Infrared-active excitations related to Ho(3+) ligand-field splitting at the commensurate-incommensurate magnetic phase transition in HoMn(2)O(5)

Abstract

Linearly polarized spectra of far-infrared (IR) transmission in HoMn(2)O(5) multiferroic single crystals have been studied in the frequency range between 8.5 and 105 cm(-1) and for temperatures between 5 and 300 K. Polarization of IR-active excitations depends on the crystallographic directions in HoMn(2)O(5) and is sensitive to the magnetic phase transitions. We attribute some of the infrared-active excitations to electric-dipole transitions between ligand-field (LF) split states of Ho(3+) ions. For light polarization along crystalline b axis, the oscillator strength of electric dipoles at low frequencies (10.5, 13, and 18 cm(-1)) changes significantly at the commensurate-incommensurate antiferromagnetic phase transition at T(3)=19 K. This effect shows a strong correlation with the pronounced steps of the b-directional static dielectric function. We propose that the LF on Ho(3+) connects the magnetism and dielectric properties of this compound through coupling with the Mn spin structure. We comment on the possibility for composite excitations of magnons and excited LF states.