Abstract
The developments of nonlinear optical (NLO) crystals in the last decade are reviewed from two aspects. In the theoretical part, on the ab initio plane-wave pseudopotential energy method, calculation of the optical responses, including the second harmonic generation coefficients, a computer-program package, and a real-space atom-cutting method are described and employed to evaluate the degree of approximation of the anionic group theory for nonlinear optical crystals. The ab initio method combined with the anionic group theory gives much more insight into the understanding of the relationship between the optical responses and microscopic structures of NLO crystals, borate-based NLO crystals in particular. In the experimental part, we describe how to use the anionic group theory method and an experimental evaluation system to develop a series of borate-based UV-NLO crystals such as KBe2BO3F2 (KBBF) and K2Al2B2O7 (KABO). The capability of these new UV-NLO crystals in producing deep-UV harmonic output is evaluated and determined. Finally, recent advances in the generation of deep- and vacuum-UV harmonic output with these new NLO crystals are reported.
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