Direct measurement of individual phonon lifetimes in the clathrate compound Ba7.81Ge40.67Au5.33

Pierre-François Lory, Stéphane Pailhès (), Valentina M. Giordano, Holger Euchner, Hong Duong Nguyen, Reiner Ramlau, Horst Borrmann, Marcus Schmidt, Michael Baitinger, Matthias Ikeda, Petr Tomeš, Marek Mihalkovič, Céline Allio, Mark Robert Johnson, Helmut Schober, Yvan Sidis, Frédéric Bourdarot, Louis Pierre Regnault, Jacques Ollivier, Silke Paschen, Yuri Grin and Marc Boissieu ()
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Pierre-François Lory: Institut Laue-Langevin
Stéphane Pailhès: University Lyon, University Claude Bernard Lyon 1, CNRS, Institute of Light and Matter
Valentina M. Giordano: University Lyon, University Claude Bernard Lyon 1, CNRS, Institute of Light and Matter
Holger Euchner: Vienna University of Technology
Hong Duong Nguyen: Max-Planck-Institut für Chemische Physik fester Stoffe
Reiner Ramlau: Max-Planck-Institut für Chemische Physik fester Stoffe
Horst Borrmann: Max-Planck-Institut für Chemische Physik fester Stoffe
Marcus Schmidt: Max-Planck-Institut für Chemische Physik fester Stoffe
Michael Baitinger: Max-Planck-Institut für Chemische Physik fester Stoffe
Matthias Ikeda: Vienna University of Technology
Petr Tomeš: Vienna University of Technology
Marek Mihalkovič: Slovak Academy of Sciences
Céline Allio: Goethe-University
Mark Robert Johnson: Institut Laue-Langevin
Helmut Schober: Institut Laue-Langevin
Yvan Sidis: Laboratoire Léon Brillouin, CNRS, CEA, UMR-12
Frédéric Bourdarot: University Grenoble Alpes, CEA, INAC
Louis Pierre Regnault: University Grenoble Alpes, CEA, INAC
Jacques Ollivier: Institut Laue-Langevin
Silke Paschen: Vienna University of Technology
Yuri Grin: Max-Planck-Institut für Chemische Physik fester Stoffe
Marc Boissieu: University Grenoble Alpes, CNRS, Grenoble-INP, SIMaP

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Engineering lattice thermal conductivity requires to control the heat carried by atomic vibration waves, the phonons. The key parameter for quantifying it is the phonon lifetime, limiting the travelling distance, whose determination is however at the limits of instrumental capabilities. Here, we show the achievement of a direct quantitative measurement of phonon lifetimes in a single crystal of the clathrate Ba7.81Ge40.67Au5.33, renowned for its puzzling ‘glass-like’ thermal conductivity. Surprisingly, thermal transport is dominated by acoustic phonons with long lifetimes, travelling over distances of 10 to 100 nm as their wave-vector goes from 0.3 to 0.1 Å−1. Considering only low-energy acoustic phonons, and their observed lifetime, leads to a calculated thermal conductivity very close to the experimental one. Our results challenge the current picture of thermal transport in clathrates, underlining the inability of state-of-the-art simulations to reproduce the experimental data, thus representing a crucial experimental input for theoretical developments.

Date: 2017
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DOI: 10.1038/s41467-017-00584-7

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