Glass-like thermal conductivity and phonon transport mechanism in disordered crystals
Solid materials with ultra-low thermal conductivity (κ) are of great interest in thermoelectrics for energy conversion or as thermal barrier coatings for thermal insulation. Many low-κ materials exhibit unique properties, such as weak or even insignificant dependence on temperature (T) for κ, i.e., an anomalous glass-like behavior. However, a comprehensive theoretical model elucidating the microscopic phonon mechanism responsible for the glass-like κ-T relationship is still absent. Herein, we take rare-earth tantalates (RE3TaO7) as examples to reexamine phonon thermal transport in defective crystals. By combining experimental studies and atomistic simulations up to 1800 K, we revealed that diffusion-like phonons related to inhomogeneous interatomic bonding contribute more than 70% to the total κ, overturning the conventional understanding that low-frequency phonons dominate heat transport. Furthermore, due to the bridging effects of interatomic bonding, the κ of high-entropy tantalates is not necessarily lower than that of medium-entropy materials, suggesting that attempts to reduce κ through high-entropy engineering are limited, at least in defective fluorite tantalates. The new physical mechanism of multimodal phonon thermal transport in defective structures demonstrated in this work provides a reference for the analysis of phonon transport and offers a new strategy to develop and design low-κ materials by regulating the inhomogeneity of interatomic bonding.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:11 |
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| Enthalten in: |
Materials horizons - 11(2024), 6 vom: 18. März, Seite 1567-1578 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Ren, Guoliang [VerfasserIn] |
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| Links: |
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| Anmerkungen: |
Date Revised 18.03.2024 published: Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1039/d3mh01681a |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM367555212 |
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| 520 | |a Solid materials with ultra-low thermal conductivity (κ) are of great interest in thermoelectrics for energy conversion or as thermal barrier coatings for thermal insulation. Many low-κ materials exhibit unique properties, such as weak or even insignificant dependence on temperature (T) for κ, i.e., an anomalous glass-like behavior. However, a comprehensive theoretical model elucidating the microscopic phonon mechanism responsible for the glass-like κ-T relationship is still absent. Herein, we take rare-earth tantalates (RE3TaO7) as examples to reexamine phonon thermal transport in defective crystals. By combining experimental studies and atomistic simulations up to 1800 K, we revealed that diffusion-like phonons related to inhomogeneous interatomic bonding contribute more than 70% to the total κ, overturning the conventional understanding that low-frequency phonons dominate heat transport. Furthermore, due to the bridging effects of interatomic bonding, the κ of high-entropy tantalates is not necessarily lower than that of medium-entropy materials, suggesting that attempts to reduce κ through high-entropy engineering are limited, at least in defective fluorite tantalates. The new physical mechanism of multimodal phonon thermal transport in defective structures demonstrated in this work provides a reference for the analysis of phonon transport and offers a new strategy to develop and design low-κ materials by regulating the inhomogeneity of interatomic bonding | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Che, Junwei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Hanchao |e verfasserin |4 aut | |
| 700 | 1 | |a Yu, Yali |e verfasserin |4 aut | |
| 700 | 1 | |a Hao, Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Yinchun |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Fan |e verfasserin |4 aut | |
| 700 | 1 | |a Zhao, Xiaofeng |e verfasserin |4 aut | |
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