Enrico Di Lucente^1*, Michele Simoncelli², Nicola Marzari^1,3

1 Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, Lausanne 1015, Switzerland

2 TCM Group, Cavendish Laboratory, University of Cambridge, 19 JJ Thomson Avenue, Cambridge, CB3 0HE, United Kingdom

3 Laboratory for Materials Simulations, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland

* Corresponding authors emails: enrico.dilucente@epfl.ch

DOI10.24435/materialscloud:xn-qr [version v1]

Publication date: Jan 05, 2024

How to cite this record

Enrico Di Lucente, Michele Simoncelli, Nicola Marzari, Crossover from Boltzmann to Wigner thermal transport in thermoelectric skutterudites, Materials Cloud Archive 2024.1 (2024), https://doi.org/10.24435/materialscloud:xn-qr

Description

Skutterudites are crystals with a cagelike structure that can be augmented with filler atoms (“rattlers”), usually leading to a reduction in thermal conductivity that can be exploited for thermoelectric applications. Here, we leverage the recently introduced Wigner formulation of thermal transport to elucidate the microscopic physics underlying heat conduction in skutterudites, showing that filler atoms can drive a crossover from the Boltzmann to the Wigner regimes of thermal transport, i.e., from particlelike conduction to wavelike tunneling. At temperatures where the thermoelectric efficiency of skutterudites is largest, wavelike tunneling can become comparable to particlelike propagation. We define a Boltzmann deviation descriptor able to differentiate the two regimes and relate the competition between the two mechanisms to the materials' chemistry, providing a design strategy to select rattlers and identify optimal compositions for thermoelectric applications.

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Keywords

Thermal conductivity Phonons Thermoelectrics MARVEL