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

Anharmonicity in Thermal Insulators: An Analysis from First Principles