Abstract: In this paper, the zero-field-splitting parameter b₂⁰ and the electron spectra of ZnAl₂O₄:Cr³⁺ crystal have been studied in terms of the Newman superposition model and the method of the diagonalization Hamiltonian matrices, the calculated results agree well with the experiments. The investigations show that the local structure of the (CrO₆)^9- group in the ZnAl₂O₄:Cr³⁺ Crystal is of the compressed trigonal distortion (△ θ=3.06°), and point out that the spin doublets can not be omitted for the ZFS parameter of the ground state ⁴A₂, and it can be omitted for the ground state g factor.

Key words: ZnAl₂O₄:Cr³⁺, Zero-field splitting, Lattice distortion, Electron spectra