Thermoelectric Band Engineering: The Role of Carrier Scattering

TL;DR

This paper uses first-principles calculations and advanced scattering simulations to evaluate how complex band structures and anisotropy influence thermoelectric performance, highlighting the importance of scattering mechanisms.

Contribution

It introduces a realistic assessment method combining band structure and electron-phonon scattering simulations for thermoelectric materials.

Findings

Strong intervalley scattering in silicon limits valley convergence benefits.

Band anisotropy's impact depends on scattering strength.

Convergence of valleys and bands can enhance thermoelectric efficiency.

Abstract

Complex electronic band structures, with multiple valleys or bands at the same or similar energies can be beneficial for thermoelectric performance, but the advantages can be offset by inter-valley and inter-band scattering. In this paper, we demonstrate how first-principles band structures coupled with recently developed techniques for rigorous simulation of electron-phonon scattering provide the capabilities to realistically assess the benefits and trade-offs associated with these materials. We illustrate the approach using n-type silicon as a model material and show that intervalley scattering is strong. This example shows that the convergence of valleys and bands can improve thermoelectric performance, but the magnitude of the improvement depends sensitively on the relative strengths of intra- and inter-valley electron scattering. Because anisotropy of the band structure also plays an important role, a measure of the benefit of band anisotropy in the presence of strong intervalley scattering is presented.