Abstract
Although the field of nonlinear optics is over 25 years old. our understanding of the nonlinear optical properties of solids is poor. For χ(3) simple bonding molecular orbital approaches1 are unable to account in a quantitative way for the magnitude, dispersion or anisotropy. On the other hand, the number of full band structure calculations of the nonlinear optical constants of solids, arid semiconductors in particular, is small. The difficulties associated with these calculations is two-fold: first is the complex nature of the nonlinear response function itself, and second is the requirement of knowing both the electron energy bands and wavefunctions through the Brillouin zone. The only previous full band structure calculation of χ(3) focussed solely on the zero frequency limit and did not address its anisotropy which has been known for some time3,4. It has been suggested by some authors1 that the magnitude and anisotropy of χ(3) could only be understood in terms of local field effects.
© 1988 Optical Society of America
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