Second-Order Nonlinear Optics from First Principles
Abstract
We present a new first-principle theory for the calculation of the macroscopic second-order susceptibility chi(2), based on the Time-Dependent Density-Functional Theory approach. Our method allows to include straightforwardly the many-body effects. We apply the theory to the computation of the Second-Harmonic Generation spectroscopy, showing a very good agreement with experiment for cubic semiconductor GaAs.
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