Probing the uniaxial strains in MoS$_2$ using polarized Raman spectroscopy: A first-principles study

TL;DR

This study uses first-principles calculations to show how polarized Raman spectroscopy can detect and characterize uniaxial strain in monolayer MoS$_2$, revealing strain direction and magnitude through vibrational mode analysis.

Contribution

It introduces a detailed first-principles analysis of Raman mode splitting and intensity changes under uniaxial strain in MoS$_2$, providing new non-destructive strain characterization methods.

Findings

The $E'$ mode splits into $E_{ ext{parallel}}'$ and $E_ot'$ modes under strain.

The $E_{ ext{parallel}}'$ mode frequency shifts depend on strain type.

Polarized Raman spectra reveal strain direction and magnitude.

Abstract

Characterization of strain in two-dimensional (2D) crystals is important for understanding their properties and performance. Using first-principles calculations, we study the effects of uniaxial strain on the Raman-active modes in monolayer MoS$_2$. We show that the in-plane $E'$ mode at 384 cm$^{-1}$ and the out-of-plane $A_1'$ mode at 403 cm$^{-1}$ can serve as fingerprints for the uniaxial strain in this 2D material. Specifically, under a uniaxial strain, the doubly degenerate $E'$ mode splits into two non-degenerate modes: one is $E_{\parallel}'$ mode in which atoms vibrate in parallel to the strain direction, and the other is $E_\perp'$ mode in which atoms vibrate perpendicular to the strain direction. The frequency of the $E_{\parallel}'$ mode blue-shifts for a compressive strain, but red-shifts for a tensile strain. In addition, due to the strain-induced anisotropy in the MoS$_2$ lattice, the polarized Raman spectra of the $E_{\parallel}'$ and $E_{\perp}'$ modes exhibit distinct angular dependence for specific laser polarization setups, allowing for a precise determination of the direction of the uniaxial strain with respect to the crystallographic orientation. Furthermore, we find that the polarized Raman intensity of the $A_1'$ mode also shows evident dependence on the applied strain, providing additional effective clues for determining the direction of the strain even without knowledge of the crystallographic orientation. Thus, polarized Raman spectroscopy offers an efficient non-destructive way to characterize the uniaxial strains in monolayer MoS$_2$.