Correlation of substitutional hydrogen to refractive index profiles in annealed proton-exchanged Z - and X -cut LiNbO3

• Published in: Journal of applied physics 1995-03, Vol.77 (6), p.2697-2708
• Main Authors: Zavada, J. M., Casey, H. C., States, R. J., Novak, S. W., Loni, A.
• Format: Article
• Language: English
• ISSN: 0021-8979; 1089-7550
• DOI: 10.1063/1.358738

Previous disagreements concerning a linear correlation between the hydrogen (H) concentration and the extraordinary refractive index ne in proton-exchanged lithium niobate (LiNbO3) have been resolved by partitioning the total H into optically active substitutional H and optically inactive interstitial H. The H and Li spatial variations in both Z- and X-cut crystals were determined by secondary-ion-mass spectrometry (SIMS) with a quantitative evaluation in atoms/cm3. These samples were proton exchanged in neat benzoic acid at 185 °C and then were annealed at 400 °C for times t from 6 to 240 min in wet flowing oxygen. For the Z-cut crystals, fit of the SIMS measured H profiles by expressions obtained from the diffusion equation for diffusion from a finite layer gave a substitutional H diffusivity of DZs=5.0±0.3×10−12 cm2/s and an interstitial H diffusivity of DZi=1.4±0.1×10−11 cm2/s. The wet flowing oxygen acts as a constant source of interstitial H at the surface with the diffusivity DZi and gives an integrated H concentration due to the flowing wet oxygen which increases as √t. The Li diffusivity was DLiZ=4.8±0.2×10−12 cm2/s which is nearly equal to DZs. For X-cut crystals, the substitutional H diffusivity was DXs=3.4±0.2×10−12 cm2/s and the interstitial diffusivity was DXi=1.3±0.2×10−11 cm2/s. The ne profiles were evaluated by means of optical prism-coupling measurements and numerical simulations. In both cases of crystal orientation, the effective index diffusivity is nearly equal to the diffusivity of substitutional H. Furthermore, there is an excellent linear relationship between the ne profile and the corresponding substitutional H distribution.