Crystal-Field Spectra of d3,7 Ions. I. Electronic Absorption Spectrum of CoCl4= in Three Crystalline Environments

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Abstract
The electronic absorption spectrum of the CoCl4= complex ion has been studied in crystals of the type R2CoCl4, where R is Cs, N(CH3)4, or quinolinium ion. The measurements have been made with single crystals at various temperatures down to 4.2°K with high resolution in the near infrared, visible, and near ultraviolet regions of the spectrum. The data include transitions from the ground state to states arising from six of the seven terms of the free ion. Analyses of the bands have been made, as well as an attempt to sort out the effects of spin—orbit coupling, the site symmetry, and the vibrations of the excited states. It is concluded that the assumption of cubic symmetry for the crystal field is valid only for the determination of the approximate energies of the electronic states and not for the details of the splitting patterns of orbitally degenerate states. The usefulness of crystal‐field theory which includes spin—orbit coupling and two inter‐electronic repulsion parameters is discussed.

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