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AGU: Geophysical Research Letters

 

Keywords

  • sulfuric acid
  • photodissociation and vibrationally excited states
  • quantum yield

Index Terms

  • Atmospheric Composition and Structure: Aerosols and particles
  • Atmospheric Composition and Structure: Chemical kinetic and photochemical properties
  • Atmospheric Composition and Structure: Radiation: transmission and scattering
  • Atmospheric Composition and Structure: Troposphere: composition and chemistry
  • Atmospheric Composition and Structure: Troposphere: constituent transport and chemistry

Abstract

Photodissociation yields for vibrationally excited states of sulfuric acid under atmospheric conditions

Yifat Miller

Department of Physical Chemistry and Fritz Haber Research Center, Hebrew University, Jerusalem, Israel

R. B. Gerber

Department of Physical Chemistry and Fritz Haber Research Center, Hebrew University, Jerusalem, Israel

Department of Chemistry, University of California, Irvine, California, USA

Veronica Vaida

Department of Chemistry and Biochemistry and Cooperative Institute for Research in Environmental Science, University of Colorado, Boulder, Colorado, USA

Theoretical investigations of the dynamics of the sunlight initiated dehydration of sulfuric acid are performed under atmospheric conditions. The relevant time scales for collisional deactivation and for vibrational fluorescence, which may compete with sulfuric acid dehydration in the upper stratosphere and the mesosphere are evaluated to provide a realistic quantum yield consistent with spectroscopic and theoretical results. The results obtained allow evaluation of the J values for this photochemical reaction in the atmosphere. At the higher altitudes of the upper stratosphere and the mesosphere the J values obtained are sufficiently large to satisfy model requirements and explain field observations of SO2 vertical profiles and the concentration of condensation nuclei in the stratosphere for air of recent polar origin.

Received 29 April 2007; accepted 18 July 2007; published 25 August 2007.

Citation: Miller, Y., R. B. Gerber, and V. Vaida (2007), Photodissociation yields for vibrationally excited states of sulfuric acid under atmospheric conditions, Geophys. Res. Lett., 34, L16820, doi:10.1029/2007GL030529.

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