Crystallization characteristics of Li2O–Nb2O5 compound films on sapphire substrates and formation of crack-free and thick LiNbO3 epitaxial films

摘要

? 2022 Elsevier Ltd and Techna Group S.r.l.The formation of crystal phases in Li2O–Nb2O5 compound films deposited on sapphire C-plane and A-plane substrates was studied by X-ray diffraction. Sufficiently oxidized samples with Li-deficient or stoichiometric compositions were prepared by co-sputtering from LiNbO3 (LN) and Li2O targets. Crystallization during deposition at elevated temperatures and solid-phase crystallization (SPC) of deposited amorphous films were investigated. For films on sapphire C-planes, nucleation into Li3NbO4(222) domains occurred at the onset temperature of crystallization. In the case of stoichiometric films, the LN(006) signal indicating epitaxial growth was the primary one for crystallization during deposition above 460 °C and SPC above 750 °C. Misoriented LN(104) domains tended to coexist with LN(006) domains. In the case of Li-deficient films, LiNb3O8(_602) domains coexisted with LN(006) at temperatures above 750 °C as a result of Li2O loss. For films on sapphire A-planes, epitaxial LN(110) domains were predominant. Li3NbO4(222) domains were totally absent and the signal intensity of LiNb3O8(212) was less than 10 of that of LN(110) even for the Li-deficient films, which reflected fast crystallization of LN(110) domains. The SPC rate of stoichiometric film was considerably lower than that of Li-deficient film. As-crystallized LN film on the sapphire C-plane was strained with a narrow domain width. Thick film cracked as a result of stress caused by lattice mismatch with the substrate. In contrast, LN film processed by SPC was not strained and had large domains with flat film surface. Based on these results, crack-free 1-μm-thick LN epitaxial films on a sapphire C-plane were achieved. First, an amorphous LN buffer was subject to SPC to obtain a relaxed buffer layer. Subsequently, a stress-free thick LN overlayer was grown by co-sputtering from Li2O and LN targets at 530 °C. The relaxed buffer layer effectively mitigated the strain caused by the lattice mismatch with the substrate.