Optical properties of ZnCr2Se4 - Spin-phonon coupling and electronic d-d-like excitations

Abstract

We studied the optical properties of antiferromagnetic ZnCr2Se4 by infrared spectroscopy up to 28,000 cm-1 and for temperatures from 5 to 295 K. At the magnetic phase transition at 21 K, one of the four phonon modes reveals a clear splitting of 3 cm-1 as a result of spin-phonon coupling, the other three optical eigenmodes only show shifts of the eigenfrequencies. The antiferromagnetic ordering and the concomitant splitting of the phonon mode can be suppressed in a magnetic field of 7 T. At higher energies we observed a broad excitation band which is dominated by a two-peak-structure at about 18,000 cm-1 and 22,000 cm-1, respectively. These energies are in good agreement with the expected spin-allowed crystal-field transition of the Cr3+ ions. The unexpected strength of these forbidden onsite d-d transitions is attributed to a considerable hybridization of the selenium p with the chromium d orbitals.

8 pages, 6 figures

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• Far-infrared optical excitations in multiferroic TbMnO_3
• Exciton-magnon transitions in the frustrated chromium antiferromagnets CuCrO2, alpha-CaCr2O4, CdCr2O4, and ZnCr2O4
• Evolution of optical properties of chromium spinels CdCr${}_2$O${}_4$, HgCr${}_2$S${}_4$, and ZnCr${}_2$Se${}_4$ under high pressure
• On the complexity of spinels: Magnetic, electronic, and polar ground states