Fig.…”
Section: Significancementioning
confidence: 86%
“…A recent model that considers SO 2 photoexcitation rather than photolysis and volcanic plume chemistry (including heterogeneous stratospheric chemistry) suggests that UV photo excitation of SO 2 is another route to the observed S-MIF in volcanic sulfate. This new mechanism may also provide information about the ozone-depletion chemistry in the plume (30) and is relevant for the present data. Laboratory experiments indicate that SO 2 photodissociation is wavelength-dependent (Δ 36 S/Δ 33 S slopes vary from −1 at λ = 193 nm to −4 at λ = 248 nm as shown in Fig.…”
Section: Significancementioning
confidence: 86%
“…This would also explain the very large variation in the isotopic fractionation with temperature (34), because relatively small differences in temperature lead to significant differences in the population of the rotational states, which can have a large effect on the fine structure of the cross-sections. High-resolution measurements of the isotopologue-specific cross-sections of CO 2 similar to studies performed for SO 2 (36,37) are needed to fully unravel isotopic fractionation fully on a subnanometer scale.…”
Section: Isotope Effectsmentioning
confidence: 99%
“…The photochemistry of SO 2 is complex, and modeling of the isotope effects, especially in the atmosphere, is challenging. In this issue, a unique photochemical photoexcitation mechanism that occurs in the stratosphere is presented (11). In Whitehill et al (18), a creative series of experiments and trapping the photoexcited sulfur dioxide a new mass independent isotopic signature pattern was observed.…”
mentioning
confidence: 99%
“…Further supporting evidence is the disappearance of the isotopic anomaly at ∼2 billion years ago during the time associated with a global oxygenation event and development of the protective ozone layer. Various aspects of the physical chemistry of the process, biological interactions, and the preservation and new interpretations are provided in contributions to this special issue (8,9,11). The data are a collection of published data kindly provided by James Farquhar.…”
mentioning
confidence: 99%
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