First-principles calculation and experimental investigation of lattice dynamics in the rare-earth pyrochlores

Physical Review B. Volume 93, Issue 21, 29 June 2016, Article number 214308.We present a model of the lattice dynamics of the rare-earth titanate pyrochlores R2Ti2O7 (R=Tb,Dy,Ho), which are important materials in the study of frustrated magnetism. The phonon modes are obtained by density functional calculations, and these predictions are verified by comparison with scattering experiments. Single crystal inelastic neutron scattering is used to measure acoustic phonons along high symmetry directions for R=Tb, Ho; single crystal inelastic x-ray scattering is used to measure numerous optical modes throughout the Brillouin zone for R=Ho; and powder inelastic neutron scattering is used to estimate the phonon density of states for R=Tb, Dy, Ho. Good agreement between the calculations and all measurements is obtained, allowing confident assignment of the energies and symmetries of the phonons in these materials under ambient conditions. Knowledge of the phonon spectrum is important for understanding spin-lattice interactions, and can be expected to be transferred readily to other members of the series to guide the search for unconventional magnetic excitations. © 2016 American Physical Society