Abstract

Polarized single crystal absorption spectra, at 4.2 K, are reported for Cs2UO2Cl4 doped with ∼1 per cent Br. Bromide substitution removes the centre of symmetry and introduces electric-dipole intensity into parity forbidden electronic transitions. All the absorption features of the UO2Cl3Br2- ion can be accounted for in terms of an analogous set of excited states to those observed in pure Cs2UO2Cl4. This result favours σγ configurations over π3γ configurations. The properties of the orthorhombic splitting strongly suggest a role for the π3δ configuration in some of the higher energy states.

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