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.
In this study, a numerical simulation method and analytical models for predicting the boundary scattering mean free path (MFP) of phonons in polycrystalline nanostructures are developed. The grain morphologies are assumed to be approximately equiaxed, i.e., forbidding needle-like or pancake-like morphologies. Adapting a technique from rarefied gas dynamics, the method evaluates the MFP from the mean square displacements of phonons that experience random motion and interface collisions in nanostructures. We confirm that the MFP in simple cubic polycrystalline nanostructures obtained by the simulations agrees with that reported in a previous study; this result supports the validity of the method. Two analytical models for high and low interfacial transmission probabilities at the crystal interfaces are also derived by considering the mean square displacements. We find that the grain-boundary intercept length distribution of polycrystalline structures is an essential parameter for determining this boundary scattering MFP. These analytical models reproduce the MFPs in simple cubic and Voronoi diagram polycrystalline nanostructures calculated by the numerical simulations. This result indicates that the boundary scattering MFP of phonons in polycrystalline nanostructures can be obtained once the intercept length distribution is evaluated, without any additional numerical simulations.
more » « less- PAR ID:
- 10372800
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- Journal of Applied Physics
- Volume:
- 132
- Issue:
- 13
- ISSN:
- 0021-8979
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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