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Second-order nonlinear optical response of graphene

Although massless Dirac fermions in graphene constitute a centrosymmetric medium for in-plane excitations, their second-order nonlinear optical response is nonzero if the effects of spatial dispersion are taken into account. Here we present a rigorous quantum-mechanical theory of the second-order nonlinear response of graphene beyond the electric dipole approximation, which includes both intraband and interband transitions. The resulting nonlinear susceptibility tensor satisfies all symmetry and permutation properties, and can be applied to all three-wave mixing processes. We obtain useful analytic expressions in the limit of a degenerate electron distribution, which reveal quite strong second-order nonlinearity at long wavelengths, Fermi-edge resonances, and unusual polarization properties.