Uncovering design principles for amorphous-like heat conduction using two-channel lattice dynamics

Riley Hanus; Janine George; Max Wood; Alexander Bonkowski; Yongqiang Cheng; Douglas L. Abernathy; Michael E. Manley; Geoffroy Hautier; G. Jeffrey Snyder; Raphaël P. Hermann

doi:10.1016/j.mtphys.2021.100344

Uncovering design principles for amorphous-like heat conduction using two-channel lattice dynamics

Riley Hanus, Janine George, Max Wood, Alexander Bonkowski, Yongqiang Cheng, Douglas L. Abernathy, Michael E. Manley, Geoffroy Hautier, G. Jeffrey Snyder, Raphaël P. Hermann

Research output: Contribution to journal › Article › peer-review

53 Scopus citations

Abstract

The physics of heat conduction puts practical limits on many technological fields such as energy production, storage, and conversion. It is now widely appreciated that the phonon-gas model does not describe the full vibrational spectrum in amorphous materials, since this picture likely breaks down at higher frequencies. A two-channel heat conduction model, which uses harmonic vibrational states and lattice dynamics as a basis, has recently been shown to capture both crystal-like (phonon-gas channel) and amorphous-like (diffuson channel) heat conduction. While materials design principles for the phonon-gas channel are well established, similar understanding and control of the diffuson channel is lacking. In this work, in order to uncover design principles for the diffuson channel, we study structurally-complex crystalline Yb₁₄ (Mn,Mg)Sb₁₁, a champion thermoelectric material above 800 K, experimentally using inelastic neutron scattering and computationally using the two-channel lattice dynamical approach. Our results show that the diffuson channel indeed dominates in Yb₁₄MnSb₁₁ above 300 K. More importantly, we demonstrate a method for the rational design of amorphous-like heat conduction by considering the energetic proximity phonon modes and modifying them through chemical means. We show that increasing (decreasing) the mass on the Sb-site decreases (increases) the energy of these modes such that there is greater (smaller) overlap with Yb-dominated modes resulting in a higher (lower) thermal conductivity. This design strategy is exactly opposite of what is expected when the phonon-gas channel and/or common analytical models for the diffuson channel are considered, since in both cases an increase in atomic mass commonly leads to a decrease in thermal conductivity. This work demonstrates how two-channel lattice dynamics can not only quantitatively predict the relative importance of the phonon-gas and diffuson channels, but also lead to rational design strategies in materials where the diffuson channel is important.

Original language	English
Article number	100344
Journal	Materials Today Physics
Volume	18
DOIs	https://doi.org/10.1016/j.mtphys.2021.100344
State	Published - May 2021

Funding

This work was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (neutron scattering and diffuson-channel calculations). RH acknowledges the DOE Science Graduate Research Award program (2018 Solicitation 2). Inelastic neutron scattering work at the BL-18 ARCS beamline used resources at the Spallation Neutron Source, a U.S. DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. JG acknowledges funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 837910 . JG and GH furthermore thank the Consortium des Équipements de Calcul Intensif en Fédération Wallonie Bruxelles (CÉCI) for computational resources. GJS and MW acknowledge the support of award 70NANB19H005 from the U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). This work was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (neutron scattering and diffuson-channel calculations). RH acknowledges the DOE Science Graduate Research Award program (2018 Solicitation 2). Inelastic neutron scattering work at the BL-18 ARCS beamline used resources at the Spallation Neutron Source, a U.S. DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. JG acknowledges funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 837910. JG and GH furthermore thank the Consortium des Équipements de Calcul Intensif en Fédération Wallonie Bruxelles (CÉCI) for computational resources. GJS and MW acknowledge the support of award 70NANB19H005 from the U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). RH thanks Phillip B. Allen for helpful discussions surrounding the physical interpretation of simulated results and terminology. RH thanks Michele Simoncelli for correspondence regarding the computational details of the unified two-channel lattice dynamical approach.

