Abstract
The development of photosensitization strategies for titanium dioxide is necessary for the enhancement of its optical and electronic properties towards its application potential in solar photoelectrochemistry. In this work, significant differences in the photosensitizing capability of the 6th group transition metal oxides applied on the surface of titania nanotubes are reported. For the first time, correlations between the experimentally determined Tauc coefficients, sample photoresponse, and ab-initio simulated properties of the heterojunctions are established. Experimental results show undoubtedly that the decoration of TiO2 nanotubes with chromium oxides leads to the enhanced photoresponse, which originates from the interplay of mid-gap states and both direct and indirect nature of the transitions contributing to the optical absorption. The opposite tendency and decrease of photocurrent were found for molybdenum and tungsten oxides which exhibited forbidden nature of dominating transition. Although computations report intraband states in all interfaces, experimentally only chromium oxides contribute to the photocurrent. The uniqueness of this interface lies in the highest density of states in the vicinity of the conduction band and the low energy difference between the direct and indirect transitions of the innate chromium oxide. The obtained results demonstrate that the determination of the Tauc exponent and the nature of optical transition are more reliable experimental predictors of the photoactivity enhancement in the heterojunctions than the value of the band gap.
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