An Initio Studies of Ground and Excited Electronic States of MgAr, CdAr, and BeAr

Abstract

The ground state and several excited state potential energy surfaces for the diatomic molecules MgAr, CdAr, and BeAr have been computed using complete active space self-consistent field (CASSCF) wavefunctions and valence double- and triple-zeta quality basis sets augmented with polarization and diffuse functions. Pump-and-probe laser experiments have examined the quenching of excited singlet states of metal-rare gas complexes such as CdXe to produce triplets that dissociate to 3P sub J metal atoms. This quenching, which is detected for CdXe but not for CdAr or MgAr, is thought to occur via a crossing or strong coupling of a repulsive triplet curve with an attractive singlet curve. The present work indicates that the attractive C 1 Pi and repulsive c 3 Sigma(+) curves of MgAr and CdAr do not intersect in the energetically accessible region of the C 1 Pi surface, unlike the corresponding curves for the CdXe diatom. These data are consistent with the absence of 3P sub J Mg and 3P sub J Cd atoms in the MgAr and CdAr experiments, respectively. However, an alternative quenching mechanism involving vibronic coupling between the C 1 Pi vibrational eigenstates and the continuum eigenstates of the underlying repulsive 3 Sigma(+) surface may be operative.

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Document Details

Document Type
Technical Report
Publication Date
Jul 26, 1991
Accession Number
ADA239248

Entities

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  • Jack Simons
  • Jerry A. Boatz
  • Keld L. Bak

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  • University of Utah

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