Funders	Funder number
Consortium des Équipements de Calcul Intensif en Fédération Wallonie Bruxelles
CÉCI
U.S. Department of Energy
National Institute of Standards and Technology
U.S. Department of Commerce
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Horizon 2020 Framework Programme
H2020 Marie Skłodowska-Curie Actions	70NANB19H005, 837910
Division of Materials Sciences and Engineering
Center for Hierarchical Materials Design
Horizon 2020

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10.1016/j.mtphys.2021.100344

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title = "Uncovering design principles for amorphous-like heat conduction using two-channel lattice dynamics",

abstract = "The physics of heat conduction puts practical limits on many technological fields such as energy production, storage, and conversion. It is now widely appreciated that the phonon-gas model does not describe the full vibrational spectrum in amorphous materials, since this picture likely breaks down at higher frequencies. A two-channel heat conduction model, which uses harmonic vibrational states and lattice dynamics as a basis, has recently been shown to capture both crystal-like (phonon-gas channel) and amorphous-like (diffuson channel) heat conduction. While materials design principles for the phonon-gas channel are well established, similar understanding and control of the diffuson channel is lacking. In this work, in order to uncover design principles for the diffuson channel, we study structurally-complex crystalline Yb14 (Mn,Mg)Sb11, a champion thermoelectric material above 800 K, experimentally using inelastic neutron scattering and computationally using the two-channel lattice dynamical approach. Our results show that the diffuson channel indeed dominates in Yb14MnSb11 above 300 K. More importantly, we demonstrate a method for the rational design of amorphous-like heat conduction by considering the energetic proximity phonon modes and modifying them through chemical means. We show that increasing (decreasing) the mass on the Sb-site decreases (increases) the energy of these modes such that there is greater (smaller) overlap with Yb-dominated modes resulting in a higher (lower) thermal conductivity. This design strategy is exactly opposite of what is expected when the phonon-gas channel and/or common analytical models for the diffuson channel are considered, since in both cases an increase in atomic mass commonly leads to a decrease in thermal conductivity. This work demonstrates how two-channel lattice dynamics can not only quantitatively predict the relative importance of the phonon-gas and diffuson channels, but also lead to rational design strategies in materials where the diffuson channel is important.",

author = "Riley Hanus and Janine George and Max Wood and Alexander Bonkowski and Yongqiang Cheng and Abernathy, {Douglas L.} and Manley, {Michael E.} and Geoffroy Hautier and Snyder, {G. Jeffrey} and Hermann, {Rapha{\"e}l P.}",

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AU - George, Janine

AU - Wood, Max

AU - Bonkowski, Alexander

AU - Cheng, Yongqiang

AU - Abernathy, Douglas L.

AU - Manley, Michael E.

AU - Hautier, Geoffroy

AU - Snyder, G. Jeffrey

AU - Hermann, Raphaël P.

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AB - The physics of heat conduction puts practical limits on many technological fields such as energy production, storage, and conversion. It is now widely appreciated that the phonon-gas model does not describe the full vibrational spectrum in amorphous materials, since this picture likely breaks down at higher frequencies. A two-channel heat conduction model, which uses harmonic vibrational states and lattice dynamics as a basis, has recently been shown to capture both crystal-like (phonon-gas channel) and amorphous-like (diffuson channel) heat conduction. While materials design principles for the phonon-gas channel are well established, similar understanding and control of the diffuson channel is lacking. In this work, in order to uncover design principles for the diffuson channel, we study structurally-complex crystalline Yb14 (Mn,Mg)Sb11, a champion thermoelectric material above 800 K, experimentally using inelastic neutron scattering and computationally using the two-channel lattice dynamical approach. Our results show that the diffuson channel indeed dominates in Yb14MnSb11 above 300 K. More importantly, we demonstrate a method for the rational design of amorphous-like heat conduction by considering the energetic proximity phonon modes and modifying them through chemical means. We show that increasing (decreasing) the mass on the Sb-site decreases (increases) the energy of these modes such that there is greater (smaller) overlap with Yb-dominated modes resulting in a higher (lower) thermal conductivity. This design strategy is exactly opposite of what is expected when the phonon-gas channel and/or common analytical models for the diffuson channel are considered, since in both cases an increase in atomic mass commonly leads to a decrease in thermal conductivity. This work demonstrates how two-channel lattice dynamics can not only quantitatively predict the relative importance of the phonon-gas and diffuson channels, but also lead to rational design strategies in materials where the diffuson channel is important.

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Uncovering design principles for amorphous-like heat conduction using two-channel lattice dynamics

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