Excited Potential Energy Surfaces of $CH_{3}SH$ from the {Ab Initio} Effective Valence Shell Hamiltonian Method.

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1994

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Ohio State University

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Abstract

The ground and first and second ${^{1}A}^{\prime\prime}$ surfaces of methyl mercaptan $(CH_{3}SH)$ are calculated as a function of the C-S and S-H bond coordinates using the ab initio effective valence shell Hamiltonian $(\mathcal{H}\nu)$ method. These computations provide the first serious tests for choosing restricted valence spaces and for computing global potential energy surfaces with the $\mathcal{H}\nu$ methods. The global surfaces are computed with a modest basis, but larger basis set computations at selected geometries test convergence for vertical excitation energies, ionization potentials, and C-S and S-H bond energies. The calculations assist in the interpretation of $CH_{3}SH$ photodissociation dynamics observed by Butler and $co-workers^{1}$.

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1. J.S. Keller, P.W. Kash, E. Jensen and L.J. Butler, J. Chem. Phys, 96, 4323 (1992); E. Jensen, J.S. Keller, G.C.G. Washewsky, J.E. Stevens, R.L Graham, K.F. Freed, and L.J. Butler, J. Chem. Phys. 98, 2882 (1993).
Author Institution: The James Franck Institute and the Department of Chemistry, The University of Chicago

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