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Twisted 2D layered materials have garnered a lot of attention recently as aclass of 2D materials whose interlayer interactions and electronic propertiesare dictated by the relative rotation / twist angle between the adjacentlayers. In this work, we explore a prototype of such a twisted 2D system,artificially stacked twisted bilayer graphene (TBLG), where we probe thechanges in the interlayer interactions and electron-phonon scattering pathwaysas the twist angle is varied from 0{\deg} to 30{\deg}, using Ramanspectroscopy. The long range Moir\'e potential of the superlattice gives riseto additional intravalley and intervalley scattering of the electrons in TBLGwhich have been investigated through their Raman signatures. The densityfunctional theory (DFT) calculations of the electronic band structure of theTBLG superlattices was found to be in agreement with the resonant Ramanexcitations across the van Hove singularities in the valence and conductionbands predicted for TBLG due to hybridization of bands from the two layers. Wealso observe that the relative rotation between the graphene layers has amarked influence on the second order overtone and combination Raman modessignalling a commensurate-incommensurate transition in TBLG as the twist angleincreases. This serves as a convenient and rapid characterization tool todetermine the degree of commensurability in TBLG systems.

Probing interlayer interactions and commensurate-incommensurate transition in twisted bilayer graphene through Raman spectroscopy