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Nonlinear optics from an<i>ab initio</i>approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors
We present an ab-initio real-time-based computational approach to study nonlinear optical properties in condensed matter systems that is especially suitable for crystalline solids and periodic nanostructures. The equations of motion and the coupling of the electrons with the external electric field are derived from the Berry-phase formulation of the dynamical …