Raman Spectra and Strain Effects in Bismuth Oxychalcogenides

TL;DR

This study combines theoretical and experimental methods to analyze Raman spectra and strain effects in bismuth oxychalcogenides, revealing how interlayer interactions and strain influence vibrational modes for potential nanoelectronic applications.

Contribution

It provides the first comprehensive analysis of Raman spectra and strain effects in Bi2O2Se, Bi2O2Te, and Bi2O2S, including a universal theoretical equation for strain-induced Raman shifts.

Findings

Experimental Raman peaks match theoretical predictions.

Interlayer interaction decreases lead to softer Raman modes.

Strain causes splitting and anisotropic shifts in Raman-active modes.

Abstract

A new type of two-dimensional layered semiconductor with weak electrostatic but not van der Waals interlayer interactions, Bi2O2Se, has been recently synthesized, which shown excellent air stability and ultrahigh carrier mobility. Herein, we combined theoretical and experimental approaches to study the Raman spectra of Bi2O2Se and related bismuth oxychalcogenides (Bi2O2Te and Bi2O2S). The experimental peaks were fully consistent with the calculated results, and were successfully assigned. Bi2O2S was predicted to have more Raman-active modes due to its lower symmetry. The shift of the predicted frequencies of Raman active modes was also found to get softened as the interlayer interaction decreases from bulk to monolayer Bi2O2Se and Bi2O2Te. To reveal the strain effects on the Raman shifts, a universal theoretical equation was established based on the symmetry of Bi2O2Se and Bi2O2Te. It was predicted that the doubly degenerate modes split under in-plane uniaxial/shear strains. Under a rotated uniaxial strain, the changes of Raman shifts are anisotropic for degenerate modes although Bi2O2Se and Bi2O2Te were usually regarded as isotropic systems similar to graphene. This implies a novel method to identify the crystallographic orientation from Raman spectra under strain. These results have important consequences for the incorporation of 2D Bismuth oxychalcogenides into nanoelectronic devices.