AbstractOvertone bands in the spectral range of 1300−1920 cm^–1 have been found in Raman scattering spectrum of lithium tantalate single crystals. The Raman spectra were recorded in the 180° scattering geometry. The intensity of overtone transitions differs for different samples and, in some cases, is comparable with the Raman scattering intensity at the fundamental modes of a lithium tantalate single crystal.