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Ferroelectric lithium niobate (LiNbO3 :LN) and lithium tantalate (LiTaO3 :LT) crystals were discovered by Matthias and Remeika in 1949. They have attracted a great deal of interest because of their large piezoelectricity, pyroelectricity, electro-optic and nonlinear optical coefficients, and transparency in a wavelength range from near ultraviolet (UV) to mid-infrared. No other materials have been investigated in so many various fields or used in a wide range of applications because of their multi-functional ferroelectric properties.