Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 111, Issue 33, Pages 11979-11983Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1406315111
Keywords
UV photolysis; sulfur isotopes
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Funding
- National Science Foundation Atmospheric Chemistry Division and polar program [ATM0960594, OPP0125761]
- Agence Nationale de la Recherche [ANR-NT09-431976]
- Centre National de la Recherche Scientifique/Projet International de Cooperation Scientifique exchange program
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Sulfur-isotopic anomalies have been used to trace the evolution of oxygen in the Precambrian atmosphere and to document past volcanic eruptions. High-precision sulfur quadruple isotope measurements of sulfate aerosols extracted from a snow pit at the South Pole (1984-2001) showed the highest S-isotopic anomalies (Delta S-33 = +1.66 parts per thousand and Delta S-36 = +2 parts per thousand) in a nonvolcanic (1998-1999) period, similar in magnitude to Pinatubo and Agung, the largest volcanic eruptions of the 20th century. The highest isotopic anomaly may be produced from a combination of different stratospheric sources (sulfur dioxide and carbonyl sulfide) via SOx photochemistry, including photoexcitation and photodissociation. The source of anomaly is linked to super El Nino Southern Oscillation (ENSO) (1997-1998)-induced changes in troposphere-stratosphere chemistry and dynamics. The data possess recurring negative S-isotope anomalies (Delta S-36 = -0.6 +/- 0.2 parts per thousand) in nonvolcanic and non-ENSO years, thus requiring a second source that may be tropospheric. The generation of nonvolcanic S-isotopic anomalies in an oxidizing atmosphere has implications for interpreting Archean sulfur deposits used to determine the redox state of the paleoatmosphere.
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