High-Throughput Screening Delafossite CuMO2 (M = IIIA, 3d, 4d, 5d, and RE) Optoelectronic Functional Materials Based on First-Principles Calculations

To design and develop high-performance optoelectronic functional materials, the crystal structures and compositions should be fully considered. Copper-based chalcogenides as the core materials of optoelectronic applications have unique advantages and have attracted increasing attention. Among many copper (Cu)-based chalcogenides, ternary compounds of CuMO2 with delafossite structures have been used as promising candidates in many optoelectronic fields. However, there is not a comprehensive understanding of the variations of the intrinsic nature of delafossite CuMO2 compounds because of M3+-ion substitution. To solve these issues, CuMO2 (M = IIIA, 3d, 4d, 5d, and RE elements, a total number of 49) compounds are systematically analyzed by density functional theory based on a high-throughput computational platform. In the quasi-two-dimensional layered superlattice structure of the delafossite CuMO2 compound, the transport behavior of photogenerated carriers is affected mainly by the Cu hexagonal closed plane. The [CuO2] dumbbell structure and [MO6] octahedra mainly determine the generation of carriers excited by incident photons. The [CuM3O] tetrahedra that connect the other motifs mainly affect the behaviors between the generation and transport of photogenerated carriers. Furthermore, the heteroatomic interactions in the [CuM3O] tetrahedra are the decisive factors for the band gap values of delafossite CuMO2 compounds, which can be quantitatively described by the physical properties of the M component and can accurately predict the band gap value. Finally, these 49 delafossite CuMO2 compounds are classified and screened for the potential optoelectronic applications according to requirements and screening criteria of the band gap values for different optoelectronic functional applications. These calculated results will contribute to the further development of novel Cu-based optoelectronic functional materials and provide scientific support and theoretical guidance for subsequent related research.