Raman Linewidth Contributions from Four-Phonon and Electron-Phonon Interactions in Graphene

Abstract

The Raman peak position and linewidth provide insight into phonon anharmonicity and electron-phonon interactions (EPI) in materials. For monolayer graphene, prior first-principles calculations have yielded decreasing linewidth with increasing temperature, which is opposite to measurement results. Here, we explicitly consider four-phonon anharmonicity, phonon renormalization, and electron-phonon coupling, and find all to be important to successfully explain both the $G$ peak frequency shift and linewidths in our suspended graphene sample at a wide temperature range. Four-phonon scattering contributes a prominent linewidth that increases with temperature, while temperature dependence from EPI is found to be reversed above a doping threshold ($\hslash {\omega }_G/2$, with ${\omega }_G$ being the frequency of the $G$ phonon).

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• Assessing Phonon Coherence Using Spectroscopy
• Non-trivial phonon dynamics and significant electron-phonon coupling of the high frequency modes in a Dirac semimetal
• Electron-mediated anharmonicity and its role in the Raman spectrum of graphene