Although the field of nonlinear optics is considered to be reasonably mature, our understanding of the microscopic origin of the nonlinear optical response of solids is quite poor. Simple bonding molecular orbital techniques typically only come within an order of magnitude, at best, in predicting the magnitude of χ(2) or χ(3) and are unable to predict any dispersion or anisotropy in the nonlinear coefficients. This is true even for simple semiconductors such as Ge, Si, and GaAs, for which local field effects are often invoked to account for discrepancies between theory and experiment, Of course the difficulty in obtaining detailed knowledge is the complexity of the nonlinear response combined with the requirement of knowing both the electronic energy bands and wave functions throughout the Brillouin zone.

© 1989 Optical Society of America

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