E-symmetry optical phonons at the Γ point of LiNbO3 and LiTaO3 were experimentally resolved in spectra measured by infrared and Raman spectroscopy. For this purpose, congruent and nearly stoichiometric crystals of LiNbO3 and LiTaO3, and mixed LiNb1−xTaxO3, crystals were studied. The results show that some of the E modes have weak intensities in Raman or infrared spectra. Thus the complete assignment of E-symmetry modes has been achieved by comparing Raman and infrared data. In addition, this assignment has been confirmed by Raman measurements at low temperatures.
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