Lithium niobate (LiNbO 3 ) and lithium tantalate (LiTaO 3 ) crystals have gained increasing interest during recent years because of their fascinating physical properties, such as piezoelectricity, ferroelectricity, pyroelectricity, birefringence, electrooptical, and nonlinear-optic effects. These properties have been successfully utilized for applications in various fields. Basic experiments on acoustic surface wave propagation, electrooptical modulation, optical wave guiding, second harmonic generation, and pyroelectric detection have been performed with these crystals.LiNbO 3 and its isomorphous compound LiTaO 3 are not found in nature. The first successful growth of large single crystals by the Czochralski technique was reported by Ballman [1]. A peculiarity results from the fact that the congruently melting composition (about 48.4 mol % Li 2 O) does not coincide with the stoichiometric one (50 mol % Li 2 O). The crystals have a perovskite-like structure with oxygen octahedra and are trigonal with only one structural phase transition (paraelectric-ferroelectric) at the Curie temperature T c of about 1150 • C for LiNbO 3 and about 610 • C for LiTaO 3 . The nonpolar high-temperature phase belongs to the space group R3c (point group 3m) and at T c the transition to the ferroelectric low-temperature phase of the space group R3c (point group 3m) occurs. At room temperature LiNbO 3 is negatively birefringent. The birefringence of LiTaO 3 is very small at room temperature and positive for the congruently melting composition. More information about growth and fundamental properties of LiNbO 3 can be found in [2,3]. 83