Infrared lattice dynamics in negative thermal expansion material in single-crystal ScF₃

Simple cubic 'open' perovskite ScF₃ stands out among trifluoride materials in its large, isotropic negative thermal expansion (NTE), but also its proximity of its zero-temperature state to a structural phase transition. Here we report a temperature- and frequency-dependent lattice dynamical study of Brillouin zone center lattice excitations of single crystals of ScF₃ using infrared reflectivity measurements. In addition to quantifying the mode strengths and energies in single crystals of this interesting material, we also find strong evidence for multiphonon absorption processes which excite the zone-edge incipient soft modes associated with NTE and the structural quantum phase transition. In this way, we identify an optically-allowed pathway to excite soft modes provides a means to athermally populate modes associated with NTE in ScF₃.