Calculated thermoelectric properties of La-filled skutterudites

TL;DR

This paper investigates the electronic structures of La-filled skutterudites using first-principles calculations to understand their thermoelectric properties, highlighting the role of band structure and doping in optimizing thermoelectric performance.

Contribution

It provides a detailed first-principles analysis of La-filled skutterudites' electronic structures and their impact on thermoelectric properties, emphasizing the influence of band behavior and doping.

Findings

Near rigid band behavior with Co doping

Presence of flat transition metal bands affecting thermopower

Optimal thermoelectric properties linked to doping levels

Abstract

The thermoelectric properties of La-filled skutterudites are discussed from the point of view of their electronic structures. These are calculated from first principles within the local density approximation. The electronic structure is in turn used to determine transport related quantities. Virtual crystal calculations for La(Fe,Co)_4Sb_{12} show that the system obeys near rigid band behavior with varying Co concentration, and has a substantial band gap at a position corresponding to the composition LaFe_3% CoSb_{12}. The valence band maximum occurs at the $\Gamma$ point and is due to a singly degenerate dispersive band, which by itself would not be favorable for high thermopower. However, very flat transition metal derived bands occur in close proximity and become active as the doping level is increased, giving a non-trivial dependence of the properties on carrier concentration and explaining the favorable thermoelectric properties.