New Light-Harvesting Materials Using Accurate and Efficient Bandgap Calculations

Electronic bandgap calculations are presented for 2400 experimentally known materials from the Materials Project database and the bandgaps, obtained with different types of functionals within density functional theory and (partial) self‐consistent GW approximation, are compared for 20 randomly chosen compounds forming an unconventional set of ternary and quaternary materials. It is shown that the computationally cheap GLLB‐SC potential gives results in good agreement (around 15%) with the more advanced and demanding eigenvalue‐self‐consistent GW. This allows for a high‐throughput screening of materials for different applications where the bandgaps are used as descriptors for the efficiency of a photoelectrochemical device. Here, new light harvesting materials are proposed to be used in a one‐photon photoelectrochemical device for water splitting by combining the estimation of the bandgaps with the stability analysis using Pourbaix diagrams and with the evaluation of the position of the band edges. Using this methodology, 25 candidate materials are obtained and 5 of them appear to have a realistic possibility of being used as photocatalyst in a one‐photon water splitting device. The bandgaps of 2400 experimentally known materials from the Materials Project database are calculated using density functional theory. New light‐harvesting materials are proposed that may be used in a one‐photon photoelectrochemical device for water splitting. This is investigated by combining the estimation of the bandgaps with the stability analysis using Pourbaix diagrams and the evaluation of the position of the band edges.