Crystals of LiNbO3 single-doped with Sm3+, Tb3+, or Dy3+ and crystal of LiTaO3 single-doped with Tb3+ were grown by the Czochralski method. Luminescence spectra and decay curves for LiNbO3 samples containing Sm3+ or Dy3+ ions were recorded at different temperatures between 295 and 775 K, whereas those for samples containing Tb3+ ions were recorded at different temperatures between 10 and 300 K. Optical absorption spectra at different temperatures were recorded within the UV-blue region relevant to optical pumping of the samples. It was found that the effect of temperature on experimental luminescence lifetimes consists of the initial temperature-independent stage followed by a steep decrease with the onset at about 700, 600, and 150 K for Sm3+, Dy3+, and Tb3+ ions, respectively. Additionally, comparison of temperature impact on luminescence properties of LiNbO3:Tb3+ and LiTaO3:Tb3+ crystals has been adequately described. Experimental results were interpreted in terms of temperature-dependent charge transfer (CT) transitions within the modified Temperature—Dependent Charge Transfer phenomenological model (TDCT). Disparity of the onset temperatures and their sequence were explained based on the location of familiar zigzag curves connecting the ground state levels of rare earth ions with respect to the band-gap of the host. It was concluded also that LiNbO3:Sm3+ is suitable as an optical sensor within the 500–750 K temperature region whereas LiNbO3:Dy3+ offers the highest sensitivity at lower temperatures between 300 and 400 K.
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