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      Thickness‐Dependent Thermal Conductivity and Phonon Mean Free Path Distribution in Single‐Crystalline Barium Titanate

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          Abstract

          Nanosized perovskite ferroelectrics are widely employed in several electromechanical, photonics, and thermoelectric applications. Scaling of ferroelectric materials entails a severe reduction in the lattice (phonon) thermal conductivity, particularly at sub‐100 nm length scales. Such thermal conductivity reduction can be accurately predicted using the information of phonon mean free path (MFP) distribution. The current understanding of phonon MFP distribution in perovskite ferroelectrics is still inconclusive despite the critical thermal management implications. Here, high‐quality single‐crystalline barium titanate (BTO) thin films, a representative perovskite ferroelectric material, are grown at several thicknesses. Using experimental thermal conductivity measurements and first‐principles based modeling (including four‐phonon scattering), the phonon MFP distribution is determined in BTO. The simulation results agree with the measured thickness‐dependent thermal conductivity. The results show that the phonons with sub‐100 nm MFP dominate the thermal transport in BTO, and phonons with MFP exceeding 10 nm contribute ≈35% to the total thermal conductivity, in significant contrast to previously published experimental results. The experimentally validated phonon MFP distribution is consistent with the theoretical predictions of other complex crystals with strong anharmonicity. This work paves the way for thermal management in nanostructured and ferroelectric‐domain‐engineered systems for oxide perovskite‐based functional materials.

          Abstract

          High‐quality single‐crystalline barium titanate thin films are grown. The results show that the phonons with sub‐100 nm mean free path dominate the thermal transport in barium titanate, and phonons with mean free path exceeding 10 nm contribute ≈35% to the total thermal conductivity, in significant contrast to previously published experimental results.

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          arXiv: 2209.12720, v2

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            Author and article information

            Contributors
            hu@sc.edu
            jliu38@ncsu.edu
            Journal
            Adv Sci (Weinh)
            Adv Sci (Weinh)
            10.1002/(ISSN)2198-3844
            ADVS
            Advanced Science
            John Wiley and Sons Inc. (Hoboken )
            2198-3844
            24 April 2023
            July 2023
            : 10
            : 19 ( doiID: 10.1002/advs.v10.19 )
            : 2301273
            Affiliations
            [ 1 ] Department of Mechanical and Aerospace Engineering North Carolina State University Raleigh NC 27695 USA
            [ 2 ] Department of Mechanical Engineering University of South Carolina Columbia SC 29208 USA
            [ 3 ] Department of Physics North Carolina State University Raleigh NC 27695 USA
            Author notes
            Author information
            https://orcid.org/0000-0002-7335-5860
            Article
            ADVS5631
            10.1002/advs.202301273
            10323618
            37092575
            8b6571c8-3864-4252-b974-3e14052b8348
            © 2023 The Authors. Advanced Science published by Wiley‐VCH GmbH

            This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

            History
            : 29 March 2023
            : 24 February 2023
            Page count
            Figures: 8, Tables: 0, Pages: 10, Words: 7306
            Funding
            Funded by: National Science Foundation , doi 10.13039/100000001;
            Award ID: 2011978
            Award ID: 2030128
            Award ID: ECCS‐2025064
            Award ID: DMR‐1726294
            Funded by: Office of the Vice President for Research at the University of South Carolina
            Award ID: 80005046
            Funded by: U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences
            Award ID: DE‐SC0020992
            Funded by: North Carolina
            Categories
            Research Article
            Research Articles
            Custom metadata
            2.0
            July 6, 2023
            Converter:WILEY_ML3GV2_TO_JATSPMC version:6.3.1 mode:remove_FC converted:06.07.2023

            ferroelectric,mean free path,oxide perovskite,phonon,thermal conductivity

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