The radiative effect of the anthropogenic influence on the stratospheric sulfate aerosol layer

Myhre, Gunnar; Berglen, Tore Flatlandsmo; Myhre, C. E. Lund; Isaksen, I. S. A.

doi:10.1111/j.1600-0889.2004.00106.x

Cited by 42 publications

(36 citation statements)

References 45 publications

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“…This finding is corroborated by a recent model-based study that indicates that although 90% of the OCS transported into the stratosphere returns unprocessed to the troposphere, the remaining OCS contributes~56% to the stratospheric aerosol burden [Sheng et al, 2015]. There has been some debate, however, on the magnitude of the OCS flux to the stratosphere and on the relative contribution of OCS to the stratospheric aerosol loading [Brühl et al, 2012;Chin and Davis, 1995;Myhre et al, 2004]. While many surface flask measurements of OCS were made from 2000 to 2006 [Montzka et al, 2007], no significant trend was found over the Southern Hemisphere during this period, corroborating results from other studies [Coffey and Hannigan, 2010;Griffith et al, 1998;Rinsland et al, 2008].…”

Section: Introductionmentioning

confidence: 53%

Positive trends in Southern Hemisphere carbonyl sulfide

Kremser

Jones

Palm

et al. 2015

Geophysical Research Letters

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Transport of carbonyl sulfide (OCS) from the troposphere to the stratosphere contributes sulfur to the stratospheric aerosol layer, which reflects incoming short‐wave solar radiation, cooling the climate system. Previous analyses of OCS observations have shown no significant trend, suggesting that OCS is unlikely to be a major contributor to the reported increases in stratospheric aerosol loading and indicating a balanced OCS budget. Here we present analyses of ground‐based Fourier transform spectrometer measurements of OCS at three Southern Hemisphere sites spanning 34.45°S to 77.80°S. At all three sites statistically significant positive trends are seen from 2001 to 2014 with an observed overall trend in total column OCS at Wollongong of 0.73 ± 0.03%/yr, at Lauder of 0.43 ± 0.02%/yr, and at Arrival Heights of 0.45 ± 0.05%/yr. These observed trends in OCS imply that the OCS budget is not balanced and could contribute to constraints on current estimates of sources and sinks.

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Section: Introductionmentioning

confidence: 53%

Positive trends in Southern Hemisphere carbonyl sulfide

Kremser

Jones

Palm

et al. 2015

Geophysical Research Letters

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“…The magnitude of 13 increases with altitude. The larger isotopic fractionation for 13 C may produce a strong enough signal in the OCS isotopic composition to be detected using the ACE-FTS or MIPAS data sets leading to a better quantification of background SSA, which is important input to climate models (Myhre et al, 2004;Solomon et al, 2011).…”

Section: Atmospheric Implicationsmentioning

confidence: 99%

“…Crutzen (1976) identified OCS photolysis as a significant (non volcanic) source of material to the stratospheric sulfate aerosol (SSA) layer. This layer is important because it can enhance stratospheric ozone depletion (Solomon et al, 1993) and influence Earth's radiative balance (Turco et al, 1980;Myhre et al, 2004).…”

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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“…6 The sulfate aerosol layer is important because it enhances stratospheric ozone depletion 10 and influences Earth's radiative balance. 4,11 Photodissociation of OCS in the stratosphere occurs via the first UV absorption band, a broad Gaussian-like a) Electronic mail: johanalbrechtschmidt@gmail.com. b) Electronic mail: rschink@gwdg.de.…”

Section: Introductionmentioning

confidence: 99%

The ultraviolet spectrum of OCS from first principles: Electronic transitions, vibrational structure and temperature dependence

Schmidt

Johnson

McBane

et al. 2012

The Journal of Chemical Physics

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Global three dimensional potential energy surfaces and transition dipole moment functions are calculated for the lowest singlet and triplet states of carbonyl sulfide at the multireference configuration interaction level of theory. The first ultraviolet absorption band is then studied by means of quantum mechanical wave packet propagation. Excitation of the repulsive 2 1 A state gives the main contribution to the cross section. Excitation of the repulsive 1 1 A state is about a factor of 20 weaker at the absorption peak (E ph ≈ 45 000 cm −1 ) but becomes comparable to the 2 1 A state absorption with decreasing energy (35 000 cm −1 ) and eventually exceeds it. Direct excitation of the repulsive triplet states is negligible except at photon energies E ph < 38 000 cm −1 . The main structure observed in the cross section is caused by excitation of the bound 2 3 A state, which is nearly degenerate with the 2 1 A state in the Franck-Condon region. The structure observed in the low energy tail of the spectrum is caused by excitation of quasi-bound bending vibrational states of the 2 1 A and 1 1 A electronic states. The absorption cross sections agree well with experimental data and the temperature dependence of the cross section is well reproduced.

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The radiative effect of the anthropogenic influence on the stratospheric sulfate aerosol layer

Cited by 42 publications

References 45 publications

Positive trends in Southern Hemisphere carbonyl sulfide

Positive trends in Southern Hemisphere carbonyl sulfide

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

The ultraviolet spectrum of OCS from first principles: Electronic transitions, vibrational structure and temperature dependence

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