Polarization-resolved and helicity-resolved Raman spectra of monolayer XP3 (X = Ge and In)

Abstract

Monolayer XP₃ (X = Ge, In) is a theoretically predicted two-dimensional (2D) material with fascinating adsorption efficiency, foreshadowing its potential applications in the photovoltaic and optoelectronic communities. To achieve a comprehensive understanding of its optical properties and to further boost quickly identifying its specific applications, in this paper we systematically investigated the polarization-resolved and helicity-resolved Raman spectra excited by two commonly used laser lines (532 nm and 633 nm) through density functional theory. The dynamical stability of monolayer XP₃ is demonstrated by phonon dispersion. Monolayer GeP₃ and InP₃ are found to exhibit significantly different point group symmetries and thereby Raman properties due to the big difference in atomic size and electronic configurations between the Ge atom and In atom. Raman anisotropy of monolayer XP₃ has been found when the wave vector of linear polarized incident light is parallel to the monolayer, and all the anisotropic Raman active phonons are categorized in terms of the locations of two (four) maxima in polarization angle dependent Raman intensities of the parallel (perpendicular) configuration. The polarization direction averaged Raman spectra have been further discussed according to the characteristics of light absorbance. The calculations of helicity-resolved Raman spectra indicate a stronger helicity selection rule under helical excitation with the wave vector normal to the monolayer. The present work paves the way for the suitable design, characterization and exploitation of the proposed 2D material with controllable surface properties for applications in electronics and optoelectronics.