Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.161
Publication date: 6th July 2018
Cu(I)-based delafossites (CuMO2) have garnered significant attention for their small optical bandgaps, strong light absorption characteristics, and native p-type conductivities, which make them suitable photocathode candidates for solar fuel production. While resolving the inherently complex electronic structures of these ternary oxides is often challenging, doing so is imperative for understanding optical excitations and carrier transport mechanisms, as well as for furthering material design and discovery. Combining density functional theory (DFT) calculations and X-ray spectroscopy techniques, this research gives a detailed portrait of the band structure of rhombohedral 3R-CuFeO2, prepared by reactive co-sputtering. In particular, element-specific contributions from 3d orbitals of Fe and Cu, as well as 2p orbitals of O, in the valence and conduction bands are revealed by resonant inelastic X-ray scattering (RIXS) measurement. By combining this knowledge of electronic structure, with measurements of optical properties, carrier relaxation dynamics, and photoelectrochemical performance characteristics, this research provides insights into current limitations of this novel photocathode material and informs strategies to overcome them.
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