Theory for the nonlinear optical response of semiconductor surfaces: Application to the optical Stark effect and spectral oscillations of the Si(111)-(2×1)surface exciton

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A microscopic approach is presented to compute nonlinear optical properties of semiconductor surfaces. The method uses quasiparticle wave functions and dispersions obtained from ab initio band-structure theory as an inputfor Bloch equations which describe the optical properties. Excitonic effects in the linear absorption spectra of the Si(111)-(2×1) surface are obtained by integrating equations of motion. To demonstrate the applicability of the approach for analyzing nonlinear optical properties, ultrafast light-intensity-dependent absorption changes of the surface exciton are predicted. The numerical results discuss the optical Stark effect and spectral oscillations of the surface exciton which can both be observed in pump-probe experiments.