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Electronic structure of metal tetrahydroborates: quasi-relativistic X. cap alpha. -SW study of M(BH/sub 4/)/sub 4/ (M = Zr, Hf, Th, U)

Journal Article · · Inorg. Chem.; (United States)
DOI:https://doi.org/10.1021/ic00236a012· OSTI ID:6909138

Quasi-relativistic SCF-X..cap alpha.. scattered-wave calculations are presented for the series of metal tetrakis(tetrahydroborates) M(BH/sub 4/)/sub 4/ (M = Zr, Hf, Th, U). The bonding in the transition-metal compounds is that of tetrahedral d/sup 0/ complexes with strong covalent contributions from ..pi.. bonding ligand group orbitals. In the actinide complexes, 5f orbitals of the central atom are found to be important to covalent ligand-metal bonding but less than in the corresponding di-..pi..-(8)annulene compounds. The ligand field manifold of U(BH/sub 4/)/sub 4/ and the corresponding spin-orbit constant agree well with experimental data. Photoelectron spectra are reproduced satisfactorily with the exception of a uniform shift. An explanation is presented why the first ligand-derived band in the spectra of the actinide complexes is narrower than that in the transition-metal compounds. The difference between the zirconium and hafnium complexes in the splitting of the second band is found to be a relativistic effect due to a more effective covalent mixing of the Hf 6s orbital. 37 references, 5 figures, 6 tables.

Research Organization:
Technische Universitaet Muenchen, Garching, West Germany
OSTI ID:
6909138
Journal Information:
Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 25:16; ISSN INOCA
Country of Publication:
United States
Language:
English