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

Kejun Bu, Qingyang Hu, Xiaohuan Qi, Dong Wang, Songhao Guo, Hui Luo, Tianquan Lin, Xiaofeng Guo, Qiaoshi Zeng, Yang Ding, Fuqiang Huang, Wenge Yang, Ho-Kwang Mao and Xujie Lü ()
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Kejun Bu: Center for High Pressure Science and Technology Advanced Research
Qingyang Hu: Center for High Pressure Science and Technology Advanced Research
Xiaohuan Qi: Chinese Academy of Sciences
Dong Wang: Center for High Pressure Science and Technology Advanced Research
Songhao Guo: Center for High Pressure Science and Technology Advanced Research
Hui Luo: Center for High Pressure Science and Technology Advanced Research
Tianquan Lin: Chinese Academy of Sciences
Xiaofeng Guo: Washington State University
Qiaoshi Zeng: Center for High Pressure Science and Technology Advanced Research
Yang Ding: Center for High Pressure Science and Technology Advanced Research
Fuqiang Huang: Chinese Academy of Sciences
Wenge Yang: Center for High Pressure Science and Technology Advanced Research
Ho-Kwang Mao: Center for High Pressure Science and Technology Advanced Research
Xujie Lü: Center for High Pressure Science and Technology Advanced Research

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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 Cu12Sb4S13. 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−1·K−1) and a metallic electrical conductivity (8 × 10−6 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.

Date: 2022
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DOI: 10.1038/s41467-022-32419-5

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