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As an ultrawide bandgap (∼4.1 eV) semiconductor, single crystalline SrSnO3 (SSO) has promising electrical properties for applications in power electronics and transparent conductors. The device performance can be limited by heat dissipation issues. However, a systematic study detailing its thermal transport properties remains elusive. This work studies the temperature-dependent thermal properties of a single crystalline SSO thin film prepared with hybrid molecular beam epitaxy. By combining time-domain thermoreflectance and Debye–Callaway modeling, physical insight into thermal transport mechanisms is provided. At room temperature, the 350-nm SSO film has a thermal conductivity of 4.4 W m−1 K−1, ∼60% lower than those of other perovskite oxides (SrTiO3, BaSnO3) with the same ABO3 structural formula. This difference is attributed to the low zone-boundary frequency of SSO, resulting from its distorted orthorhombic structure with tilted octahedra. At high temperatures, the thermal conductivity of SSO decreases with temperature following a ∼T−0.54 dependence, weaker than the typical T−1 trend dominated by the Umklapp scattering. This work not only reveals the fundamental mechanisms of thermal transport in single crystalline SSO but also sheds light on the thermal design and optimization of SSO-based electronic applications.
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High frequency atomic tunneling yields ultralow and glass-like thermal conductivity in chalcogenide single crystals
Abstract Crystalline solids exhibiting glass-like thermal conductivity have attracted substantial attention both for fundamental interest and applications such as thermoelectrics. In most crystals, the competition of phonon scattering by anharmonic interactions and crystalline imperfections leads to a non-monotonic trend of thermal conductivity with temperature. Defect-free crystals that exhibit the glassy trend of low thermal conductivity with a monotonic increase with temperature are desirable because they are intrinsically thermally insulating while retaining useful properties of perfect crystals. However, this behavior is rare, and its microscopic origin remains unclear. Here, we report the observation of ultralow and glass-like thermal conductivity in a hexagonal perovskite chalcogenide single crystal, BaTiS 3 , despite its highly symmetric and simple primitive cell. Elastic and inelastic scattering measurements reveal the quantum mechanical origin of this unusual trend. A two-level atomic tunneling system exists in a shallow double-well potential of the Ti atom and is of sufficiently high frequency to scatter heat-carrying phonons up to room temperature. While atomic tunneling has been invoked to explain the low-temperature thermal conductivity of solids for decades, our study establishes the presence of sub-THz frequency tunneling systems even in high-quality, electrically insulating single crystals, leading to anomalous transport properties well above cryogenic temperatures.
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- Award ID(s):
- 1806147
- PAR ID:
- 10203338
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 11
- 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/s41467-020-19872-w
