Electron-electron interactions and doping dependence of the two-phonon Raman intensity in graphene

TL;DR

This paper investigates how electron-electron interactions and doping levels influence the two-phonon Raman intensity in graphene, revealing the role of many-body effects in Raman spectral features and providing a method to measure electron-phonon coupling.

Contribution

It demonstrates that doping-dependent changes in Raman intensity are due to combined electron-phonon and electron-electron scattering, highlighting the importance of Coulomb interactions.

Findings

Doping affects the 2D Raman peak intensity through electron-electron scattering.

Electron-phonon coupling is renormalized by Coulomb interactions, exceeding DFT predictions.

The study provides a way to determine electron-phonon coupling from Raman spectra.

Abstract

Raman spectroscopy is a fast, non-destructive means to characterize graphene samples. In particular, the Raman spectra show a significant dependence on doping. While the change in position and width of the G peak can be explained by the non-adiabatic Kohn anomaly at $\Gamma$, the significant doping dependence of the 2D peak intensity has not been explained yet. Here we show that this is due to a combination of electron-phonon and electron-electron scattering. Under full resonance, the photogenerated electron-hole pairs can scatter not just with phonons, but also with doping-induced electrons or holes, and this changes the intensity. We explain the doping dependence and show how it can be used to determine the corresponding electron-phonon coupling. This is higher than predicted by density-functional theory, as a consequence of renormalization by Coulomb interactions.