Inverse Band Structure Design via Materials Database Screening: Application to Square Planar Thermoelectrics

Electronic band structure contains a wealth of information on the electronic properties of a solid and is routinely computed. However, the more difficult problem of designing a solid with a desired band structure is an outstanding challenge. In order to address this inverse band structure design problem, we devise an approach using materials database screening with materials attributes based on the constituent elements, nominal electron count, crystal structure, and thermodynamics. Our strategy is tested in the context of thermoelectric materials, for which a targeted band structure containing both flat and dispersive components with respect to crystal momentum is highly desirable. We screen for thermodynamically stable or metastable compounds containing <i>d</i>⁸ transition metals coordinated by anions in a square planar geometry in order to mimic the properties of recently identified oxide thermoelectrics with such a band structure. In doing so, we identify 157 compounds out of a total of more than half a million candidates. After further screening based on electronic band gap and structural anisotropy, we explicitly compute the band structures for the several of the candidates in order to validate the approach. We successfully find two new oxide systems that achieve the targeted band structure. Electronic transport calculations on these two compounds, Ba₂PdO₃ and La₄PdO₇, confirm promising thermoelectric power factor behavior for the compounds. This methodology is easily adapted to other targeted band structures and should be widely applicable to a variety of design problems