Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.091
Publication date: 11th July 2022
Transition metal-oxides are promising photoelectrode materials for photoelectrochemical water splitting and solar fuel conversion. Several materials with empty or filled d-shell configurations (e.g. TiO2, BiVO4) have shown high internal quantum efficiencies, but their band gaps are too large for practical purposes. Metal-oxides with suitable bandgaps generally have open d-shell configurations and suffer from poor photoconversion efficiencies. We have recently introduced spatial collection efficiency analysis, based on optical and external quantum efficiency measurements, as a non-destructive method to probe losses in thin film semiconductor photoelectrodes under operando conditions. [1,2,3] Using hematite as a case study for strongly correlated electron materials, we show that in addition to the well-known recombination losses arising from poor charge transport properties, some of the photon absorption leads to localized excited states rather than to generation of mobile electrons and holes that contribute to the photocurrent. We extract the wavelength-dependent mobile charge carrier photogeneration yield spectrum of hematite and show that it is less than unity across the entire absorption range, fundamentally limiting the attainable photocurrent to roughly half that predicted based on above bandgap absorption. I will discuss our recent advancements on this front, and the implications of our findings on photoconversion efficiency in open d-shell transition metal-oxides.
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