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The thermal properties of Ba 3 Cu 2 Sn 3 Se 10 were investigated by measurement of the thermal conductivity and heat capacity. The chemical bonding in this diamagnetic material was investigated using structural data from Rietveld refinement and calculated electron localization. This quaternary chalcogenide is monoclinic ( P 2 1 / c ), has a large unit cell with 72 atoms in the primitive cell, and a high local coordination environment. The Debye temperature (162 K) and average speed of sound (1666 m s −1 ) are relatively low with a very small electronic contribution to the heat capacity. Ultralow thermal conductivity (0.46 W m −1 K −1 at room temperature) is attributed to the relatively weak chemical bonding and intrinsic anharmonicity, in addition to a large unit cell. This work is part of the continuing effort to explore quaternary chalcogenides with intrinsically low thermal conductivity and identify the features that result in a low thermal conductivity.
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Tuning network topology and vibrational mode localization to achieve ultralow thermal conductivity in amorphous chalcogenides
Abstract Amorphous chalcogenide alloys are key materials for data storage and energy scavenging applications due to their large non-linearities in optical and electrical properties as well as low vibrational thermal conductivities. Here, we report on a mechanism to suppress the thermal transport in a representative amorphous chalcogenide system, silicon telluride (SiTe), by nearly an order of magnitude via systematically tailoring the cross-linking network among the atoms. As such, we experimentally demonstrate that in fully dense amorphous SiTe the thermal conductivity can be reduced to as low as 0.10 ± 0.01 W m −1 K −1 for high tellurium content with a density nearly twice that of amorphous silicon. Using ab-initio simulations integrated with lattice dynamics, we attribute the ultralow thermal conductivity of SiTe to the suppressed contribution of extended modes of vibration, namely propagons and diffusons. This leads to a large shift in the mobility edge - a factor of five - towards lower frequency and localization of nearly 42% of the modes. This localization is the result of reductions in coordination number and a transition from over-constrained to under-constrained atomic network.
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- Award ID(s):
- 1939012
- PAR ID:
- 10316669
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41467-021-22999-z
