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Temperature-activated layer-breathing vibrations in few-layer graphene

We investigated the low-frequency Raman spectra of freestanding few-layer graphene (FLG) at varying temperatures (400 - 900 K) controlled by laser heating. At high temperature, we observed the fundamental Raman mode for the lowest-frequency branch of rigid-plane layer-breathing mode (LBM) vibration. The mode frequency redshifts dramatically from 81 cm-1 for bilayer to 23 cm-1 for 8-layer. The thickness dependence is well described by a simple model of coupled oscillators. Notably, the LBM Raman response is unobservable at room temperature, and it is turned on at higher temperature (>600 K) with a steep increase of Raman intensity. The observation suggests that the LBM vibration is strongly suppressed by molecules adsorbed on the graphene surface, but is activated as desorption occurs at high temperature.