Absolute scale of second-order nonlinear-optical coefficients

TLDR

The study measured second‑order nonlinear‑optical coefficients of several key materials using second‑harmonic generation, parametric fluorescence, and difference‑frequency generation across near‑infrared wavelengths. The measurements yielded more accurate, consistent coefficients, revealing that many accepted standard values are overestimated due to neglecting multiple reflections, and that Miller’s Δ varies with wavelength, limiting the applicability of Miller’s rule.

Abstract

The absolute scale of the second-order nonlinear-optical coefficients of several important nonlinear-optical materials has been obtained with improved accuracy. Second-harmonic generation, parametric fluorescence, and difference-frequency generation measurements have been made at several wavelengths in the near-infrared region. The second-harmonic generation measurement was performed at the fundamental wavelengths of 1.548, 1.533, 1.313, 1.064, and 0.852 µm. The materials measured included congruent LiNbO3,1%MgO:LiNbO3,5%MgO:LiNbO3,LiTaO3,KNbO3,KTiOPO4,KH2PO4, quartz, GaAs, GaP, α-ZnS, CdS, ZnSe, and CdTe. We made the parametric fluorescence measurement to determine the nonlinear-optical coefficients of congruent LiNbO3 and 5%MgO:LiNbO3 at pump wavelengths of 0.532 and 0.488 µm. We made the difference-frequency generation measurement for congruent LiNbO3 at a pump wavelength of 0.532 µm. The second-harmonic generation, parametric fluorescence, and difference-frequency generation measurements yielded consistent data on the nonlinear-optical coefficients of the materials. We found that many of the currently accepted standard values are overestimated because of neglect of the multiple-reflection effect in (nearly) plane-parallel-plate samples. The dispersion of the nonlinear-optical coefficients showed that Miller’s Δ is barely constant over the wavelength range measured and thus that Miller’s rule is not so good as other methods for wavelength scaling of the nonlinear-optical coefficients.