Quantum Condensed Matter Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
Nat Nanotechnol. 2013 Jun;8(6):445-51. doi: 10.1038/nnano.2013.95. Epub 2013 Jun 2.
Materials with very low thermal conductivity are of great interest for both thermoelectric and optical phase-change applications. Synthetic nanostructuring is most promising for suppressing thermal conductivity through phonon scattering, but challenges remain in producing bulk samples. In crystalline AgSbTe2 we show that a spontaneously forming nanostructure leads to a suppression of thermal conductivity to a glass-like level. Our mapping of the phonon mean free paths provides a novel bottom-up microscopic account of thermal conductivity and also reveals intrinsic anisotropies associated with the nanostructure. Ground-state degeneracy in AgSbTe2 leads to the natural formation of nanoscale domains with different orderings on the cation sublattice, and correlated atomic displacements, which efficiently scatter phonons. This mechanism is general and suggests a new avenue for the nanoscale engineering of materials to achieve low thermal conductivities for efficient thermoelectric converters and phase-change memory devices.
具有极低热导率的材料在热电和光学相变应用中都具有很大的兴趣。通过声子散射来抑制热导率,合成纳米结构是最有前途的方法,但在生产块状样品方面仍存在挑战。在晶态 AgSbTe2 中,我们表明自发形成的纳米结构导致热导率降至玻璃态水平。我们对声子平均自由程的映射提供了热导率的一种新颖的自下而上的微观解释,也揭示了与纳米结构相关的固有各向异性。AgSbTe2 的基态简并导致在阳离子亚晶格上具有不同有序性的纳米尺度畴的自然形成,以及相关的原子位移,这些都有效地散射声子。这种机制是普遍的,为通过纳米尺度工程来实现高效热电转换器和相变存储器件的低热导率提供了一种新途径。