Advances in theory and computational methods for next-generation thermoelectric materials

This is a review of theoretical and methodological development over the past decade pertaining to computational characterization of thermoelectric materials from first principles. Primary focus is on electronic and thermal transport in solids. Particular attention is given to the relationships between the various methods in terms of the theoretical hierarchy as well as the tradeoff of physical accuracy and computational efficiency of each. Further covered are up-and-coming methods for modeling defect formation and dopability, keys to realizing a material's thermoelectric potential. We present and discuss all these methods in close connection with parallel developments in high-throughput infrastructure and code implementation that enable large-scale computing and materials screening. In all, it is demonstrated that advances in computational tools are now ripe for efficient and accurate targeting of the needles in the haystack, which are “next-generation” thermoelectric materials.