论文标题

热绝缘子的非谐性:第一原理的分析

Anharmonicity in Thermal Insulators: An Analysis from First Principles

论文作者

Knoop, Florian, Purcell, Thomas A. R., Scheffler, Matthias, Carbogno, Christian

论文摘要

原子运动的非谐性限制了晶体固体中的热导率。然而,缺乏对在强热绝缘体中活跃的机制的微观理解。在这封信中,我们对465个实验性的材料进行了针对其非谐调性的实验性材料,并对其中58个进行了完全过度的绿色kubo计算,找到了28个具有$κ<10 $ w/mk的热绝缘子,包括6张UltraLow $κ\κ\ Lessim 1 $ W/mk。我们的分析表明,潜在的强性无谐动力学是由元稳定的内在缺陷几何形状的探索驱动的。这与常用的扰动方法有所不同,其中假定动力学围绕单个稳定的几何形状发展。

The anharmonicity of atomic motion limits the thermal conductivity in crystalline solids. However, a microscopic understanding of the mechanisms active in strong thermal insulators is lacking. In this letter, we classify 465 experimentally known materials with respect to their anharmonicity and perform fully anharmonic ab initio Green-Kubo calculations for 58 of them, finding 28 thermal insulators with $κ< 10$ W/mK including 6 with ultralow $κ\lesssim 1$ W/mK. Our analysis reveals that the underlying strong anharmonic dynamics is driven by the exploration of meta-stable intrinsic defect geometries. This is at variance with the frequently applied perturbative approach, in which the dynamics is assumed to evolve around a single stable geometry.

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