First-principles calculations of double resonance Raman spectra for monolayer MoTe$_2$

TL;DR

This study presents a first-principles computational approach combining density functional theory and Wannier functions to accurately simulate double resonance Raman spectra of monolayer MoTe$_2$, capturing key experimental features.

Contribution

It introduces a novel computational method that integrates ab-initio calculations with the electron-phonon Wannier approach to model DRR spectra in 2D materials.

Findings

Successfully reproduces experimental Raman spectra features

Identifies key DRR modes and their Brillouin zone origins

Analyzes laser polarization dependence of Raman modes

Abstract

Since double resonance Raman (DRR) spectra are laser-energy dependent, the first-principles calculations of DRR for two-dimensional materials are challenging. Here, the DRR spectrum of monolayer MoTe$_2$ is calculated by home-made program, in which we combine {\em ab-initio} density-functional-theory calculations with the electron-phonon Wannier (EPW) method. Within the fourth-order perturbation theory, we are able to quantify not only the electron-photon matrix elements within the dipole approximation, but also the electron-phonon matrix elements using the Wannier functions. The reasonable agreement between the calculated and experimental Raman spectra is achieved, in which we reproduce some distinctive features of transition metal dichalcogenides (TMDCs) from graphene (for example, the dominant intervalley process involving an electron or a hole). Furthermore, we perform an analysis of the possible DRR modes over the Brillouin zone, highlighting the role of low-symmetry points. Raman tensors for some DRR modes are given by first principles calculations from which laser polarization dependence is obtained.