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Evidence for Interlayer Electronic Coupling in Multilayer Epitaxial Graphene from Polarization Dependent Coherently Controlled Photocurrent Generation

Most experimental studies to date of multilayer epitaxial graphene on C-face SiC have indicated that the electronic states of different layers are decoupled as a consequence of rotational stacking. We have measured the third order nonlinear tensor in epitaxial graphene as a novel approach to probe interlayer electronic coupling, by studying THz emission from coherently controlled photocurrents as a function of the optical pump and THz beam polarizations. We find that the polarization dependence of the coherently controlled THz emission expected from perfectly uncoupled layers, i.e. a single graphene sheet, is not observed. We hypothesize that the observed angular dependence arises from weak coupling between the layers; a model calculation of the angular dependence treating the multilayer structure as a stack of independent bilayers with variable interlayer coupling qualitatively reproduces the polarization dependence, providing evidence for coupling.