Discarded gems: Thermoelectric performance of materials with band gap emerging at the hybrid-functional level

TL;DR

This study uses hybrid functional calculations to identify materials with previously underestimated band gaps that could have promising thermoelectric properties, highlighting the importance of accurate electronic structure methods.

Contribution

The paper demonstrates that hybrid functional calculations can reveal finite band gaps in materials previously predicted as metallic by standard DFT, uncovering new thermoelectric candidates.

Findings

Eight compounds with emergent band gaps identified

MgSc2 Hg and Li2 CaSi show promising thermoelectric properties

Reassessment of band gaps can discover new thermoelectric materials

Abstract

A finite electronic band gap is a standard filter in high-throughput screening of materials using density functional theory (DFT). However, because of the systematic underestimation of band gaps in standard DFT approximations, a number of compounds may incorrectly be predicted metallic. In a more accurate treatment, such materials may instead appear as low band gap materials and could e.g. have good thermoelectric properties if suitable doping is feasible. To explore this possibility, we performed hybrid functional calculations on 1093 cubic materials listed in the MaterialsProjects database with four atoms in the primitive unit cell, spin-neutral ground state, and a formation energy within 0.3 eV of the convex hull. Out of these materials, we identified eight compounds for which a finite band gap emerges. Evaluating electronic and thermal transport properties of these compounds, we found the compositions MgSc2 Hg and Li2 CaSi to exhibit promising thermoelectric properties. These findings underline the potential of reassessing band gaps and band structures of compounds to indentify additional potential thermoelectric materials.