Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.230
Publication date: 6th July 2018
Unassisted water splitting by this approach requires efficient, stable and low-cost photoelectrode materials. Of the material candidates for photocathodes, Cu2O stands out as best performing oxide for hydrogen production currently available. Although numerous experimental investigations greatly enhanced performance and stability of Cu2O photocathode, there is lack of detailed theoretical understanding of charge
transport mechanism in Cu2O buried junction photocathodes. On the macroscopic scale within the drift-diffusion approximation of charge transport in semiconductors, device simulation studies so far studied Cu2O photovoltaics. The charge transport in photoelectrochemical Cu2O buried junctions has not been addressed so far by device simulation study.
In our work, we discuss existing belief that separation of the valence band of p-type Cu2O to conduction band of n-type buffer layer limits the available photovoltage, providing example calculation with Al:ZnO buffer layer, which does not follow this rule. To explain the measured low photovoltage obtained with Al:ZnO buffer layer, we identify recombination at defect-rich Al:ZnO/Cu2O interface as a responsible mechanism. Furthermore, our device simulations of onset voltage of TiO2/Ga2O3/Cu2O photocathode correspond well with the measured value. We describe how the two energy barriers for electron transport at Cu2O/Ga2O3 and at TiO2/Ga2O3 interfaces cause anodic shift of the onset voltage. Numerical quantification of the drift and diffusion currents throughout the TiO2/Ga2O3/Cu2O photocathode brings us to conclusion that electron diffusion in Cu2O bulk close to Cu2O/Ga2O3 dominates the electron current at the onset voltage. Variation of electron affinity, mobility and doping of Ga2O3 buffer layer in our model result in important improvements on onset voltage up to 1.65 V vs RHE and ratiometric power-saved of the Cu2O photocathode, providing future ideas for experimental developments.
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