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Temperature coefficient of frequency of LiTaO3 single crystals was tuned by changing the Li stoichiometry. For this purpose, congruent 36°Y cut crystals, available commercially, were treated by vapor transport equilibration and temperature coefficient of frequency of surface acoustic waves propagating along X-axis as a function of Li concentration was studied. The temperature coefficient of frequency of -7 ppm/° was achieved for surface acoustic waves propagating in the crystals containing 49.43 mol % of Li2O.