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

Negi, Ankit; Rodriguez, Alejandro; Zhang, Xuanyi; Comstock, Andrew H.; Yang, Cong; Sun, Dali; Jiang, Xiaoning; Kumah, Divine; Hu, Ming; Liu, Jun

doi:10.1002/advs.202301273

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

Journal Article · Mon Apr 24 00:00:00 EDT 2023 · Advanced Science

DOI:https://doi.org/10.1002/advs.202301273· OSTI ID:2350565

Negi, Ankit ^[1]; Rodriguez, Alejandro ^[2]; Zhang, Xuanyi ^[3]; Comstock, Andrew H. ^[3]; Yang, Cong ^[3]; Sun, Dali ^[3]; Jiang, Xiaoning ^[3]; Kumah, Divine ^[3]; Hu, Ming ^[2]; ^[3]

North Carolina State University, Raleigh, NC (United States); North Carolina State University
Univ. of South Carolina, Columbia, SC (United States)
North Carolina State University, Raleigh, NC (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: North Carolina State University, Raleigh, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0020992

OSTI ID:: 2350565

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 19 Vol. 10; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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

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