Spectral Representation for the Effective Macroscopic Response of a Polycrystal: Application to Third-Order Nonlinear Susceptibility

Erratum: In our paper, we show that the spectral representation for isotropic two-component composites also applies to uniaxial polycrystals. We have learned that this result was, in fact, first conjectured by G.W. Milton. While our derivation is more detailed, our result for the spectral function is the same as Milton's. We very much regret not having been aware of this work at the time of writing our paper. Original abstract: We extend the spectral theory used for the calculation of the effective linear response functions of composites to the case of a polycrystalline material with uniaxially anisotropic microscopic symmetry. As an application, we combine these results with a nonlinear decoupling approximation as modified by Ma et al., to calculate the third-order nonlinear optical susceptibility of a uniaxial polycrystal, assuming that the effective dielectric function of the polycrystal can be calculated within the effective-medium approximation.