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Title: Electronic structure of homoleptic transition metal hydrides: TiH/sub 4/, VH/sub 4/, CrH/sub 4/, MnH/sub 4/, FeH/sub 4/, CoH/sub 4/, and NiH/sub 4/

Journal Article · · J. Chem. Phys.; (United States)
OSTI ID:5939935

Ab initio molecular electronic structure theory has been applied to the family of transition metal tetrahydrides TiH/sub 4/ through NiH/sub 4/. For the TiH/sub 4/ molecule a wide range of contracted Gaussian basis sets has been tested at the self-consistent-field (SCF) level of theory. The largest basis, labeled M(14s 11p 6d/10s 8p 3d), H(5s 1p/3s 1p), was used for all members of the series and should yield wave functions approaching true Hartree-Fock quality. Predicted SCF dissociation energies (relative to M+4H) and M--H bond distances are TiH/sub 4/ 132 kcal, 1.70 A; VH/sub 4/ 86 kcal, 1.64 A; CrH/sub 4/ 65 kcal, 1.59 A; MnH/sub 4/ -- 36 kcal, 1.58 A; FeH/sub 4/ 0 kcal, 1.58 A; CoH/sub 4/ 27 kcal, 1.61 A; and NiH/sub 4/ 18 kcal, 1.75 A. It should be noted immediately that each of these SCF dissociation energies will be increased by electron correlation effects by perhaps as much as 90 kcal. For all of these molecules except TiH/sub 4/ excited states have also been studied. One of the most interesting trends seen for these excited states is the shortening of the M--H bond as electrons are transferred from the antibonding 4t/sub 2/ orbital to the nonbonding 1e orbitals.

Research Organization:
Department of Chemistry and Lawrence Berkeley Laboratory, University of California, Berkeley, California 94720
OSTI ID:
5939935
Journal Information:
J. Chem. Phys.; (United States), Vol. 71:2
Country of Publication:
United States
Language:
English