Pressure-induced optical anisotropy of HfS2

Abstract

The effect of pressure on Raman scattering (RS) in bulk HfS2 is investigated under hydrostatic and non-hydrostatic pressure conditions. The RS line shape does not change significantly in the hydrostatic regime up to P = 9.6 GPa, showing a systematic blueshift of the spectral features. In a non-hydrostatic environment, seven peaks appear in the spectrum at P = 7 GPa, which dominate the RS line shape up to P = 10.5 GPa. The change in the RS line shape manifests a pressure-induced phase transition in HfS2. The simultaneous observation of both low-pressure (LP) and high-pressure (HP) related RS peaks suggests the coexistence of two different phases over a wide pressure range. It is found that the HP-related phase is metastable and persists during the decompression cycle down to P = 1.2 GPa, while the LP-related features eventually recover at even lower pressure. The angle-resolved polarized RS performed under P = 7.4 GPa revealed a strong in-plane anisotropy of both the LP-related A1g mode and the HP peaks. The anisotropy is related to the possible distortion of the structure induced by the non-hydrostatic component of the pressure. The results are explained in terms of a distorted Pnma phase as a possible pressure-induced phase of HfS2.