4.6 Article

Large Effect of Temperature Cycling on the Electrical and Optical Properties of TiO2:H Thin Films

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 127, Issue 29, Pages 14415-14424

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.3c02215

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Hydrogenated titanium dioxide (TiO2:H) thin films with thicknesses ranging from 33 to 300 nm were grown using reactive radio-frequency magnetron sputter deposition. The electrical resistivity, Seebeck coefficient, and optical absorption coefficient of these films were characterized. However, heating to temperatures above 430 K resulted in irreversible property changes, which depended on the atmosphere during thermal treatment.
In this study, hydrogenatedtitanium dioxide (TiO2:H)thin films of thicknesses between 33 and 300 nm were grown via thereactive radio-frequency magnetron sputter deposition technique. Thesethin films were characterized with respect to electrical resistivity,Seebeck coefficient, and optical absorption coefficient. However,heating to temperatures above 430 K results in irreversible propertychanges of the thin films. The characteristics of these changes dependedon the atmosphere, in which the samples were thermally treated (10(-7) mbar vacuum or 1 bar of 99.99% N-2). Inorder to explain these findings, we investigated our samples not onlyin the as-deposited state but also after thermal cycling over differenttemperature ranges. Mott's three-dimensional (3D) variablerange hopping model was identified as the most appropriate electricalconductivity model in the as-deposited state for the temperature rangeof 223-430 K, after which it changes irreversibly to the smallpolaron hopping model in the 223-615 K temperature range. Thisthermally induced change appears to be due to changes in the numberof intrinsic (interstitial titanium Ti-int, titanium vacanciesV(Ti), and oxygen vacancies V-o) and extrinsic(hydrogen dopants) defects in the material. Spectroscopic ellipsometrymeasurements support this assumption. For this, we developed a dielectricdispersion model for TiO2:H thin films, which combinesthe Cody-Lorentz model with an additional Lorentz oscillator.In the as-deposited state, an additional peak of the absorption coefficientappears at 1.3-1.4 eV, which disappears for samples thermallytreated in N-2 atmosphere but is retained for samples thermallytreated in vacuum.

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