Raman scattering from moir\'e phonons

TL;DR

This paper presents a theoretical framework for using Raman spectroscopy to probe moiré phonon modes in twisted bilayer graphene, revealing low-frequency peaks and the influence of twist angle and polarization.

Contribution

It introduces a novel theoretical approach to identify and analyze moiré phonons via Raman spectroscopy in twisted 2D materials.

Findings

Raman spectra show low-frequency peaks distinguishing TBG from decoupled layers.

Moiré phonons include acoustic-like and zone-folded optical modes.

Raman response depends strongly on twist angle and light polarization.

Abstract

We develop a theoretical framework for probing moir\'e phonon modes using Raman spectroscopy, and illustrate it with the example of twisted bilayer graphene (TBG). These moir\'e phonons arise from interlayer sliding motion in twisted 2D materials and correspond to fluctuations of the stacking order in reconstructed moir\'e superlattices. These include both acoustic-like phason modes and a new set of low-energy optical modes originating from the zone-folding of monolayer graphene's acoustic modes, which are accessible via Raman spectroscopy. We show that the Raman response of TBG exhibits a series of low-frequency peaks that clearly distinguish it from that of decoupled layers. We further examine the role of anharmonic interactions in shaping the phonon linewidths and demonstrate the strong dependence of the Raman spectra on both the twist angle and the polarization of the incident light. Our findings establish Raman spectroscopy as a powerful tool for exploring moir\'e phonons in a broad class of twisted van der Waals systems.