Theory of Raman and Resonant Inelastic X-ray Scattering from Collective Orbital Excitations in YTiO$_3$

TL;DR

This paper develops and compares two theoretical models for orbital excitations in YTiO$_3$, successfully matching experimental Raman and RIXS spectra and elucidating the nature of orbital interactions.

Contribution

It introduces two models for orbital excitations in YTiO$_3$, demonstrating that the superexchange model accurately reproduces experimental spectra.

Findings

Superexchange model fits experimental spectra well

Orbital excitations are collective (orbitons) in the superexchange model

Lattice distortion model describes local dd-transitions

Abstract

We present two different theories for Raman scattering and Resonant Inelastic X-ray Scattering (RIXS) in the low temperature ferromagnetic phase of YTiO$_3$ and compare this to the available experimental data. For description of the orbital ground-state and orbital excitations, we consider two models corresponding to two theoretical limits: one where the $t_{2g}$ orbitals are degenerate, and the other where strong lattice distortions split them. In the former model the orbitals interact through superexchange. The resulting superexchange Hamiltonian yields an orbitally ordered ground state with collective orbital excitations on top of it - the orbitons. In the orbital-lattice model, on the other hand, distortions lead to local dd-transitions between crystal field levels. Correspondingly, the orbital response functions that determine Raman and RIXS lineshapes and intensities are of cooperative or single-ion character. We find that the superexchange model yields theoretical Raman and RIXS spectra that fit very well to the experimental data.