Henriques Alexandre, Lima Mariana S L, Nilsen Gøran J, Gutmann Matthias J, Wirth Steffen, Brito Walber H, Martelli Valentina
Institute of Physics, University of São Paulo, São Paulo, 05508-090, Brazil.
ISIS Neutron and Muon Source, Didcot, Oxfordshire, OX11 0QX, UK.
Adv Sci (Weinh). 2025 Aug;12(31):e02379. doi: 10.1002/advs.202502379. Epub 2025 Jun 4.
Unraveling the underlying mechanisms at the origin of ultra-low thermal conductivity in pristine crystals is of central relevance to designing new functional materials. Here, a study of thermal conductivity κ(T) in an extended temperature range (1.5-400 K) is reported in the single-crystalline bismuthate perovskite BaBiO. The measured κ(T) shows an anomalous glass-like behavior with a ≈ T dependence at low temperatures and a plateau in a wide temperature range from about 20 to 260 K, surprisingly recovering the expected downturn for a crystal only for T > 300 K. The measured room temperature κ ≈ 1.6 W m K agrees with the calculated value, including three-phonon and isotope disorder scattering. However, the departure of the experimental from the calculated κ(T) for T < 300 K, at the onset of the plateau, indicates that an additional scattering mechanism comes into play at lower temperatures. It is proposed that a tunneling two-level system associated with the BiO octahedra rotation offers an additional phonon scattering mechanism and may explain the observed κ(T) suppression. The findings may have significant implications for the pairing mechanism and unconventional superconductivity of doped-BaBiO aside from suggesting it as a candidate building block for functional heterostructures.
揭示原始晶体中超低热导率起源的潜在机制对于设计新型功能材料至关重要。在此,报道了在单晶铋酸盐钙钛矿BaBiO中在扩展温度范围(1.5 - 400 K)内对热导率κ(T)的研究。所测量的κ(T)在低温下呈现出异常的类玻璃行为,具有≈T依赖性,并且在约20至260 K的宽温度范围内出现平台,令人惊讶的是,仅在T > 300 K时才恢复晶体预期的下降趋势。所测量的室温κ≈1.6 W m K与计算值相符,计算中包括三声子和同位素无序散射。然而,在平台起始处,对于T < 300 K时实验κ(T)与计算值的偏差表明,在较低温度下有额外的散射机制起作用。有人提出,与BiO八面体旋转相关的隧穿双能级系统提供了一种额外的声子散射机制,并且可能解释所观察到的κ(T)抑制现象。这些发现除了表明它作为功能异质结构的候选构建块外,可能对掺杂BaBiO的配对机制和非常规超导性具有重要意义。