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Measurements and calculations have shown significant disagreement regardingthe sign and variations of the thermal expansion coefficient (TEC) of graphene$\alpha(T)$. Here we report dedicated Raman scattering experiments conductedfor graphene monolayers deposited on silicon nitride substrates and over thebroad temperature range 150--900~K. The relation between those measurements forthe G band and the graphene TEC, which involves correcting the measured signalfor the mismatch contribution of the substrate, is analyzed based on varioustheoretical candidates for $\alpha(T)$. Contrary to calculations in thequasiharmonic approximation, a many-body potential reparametrized for graphenecorrectly reproduces experimental data. These results indicate that the TEC ismore likely to be positive above room temperature.

Interplay between Raman shift and thermal expansion in graphene: temperature-dependent measurements and analysis of substrate corrections