Fine particles of barium titanate single crystal with an average particle size of about 66 nm were prepared by a hydrothermal method. In the as-prepared sample, there was a large amount of the hydroxyl group and barium vacancy, and its crystal structure was assigned to cubic with an expanded lattice using a Rietveld method. The hydroxyl group desorbed with increasing calcination temperature, especially desorbing remarkably in the range from 200 to 300 °C. Above 700 °C, there was no hydroxyl group in the particle, and the crystal structure of the sample treated at 800 °C was assigned to tetragonal with tetragonality of 1.001 using a Rietveld method. The state of the lattice vibration was measured by an infrared reflection method, and analyzed using a nonlinear least-squares method with a four-parameter semiquantum model. As the result, the crystal structure of the as-prepared sample estimated using Fourier transform infrared and Raman was assigned to tetragonal. On the O6 octahedra deformation mode, the resonance frequency was independent of the concentration of the lattice hydroxyl group while the damping factor decreased with decreasing concentration of the lattice hydroxyl group. The role of the lattice hydroxyl group on the O6 octahedra deformation mode is discussed.
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