Abstract

We present what are to our knowledge the first theoretical and experimental results for dispersion in the anisotropy (σ) of ${\overleftrightarrow{\chi }}^{\left(3\right)}$ associated with optical third-harmonic generation in Si. The theory is based on a full empirical tight-binding band-structure calculation, and the results agree well with our measurements for 0.72 μm < λ < 1.9 μm. The calculated low-frequency limit of σ agrees with measurements from the literature better than earlier calculations do. In addition, the dispersion in the relative phase of χ₁₂₁₂⁽³⁾/χ₁₁₁₁⁽³⁾ also shows good agreement with experiment.

© 1989 Optical Society of America

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