Raman spectrum and phonon thermal transport in van der Waals semiconductor GaPS4

Abstract

The emergent van der Waals semiconductor GaPS4 is heralding frontiers for gallium-based semiconductors. Despite its potential, the intricacies of its Raman spectrum and phonon heat transport remain elusive. In this research, experimental and theoretical methods are employed to give a comprehensive portrayal. The Raman spectra and phonon calculations obtained were cross-validated, affirming the study's credibility. A total of 28 Raman peaks were identified, with all phonon irreducible representations delineated. Advanced calculations unveiled notable shifts in the transition of GaPS4 from bulk to monolayer. During this process, phonons undergo a red shift, and the vibration contributions of different atoms change. The lifetime and group velocity of low wavenumber phonons are markedly reduced, suppressing the thermal conductivity in the monolayer. The thermal conductivity of GaPS4 bulk at 300 K is 0.5 W/m K, and 0.13 W/m K for monolayer, while the thermal conductivity in the cleavage direction is lower. These findings offer a detailed account of the complex Raman spectra and phonon thermal transport properties of GaPS4, setting the stage for its subsequent exploration and prospective applications in electronic and thermal devices, and contributing to enriching condensed matter theory of phonon thermal transport in van der Waals materials.