Transparent conductive oxides (TCOs) are widely used commercially available materials for opto-electronic applications, yet they have received very little attention for dye-sensitization applications. Now, mesoporous thin films of conductive indium-doped tin oxide (ITO) nanocrystallites are shown to 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. Spectroelectrochemical 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 interfacial charge separation dynamics.
Sampaio, R. N., Troian-Gautier, L., & Meyer, G. J. (2018). A Charge‐Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface. Angewandte Chemie, 130(47), 15616-15620. https://doi.org/10.1002/ange.201807627 (Original work published 2018)