Terahertz and infrared spectroscopic evidence of phonon-paramagnon coupling in hexagonal piezomagnetic YMnO3

TL;DR

This study investigates the terahertz and infrared responses of YMnO3, revealing phonon-paramagnon coupling and magnetic excitations that vary with temperature, supported by density functional theory calculations.

Contribution

It provides new evidence of phonon-paramagnon interactions in YMnO3 through spectroscopic measurements and theoretical analysis, highlighting temperature-dependent magnetic and lattice couplings.

Findings

Antiferromagnetic resonance softens with temperature and disappears above T_N.

Weak dielectric excitations increase in oscillator strength near room temperature.

Absorption bands are attributed to phonon-phonon and phonon-paramagnon processes.

Abstract

Terahertz and far-infrared electric and magnetic responses of hexagonal piezomagnetic YMnO3 single crystals are investigated. Antiferromagnetic resonance is observed in the spectra of magnetic permeability mu_a [H(omega) oriented within the hexagonal plane] below the Neel temperature T_N. This excitation softens from 41 to 32 cm-1 on heating and finally disappears above T_N. An additional weak and heavily-damped excitation is seen in the spectra of complex dielectric permittivity epsilon_c within the same frequency range. This excitation contributes to the dielectric spectra in both antiferromagnetic and paramagnetic phases. Its oscillator strength significantly increases on heating towards room temperature thus providing evidence of piezomagnetic or higher-order couplings to polar phonons. Other heavily-damped dielectric excitations are detected near 100 cm-1 in the paramagnetic phase in both epsilon_c and epsilon_a spectra and they exhibit similar temperature behavior. These excitations appearing in the frequency range of magnon branches well below polar phonons could remind electromagnons; however, their temperature dependence is quite different. We have used density functional theory for calculating phonon dispersion branches in the whole Brillouin zone. A detailed analysis of these results and of previously published magnon dispersion branches brought us to the conclusion that the observed absorption bands stem from phonon-phonon and phonon- paramagnon differential absorption processes. The latter is enabled by a strong short-range in-plane spin correlations in the paramagnetic phase.