The complete energy matrix including all the spin states is constructed for d(4) ions in tetragonal symmetry within a strong-field representation. The excitation levels, fine-structure splitting, and EPR parameters in Rb2CrCl4 and CrF2 are studied with the energy matrix. The contributions of the spin singlets to zero-field splitting (ZFS) are investigated for the first time. The results show that the spin-singlet contribution to D is negligible, but the contributions to a and F cannot be neglected.
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