Strategic Optimization of the Electronic Transport Properties of Pseudo-Ternary Clathrates
Journal article, 2021

While alloying is a powerful handle for materials engineering, it is an ongoing challenge to navigate the large and complex parameter space of these materials. This applies in particular for thermoelectrics and even more so clathrates. Here, a combination of density functional theory calculations, alloy cluster expansions, Monte Carlo simulations, and Boltzmann transport theory calculations is used to identify compositions that yield high power factors in the pseudo-ternary clathrates Ba8AlxGayGe46−x−y and Ba8GaxGeySi46−x−y, while accounting for weight and raw material costs. The results show how a cost-efficient performance can be achieved by reducing the number of Al and Ga atoms per unit cell, while compensating the resulting increase in the carrier concentration via an extrinsic dopant. The approach used in this study is transferable and can be a useful tool for mapping the thermodynamic and transport properties of other multinary systems.

clathrate

Monte Carlo

cluster expansion

chemical ordering

transport properties

thermoelectrics

power factor

Author

Joakim Brorsson

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Applied Surface Chemistry

Anders Palmqvist

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Applied Surface Chemistry

Paul Erhart

Chalmers, Physics, Condensed Matter and Materials Theory

Advanced Electronic Materials

2199-160X (ISSN)

Vol. In Press

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Swedish Research Council (VR) (2020-04935), 2020-12-01 -- 2024-11-30.

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Subject Categories

Inorganic Chemistry

Other Engineering and Technologies not elsewhere specified

Other Physics Topics

DOI

10.1002/aelm.202100756

More information

Latest update

11/29/2021