Theory of the Raman spectrum of rotated double-layer graphene

TL;DR

This paper theoretically analyzes how the Raman spectrum of rotated double-layer graphene depends on the twist angle, revealing complex behaviors of the 2D peak and providing methods to determine the angle via Raman spectroscopy.

Contribution

It introduces a simplified model linking Raman features to the twist angle, accounting for electronic interactions and decomposing the 2D peak, aligning well with experimental data.

Findings

Raman G peak intensity varies simply with angle 

Raman 2D peak shows complex dependence on 

Decomposition of 2D peak reveals two components with distinct linewidths

Abstract

We study theoretically the Raman spectrum of the rotated double-layer graphene, consisting of two graphene layers rotated with respect to each other by an arbitrary angle \theta. We find a relatively simple dependence of the Raman G peak intensity on the angle \theta. On the other hand, the Raman 2D peak position, intensity, and width show a much more complicated dependence on the angle \theta. We account for all of these effects, including dependence on the incoming photon energy, in good agreement with the experimental data. We find that it is sufficient to include the interaction between the graphene layers on the electronic degrees of freedom (resulting in the occurrence of van Hove singularities in the density of states). We assume that the phonon degrees of freedom are unaffected by the interaction between the layers. Furthermore, we decompose the Raman 2D peak into two components having very different linewidths; these widths are almost independent of the angle \theta. The change in the intensity and the peak position of one of these two components gives insight into the dependence of the overall Raman 2D peak features as a function of the angle \theta. Additionally, we show regions in the phonon spectrum giving rise to the Raman 2D peak signal. This work provides an insight into the interplay between the mechanical degree of freedom (angle \theta) and the electronic degrees of freedom (singularities in the density of states) in rotated double-layer graphene. Additionally, this work provides a way to establish experimentally the value of the rotation angle \theta using Raman spectroscopy measurement. This procedure becomes even more robust if one repeats the Raman spectroscopy measurement with a different incoming photon energy.