Nested order-disorder framework containing a crystalline matrix with self-filled amorphous-like innards.

Bu, Kejun; Hu, Qingyang; Qi, Xiaohuan; Wang, Dong; Guo, Songhao; Luo, Hui; Lin, Tianquan; Guo, Xiaofeng et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

Solids can be generally categorized by their structures into crystalline and amorphous states with different interactions among atoms dictating their properties. Crystalline-amorphous hybrid structures, combining the advantages of both ordered and disordered components, present a promising opportunity to design materials with emergent collective properties. Hybridization of crystalline and amorphous structures at the sublattice level with long-range periodicity has been rarely observed. Here, we report a nested order-disorder framework (NOF) constructed by a crystalline matrix with self-filled amorphous-like innards that is obtained by using pressure to regulate the bonding hierarchy of Cu<sub>12</sub>Sb<sub>4</sub>S<sub>13</sub>. Combined in situ experimental and computational methods demonstrate the formation of disordered Cu sublattice which is embedded in the retained crystalline Cu framework. Such a NOF structure gives a low thermal conductivity (~0.24 W·m<sup>-1</sup>·K<sup>-1</sup>) and a metallic electrical conductivity (8 × 10<sup>-6</sup> Ω·m), realizing the collaborative improvement of two competing physical properties. These findings demonstrate a category of solid-state materials to link the crystalline and amorphous forms in the sublattice-scale, which will exhibit extraordinary properties.