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.

Absolute scale of second-order nonlinear-optical coefficients

Standards which eliminate ambiguity in reporting nonlinear phenomena, especially in the increasingly complex realm of biaxial crystals, are proposed. In order to restore uniformity to the designation of crystallographic axes and crystal tensor properties, adoption of IEEE/ANSI Std. 176, with a small but much needed modification for crystal class mm2, is recommended. For the reporting of nonlinear interaction characteristics, other frames are proposed which result in simpler rules than heretofore given for categorizing phase-matching loci, and for characterizing eigenmode polarizations, double refraction, effective nonlinear coupling, and first- and second-order acceptance bandwidths (angular, spectral, thermal) along these loci. Similarities as well as differences between biaxial and uniaxial crystals are emphasized. >

Simplified characterization of uniaxial and biaxial nonlinear optical crystals: a plea for standardization of nomenclature and conventions

The family of metal thiophosphates is an important but long-ignored compound system of the nonlinear optical (NLO) materials with desirable properties for the mid-infrared (mid-IR) coherent light generation. In the present work, the mid-IR NLO capabilities of metal thiophosphate crystals are systematically investigated based on their structure-property relationship. The linear and nonlinear optical properties of these crystals are predicted and analyzed using the first-principles calculations. In particular, several metal thiophosphate compounds are highlighted to exhibit good mid-IR NLO performances, as supported by the primary experimental results. These candidates would greatly promote the development of the mid-IR NLO functional materials.

Metal Thiophosphates with Good Mid-infrared Nonlinear Optical Performances: A First-Principles Prediction and Analysis

KTP has been found to be phase matchable for type-2 second-harmonic generation of the third harmonics of the CO2 laser wavelengths at 9.2714 and 9.5525 microm at 20.0 degrees C. The resulting angle and temperature-tuning data combined with the literature values of the Nd:YAG laser-pumped optical parametric oscillator were used to improve the Sellmeier equations and the thermo-optic dispersion formula that reproduce well the temperature-tuned 90 degree phase-matching conditions of the flux-grown crystals. Applications to quasi phase matching are presented.

Sellmeier and thermo-optic dispersion formulas for KTP

The development of frequency-conversion technology in the infrared region is in urgent need of new excellent infrared nonlinear optical (IR NLO) materials. How to achieve a good balance between laser damage threshold (LDT) and NLO coefficient (dij) for new IR NLO candidates is still a challenge. The combination of the highly electropositive alkali metal (Na) and Zn with d(10) electronic configuration into crystal structure affords one new IR NLO material, Na2ZnGe2S6. It exhibits excellent properties including a wide transparent region (0.38-22 μm), large band gap (3.25 eV), and especially a balance between a strong NLO coefficient (30-fold that of KDP) and a high LDT (6-fold that of AgGaS2), indicating a promising application in the IR region. Moreover, novel common-vertex-linked wavelike ∞[GeS3]n chains are interestingly discovered in Na2ZnGe2S6, which rarely exist in the reported thiogermanides containing alkali metals. In addition, calculated SHG density and dipole moment demonstrate that the large NLO response is mainly attributed to the cooperative effects of the [GeS4] and [ZnS4] units.

Na2ZnGe2S6: A New Infrared Nonlinear Optical Material with Good Balance between Large Second-Harmonic Generation Response and High Laser Damage Threshold.

The author reports the stable generation of 0.2-W average power IR pulses around 3.2 mu m from the KTP parametric oscillator pumped by the Nd:YAG laser at 1.064 mu m. In addition, improved Sellmeier's equations, which correctly predict almost all of the nonlinear experiments thus far reported, are presented, together with the absolute values of d/sub 31/ and d/sub 32/. >

Parametric oscillation at 3.2 mu m in KTP pumped at 1.064 mu m

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Parametric oscillation at 3.2 mu m in KTP pumped at 1.064 mu m