Castelli, Ivano Eligio1; García Lastra, Juan Maria3; Hüser, Falco5; Thygesen, Kristian Sommer6; Jacobsen, Karsten Wedel1
1 Department of Physics, Technical University of Denmark2 Theoretical Atomic-scale Physics, Department of Physics, Technical University of Denmark3 Department of Energy Conversion and Storage, Technical University of Denmark4 Atomic scale modelling and materials, Department of Energy Conversion and Storage, Technical University of Denmark5 Office for Innovation & Sector Services, Administration, Technical University of Denmark6 Center for Nanostructured Graphene, Center, Technical University of Denmark
Direct production of hydrogen from water and sunlight requires stable and abundantly available semiconductors with well positioned band edges relative to the water red-ox potentials. We have used density functional theory (DFT) calculations to investigate 300 oxides and oxynitrides in the Ruddlesden–Popper phase of the layered perovskite structure. Based on screening criteria for the stability, bandgaps and band edge positions, we suggest 20 new materials for the light harvesting photo-electrode of a one-photon water splitting device and 5 anode materials for a two-photon device with silicon as photo-cathode. In addition, we explore a simple rule relating the bandgap of the perovskite to the number of octahedra in the layered structure and the B-metal ion. Finally, the quality of the GLLB-SC potential used to obtain the bandgaps, including the derivative discontinuity, is validated against G0W0@LDA gaps for 20 previously identified oxides and oxynitrides in the cubic perovskite structure.