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Vapor transport equilibration was used to prepare lithium niobate crystals of a variety of controlled off-congruent compositions. Crystals were characterized through measurement of the ferroelectric Curie temperature Tc and measurement of the temperature for noncritical phase matching TPM of second-harmonic generation from both 1.064- and 1.32-μm laser sources. Across the majority of the single-phase region, both Tc and TPM were observed to vary nearly linearly with Li/Nb ratio. The variation in TPM with Li/Nb ratio was observed to change direction within the single-phase region at some small but finite compositional interval away from the Li-rich phase boundary. Crystals equilibrated to the Li-rich phase boundary had excellent optical homogeneity. Preparation of Li-poor crystals was hampered by extremely slow lithium diffusivity and problems with second-phase precipitation.
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Bordui et al. (1992) studied this question.
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