Abstract
A two-stage vapor transport equilibration (VTE) has been employed to mitigate lithium deficiency in single crystals of lithium tantalate, LiTaO3. This work details a low-temperature vapor transport infiltration (VTI) anneal step that establishes a lithium-rich surface layer in the treated samples which annihilates the intrinsic point defect complexes of congruent LiTaO3 while allowing depth and concentration profiles of the point defects to be measured via confocal Raman spectroscopy at different stages in the process. These data are then used to calculate diffusion coefficients for lithium in LiTaO3, which range between 4.2 × 10-11 and 2.9 × 10-10 cm2/s between 950 and 1100 °C. The lithium gradients are removed, and sample chemistry is equilibrated during a second, higher-temperature anneal in an ambient atmosphere and confirmed via additional Raman measurements. Temperature-dependent impedance spectroscopy data are also used to confirm the presence or absence of lithium gradients in these samples and show that lithiation of LiTaO3 takes place at temperatures as low as 950 °C.
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Jacob M. Ivy and Geoff L. Brennecka were supported in part by the National Science Foundation under Grant No. DMR-1555015.
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Ivy, J.M., Brennecka, G.L. Lithium diffusion in lithium tantalate as measured by confocal Raman spectroscopy. J Mater Sci 57, 7035–7041 (2022). https://doi.org/10.1007/s10853-022-07105-y
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DOI: https://doi.org/10.1007/s10853-022-07105-y