Bipolar conduction asymmetries lead to ultra-high thermoelectric power factor

TL;DR

This paper demonstrates that strong conduction-valence band asymmetries in low band gap thermoelectric materials can significantly enhance power factors and ZT, with implications for material design and discovery.

Contribution

It reveals how bipolar conduction asymmetries can be exploited to achieve ultra-high thermoelectric power factors and develops descriptors for machine learning identification of such materials.

Findings

Enhanced power factors surpass unipolar limits.

Doubling of ZT figure of merit achieved.

Descriptors for rapid material screening developed.

Abstract

Low band gap thermoelectric materials suffer from bipolar effects at high temperatures, with increased electronic thermal conductivity and reduced Seebeck coefficient, leading to reduced power factor and low ZT figure of merit. In this work we show that the presence of strong transport asymmetries between the conduction and valence bands can allow high phonon-limited electronic conductivity at finite Seebeck coefficient values, leading to largely enhanced power factors. The power factors that can be achieved can be significantly larger compared to their maximum unipolar counterparts, allowing for doubling of the ZT figure of merit. We identify this behavior in low band gap cases from the half-Heusler materials family. Using both, advanced electronic Boltzmann transport calculations for realistic material bandstructures, as well as model parabolic electronic bands, we elaborate on the parameters that determine this effect. We then develop a series of descriptors which can guide machine learning studies in identifying such classes of materials with extraordinary power factors at nearly pristine conditions. For this we test more than 3000 analytical bandstructures and their features, and more than 120 possible descriptors, to identify the most promising ones that contain: i) only band structure features for easy identification from material databases, and ii) band structure and transport parameters that provide much higher correlations, but for which parameter availability can be somewhat scarce.