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Transparent conductive oxides (TCOs) are widely-used commercially available materials for opto‐electronic applications, yet have received very little attention for dye‐sensitization applications. This paper reports that mesoporous thin films of conductive indium‐doped tin oxide (ITO) nanocrystallites support long‐lived charge separation with first‐order recombination kinetics (k = 1.5 s‐1). A layer‐by‐layer technique was utilized to spatially arrange redox and/or chromophoric molecular components on ITO. Spectro‐electrochemical measurements demonstrated that upon light absorption, each component provided a free energy gradient to direct electron transfer at the conductive oxide interface. The long‐lived nature of the photogenerated charge-separated states provide favorable conditions for photocatalytic solar fuel production. Furthermore, the first‐order recombination kinetics are most ideal for the fundamental understanding of charge separation dynamics.

Sampaio, R. N.; Troian-Gautier, L.; Meyer, G. A Charge-Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface. Angew. Chem. Int. Ed. 2018, 57 (47), 15390-15394.

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