Characterization of point defects in nonlinear optical materials

Thermoluminescence (TL), optical absorption, and electron paramagnetic resonance (EPR) were used to characterize point defects in LiNbO3 and LiTaO3 Crystals. A broad TL emission, peaking at 440 nm, is observed near 94 K from LiNbO3 when the crystal is irradiated at 77 K and then rapidly warmed. From the LiTaO3 crystals two overlapping TL peaks occur at 94 and 98 K, with each showing a 350-nm maximum in spectral emission. These peaks are observed after 77-K exposure of the crystals to x rays or lasers (266, 325, or 355 nm). During excitation of these crystals at 77 K, holes are trapped on oxygen ions adjacent to lithium vacancies and electrons are trapped on niobium and tantalum ions at regular lattice sites. These defects have characteristic EPR spectra, and the trapped electron center has an optical absorption band peaking at 1200 nm in LiNbO3 and 1600 nm in LiTaO3. Upon warming, the electrons become thermally unstable and migrate to the trapped-hole sites where radiative recombination occurs.;Optical absorption and EPR were used to characterize the production and thermal decay of point defects in KD2PO4. A crystal was irradiated at 77 K with x rays and then warmed to room temperature. Immediately after the irradiation broad optical absorption bands were formed at 230, 390, and 550 nm. These bands thermally decayed in the 80 to 140 K range. Another absorption band near 450 nm appeared as the three bands disappeared. Correlations with EPR data suggest that the band at 230-nm is associated with interstitial deuterium atoms, the two bands at 390 and 550 nm are associated with self-trapped holes, and the band at 450 nm is associated with holes trapped adjacent to deuterium vacancies.;Results from quantum-mechanical calculations performed with Gaussian 98 were correlated with hyperfine data from EPR measurements for several point defects in KH2PO4. The point defects modeled with calculations are: the self-trapped hole, the proton vacancy, the silicon hole, and the oxygen vacancy. Primary results from the calculations include the minimum energy, the isotropic Fermi contact coupling terms, and the lattice relaxation