Enhanced Upper Tropical Tropospheric COS: Impact on the Stratospheric Aerosol Layer

Notholt, Justus; Kuang, Zhiming; Rinsland, C. P.; Toon, G. C.; Rex, Markus; Jones, Nicholas; Albrecht, Torsten; Deckelmann, Holger; Krieg, J.; Weinzierl, Christine; Bingemer, Heinz; Weller, Rolf; Schrems, Otto

doi:10.1126/science.1080320

Cited by 106 publications

(74 citation statements)

References 28 publications

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“…COS, the most abundant tropospheric S compound [∼500 parts per trillion (ppt)], is transported to the stratosphere (19) and removed by photolysis (∼70%) to SO 2 above 25 km. Increased COS (20-50%) in the tropical tropopause layer (the main entry region to the stratosphere), along with a substantial increase in other tracers of biomass burning (BB), including CO, HCN, CH 3 Cl, NO x , NO y in 1996 and 1999-2000, has been observed (20). Potassium (K), a tracer of BB, can serve in certain circumstances as a tracer of forest fires (21,22), and ice-core data have revealed increased K concentration after intensive biomass burning events from 1750 to 1980 (23).…”

Section: Significancementioning

confidence: 99%

Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere

Shaheen

Abaunza

Jackson

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

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Significance The highest S-isotope anomaly is observed in a nonvolcanic period, and the magnitude of anomaly is similar to the largest volcanic eruptions of the 20th century. S-quadruple isotope data provided the first evidence of how super El Niño Southern Oscillation (ENSO) events (1997–1998) have affected the transport and transformation of aerosols to the stratosphere; thus, record of paleo-ENSO events of this magnitude can be traced with the S-isotopic anomaly. High-resolution and high-precision S-isotopic fingerprinting also revealed that the tropospheric sulfate produced during fossil-fuel and biomass burning contributes to the stratospheric sulfate aerosol layer, a contribution previously unrecognized. The distribution of sulfur anomalies mimics the Archean isotope record, which is used to track the origin and evolution of oxygen on earth.

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Section: Significancementioning

confidence: 99%

Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere

Shaheen

Abaunza

Jackson

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

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“…The mixing ratio of OCS in the troposphere is about 500 ppt (parts per trillion) and OCS is generally well mixed over the ocean and decreases rapidly with altitude in the stratosphere (Chin and Davis, 1995;Notholt et al, 2003;Barkley et al, 2008). However, latitudinal, seasonal, and longitudinal variations are about 10 % or even larger over land.…”

Section: Introductionmentioning

confidence: 99%

“…Carbonyl sulfide (OCS) significantly influences the sulfur cycle (Ko et al, 2003;Notholt et al, 2003Notholt et al, , 2006Montzka et al, 2007). It has a greenhouse gas effect based on absorption of far-infrared radiation (Brühl et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

Characterization of Aura TES carbonyl sulfide retrievals over ocean

et al. 2014

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Abstract. We present a description of the NASA Aura Tropospheric Emission Spectrometer (TES) carbonyl sulfide (OCS) retrieval algorithm for oceanic observations, along with evaluation of the biases and uncertainties using aircraft profiles from the HIPPO (HIAPER Pole-to-Pole Observations) campaign and data from the NOAA Mauna Loa site. In general, the OCS retrievals (1) have less than 1.0 degree of freedom for signals (DOFs), (2) are sensitive in the mid-troposphere with a peak sensitivity typically between 300 and 500 hPa, (3) but have much smaller systematic errors from temperature, CO 2 and H 2 O calibrations relative to random errors from measurement noise. We estimate the monthly means from TES measurements averaged over multiple years so that random errors are reduced and useful information about OCS seasonal and latitudinal variability can be derived. With this averaging, TES OCS data are found to be consistent (within the calculated uncertainties) with NOAA ground observations and HIPPO aircraft measurements. TES OCS data also captures the seasonal and latitudinal variations observed by these in situ data.

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“…The mixing ratio of OCS is about 500 ppt (parts-per-trillion i.e. pmol mol −1 ) and almost constant throughout the troposphere, and decreases rapidly with altitude in the stratosphere (Chin and Davis, 1995;Notholt et al, 2003;Barkley et al, 2008).…”

Section: Introductionmentioning

confidence: 99%

OCS photolytic isotope effects from first principles: sulfur and carbon isotopes, temperature dependence and implications for the stratosphere

et al. 2013

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The isotopic fractionation in OCS photolysis is studied theoretically from first principles. UV absorption cross sections for OCS, OC33S, OC34S, OC36S and O13CS are calculated using the time-depedent quantum mechanical formalism and a recently developed ab-initio description of the photodissociation of OCS which takes into account the lowest four singlet and lowest four triplet electronic states. The calculated isotopic fractionations as a function of wavelength are in good agreement with recent measurements by Hattori et al. (2011) and indicate that photolysis leads to only a small enrichment of 34S in the remaining OCS. The photodissociation dynamics provide strong evidence that the photolysis quantum yield is unity at all wavelengths for atmospheric UV excitation, for all isotopologues. A simple stratospheric model is constructed taking into account the main sink reactions of OCS and it is found that overall stratospheric removal slightly favors light OCS in constrast to the findings of Leung et al. (2002). These results show, based on isotopic considerations, that OCS is an acceptable source of background stratosperic sulfate aerosol in agreement with a recent model study of of Brühl et al. (2012). The 13C isotopic fractionation due to photolysis of OCS in the upper stratosphere is significant and will leave a clear signal in the remaining OCS making it a candidate for tracing using the ACE-FTS and MIPAS data sets

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Enhanced Upper Tropical Tropospheric COS: Impact on the Stratospheric Aerosol Layer

Cited by 106 publications

References 28 publications

Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere

Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere

Characterization of Aura TES carbonyl sulfide retrievals over ocean

OCS photolytic isotope effects from first principles: sulfur and carbon isotopes, temperature dependence and implications for the stratosphere

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