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Origin of high thermal conductivity in disentangled ultra-high molecular weight polyethylene films: ballistic phonons within enlarged crystals

Kim, Taeyong and Drakopoulos, Stavros X. and Ronca, Sara and Minnich, Austin J. (2022) Origin of high thermal conductivity in disentangled ultra-high molecular weight polyethylene films: ballistic phonons within enlarged crystals. Nature Communications, 13 . Art. No. 2452. ISSN 2041-1723. PMCID PMC9068786. doi:10.1038/s41467-022-29904-2.

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The thermal transport properties of oriented polymers are of fundamental and practical interest. High thermal conductivities ( ≳ 50 Wm⁻¹K⁻¹) have recently been reported in disentangled ultra-high molecular weight polyethylene (UHMWPE) films, considerably exceeding prior reported values for oriented films. However, conflicting explanations have been proposed for the microscopic origin of the high thermal conductivity. Here, we report a characterization of the thermal conductivity and mean free path accumulation function of disentangled UHMWPE films (draw ratio ~200) using cryogenic steady-state thermal conductivity measurements and transient grating spectroscopy. We observe a marked dependence of the thermal conductivity on grating period over temperatures from 30–300 K. Considering this observation, cryogenic bulk thermal conductivity measurements, and analysis using an anisotropic Debye model, we conclude that longitudinal atomic vibrations with mean free paths around 400 nanometers are the primary heat carriers, and that the high thermal conductivity for draw ratio ≳ 150 arises from the enlargement of extended crystals with drawing. The mean free paths appear to remain limited by the extended crystal dimensions, suggesting that the upper limit of thermal conductivity of disentangled UHMWPE films has not yet been realized.

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URLURL TypeDescription CentralArticle Paper
Kim, Taeyong0000-0003-2452-1065
Drakopoulos, Stavros X.0000-0002-6798-0790
Ronca, Sara0000-0003-3434-6352
Minnich, Austin J.0000-0002-9671-9540
Additional Information:© The Author(s) 2022. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit Received 04 January 2022; Accepted 06 April 2022; Published 04 May 2022. The authors thank Bolin Liao and Wenkai Ouyang for assistance with PPMS measurements. This work was supported by the Office of Naval Research under Grant Number N00014-18-1-2101. Data availability: The authors declare that the data supporting the findings of this study are available within the paper and its Supplementary Material files. Contributions: T.K. and A.J.M. conceived the project. S.X.D. and S.R. fabricated the samples. T.K. performed the TG and PPMS measurements and analyzed the thermal measurements data. All authors discussed the results. T.K. and A.J.M. wrote the manuscript with contributions from all authors. The authors declare no competing interests. Peer review information: Nature Communications thanks Ziqi Liang and the other anonymous reviewer(s) for their contribution to the peer review of this work. Peer review reports are available.
Funding AgencyGrant Number
Office of Naval Research (ONR)N00014-18-1-2101
Subject Keywords:Organic molecules in materials science; Polymers
PubMed Central ID:PMC9068786
Record Number:CaltechAUTHORS:20211214-190042892
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Official Citation:Kim, T., Drakopoulos, S.X., Ronca, S. et al. Origin of high thermal conductivity in disentangled ultra-high molecular weight polyethylene films: ballistic phonons within enlarged crystals. Nat Commun 13, 2452 (2022).
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112424
Deposited By: George Porter
Deposited On:15 Dec 2021 18:44
Last Modified:09 May 2022 16:31

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