Measurements and calculations have shown significant disagreement regarding the sign and variations of the thermal expansion coefficient (TEC) of graphene α(T ). Here we report dedicated Raman scattering experiments conducted for graphene monolayers deposited on silicon nitride substrates and over the broad temperature range 150-900 K. The relation between those measurements for the G band and the graphene TEC, which involves correcting the measured signal for the mismatch contribution of the substrate, is analyzed based on various theoretical candidates for α(T ). Contrary to calculations in the quasiharmonic approximation, a many-body potential reparametrized for graphene correctly reproduces experimental data. These results indicate that the TEC is more likely to be positive above room temperature.
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