Abstract
Electronic Raman scattering up to 18000 cm-1, arising from excitons related to excited crystal-field levels of the 3d8 configuration of Ni2+, has been observed in the two-dimensional antiferromagnet K2NiF4 using ultraviolet laser excitation. The measurements involve transitions from the 3A2g ground state to the 3T2g (6500-9000 cm-1), 3T1ga (10800-12500 cm-1) and 1Ega (15000-16000 cm-1) excited states. In the magnetic phase only the spin-allowed (3A2g to 3T2g, 3A2g to 3T1ga) spectra show sharp zero-phonon lines split by an applied magnetic field. A molecular field model, acting on the single-ion substrates arising from the combined effect of the spin-orbit coupling and the tetragonal crystal field, is shown to account for the experimental results. Spin-allowed as well as spin-forbidden (3A2g to 1Ega) spectra present broad vibronic bands. The usual phonon Raman scattering is also observed and interpreted.
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