Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.195
Publication date: 18th July 2023
Development of efficient photoelectrochemical (PEC) systems for solar fuel production requires a detailed understanding of loss mechanisms that limit performance under device operation. This often proves a challenge as many PEC devices are reliant on semiconductor materials whose optoelectronic and catalytic properties are poorly understood. Spatial collection efficiency (SCE) analysis has recently been introduced as a non-destructive analytical technique to probe the spatial distribution of charge carrier collection with nanometer resolution in photoelectrodes under operating conditions, requiring only external quantum efficiency measurements and knowledge of the device optical parameters. I will demonstrate how the technique can be used to gain insight into the optoelectronic properties of emergent photoelectrode materials including quantification of i) charge carrier transport lengths and ii) excitation-wavelength dependent charge carrier localization losses, the latter of which we have found to ultimately limit the performance of several open d-shell metal-oxide photoelectrode candidates. Additionally, current techniques used to extract SCE profiles are suitable for PEC devices containing only a single active layer deposited on a current collector, which are generally not representative of practical devices. To this end, I will discuss our efforts at implementing a new numerical approach to SCE analysis which allows for characterization of losses in multilayer photoelectrodes containing selective transport layers, thereby providing a tool for quantitative characterization of losses in practical photoelectrode devices under operating conditions.