Optical response of ferromagnetic YTiO_3 studied by spectral ellipsometry

TL;DR

This study investigates the temperature-dependent optical properties of ferromagnetic YTiO_3 using spectral ellipsometry, revealing anisotropic spectral weight redistribution linked to magnetic and lattice interactions.

Contribution

It provides the first detailed spectral analysis of YTiO_3's optical response across temperature regimes, connecting optical features with magnetic and electronic interactions.

Findings

Identification of three low-energy optical bands at 2.0, 2.9, and 3.7 eV.

Observation of a crossover in optical behavior around 100 K.

Spectral weight transfer associated with superexchange and spin-orbit phenomena.

Abstract

We have studied the temperature dependence of spectroscopic ellipsometry spectra of an electrically insulating, nearly stoichiometric YTiO_3 single crystal with ferromagnetic Curie temperature T_C = 30 K. The optical response exhibits a weak but noticeable anisotropy. Using a classical dispersion analysis, we identify three low-energy optical bands at 2.0, 2.9, and 3.7 eV. Although the optical conductivity spectra are only weakly temperature dependent below 300 K, we are able to distinguish high- and low-temperature regimes with a distinct crossover point around 100 K. The low-temperature regime in the optical response coincides with the temperature range in which significant deviations from Curie-Weiss mean field behavior are observed in the magnetization. Using an analysis based on a simple superexchange model, the spectral weight rearrangement can be attributed to intersite d_i^1d_j^1 \longrightarrow d_i^2d_j^0 optical transitions. In particular, Kramers-Kronig consistent changes in optical spectra around 2.9 eV can be associated with the high-spin-state (^3T_1) optical transition. This indicates that other mechanisms, such as weakly dipole-allowed p-d transitions and/or exciton-polaron excitations, can contribute significantly to the optical band at 2 eV. The recorded optical spectral weight gain of 2.9 eV optical band is significantly suppressed and anisotropic, which we associate with complex spin-orbit-lattice phenomena near ferromagnetic ordering temperature in YTiO_3.