Zhang Peikun, Xue Minmin, Chen Changfeng, Guo Wanlin, Zhang Zhuhua
State Key Laboratory of Mechanics and Control for Aerospace Structures, Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education, and Institute for Frontier Science, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
Department of Physics and Astronomy, University of Nevada, Las Vegas, Nevada 89154, United States.
Nano Lett. 2023 Apr 26;23(8):3623-3629. doi: 10.1021/acs.nanolett.3c00827. Epub 2023 Apr 12.
Recent experimental breakthrough demonstrated a powerful synthesis approach for intercalating the van der Waals gap of layered materials to achieve property modulation, thereby opening an avenue for exploring new physics and devising novel applications, but the mechanism governing intercalant assembly patterns and properties remains unclear. Based on extensive structural search and energetics analysis by calculations, we reveal a Sabatier-like principle that dictates spatial arrangement of self-intercalated atoms in transition metal dichalcogenides. We further construct a robust descriptor quantifying that strong intercalant-host interactions favor a monodispersing phase of intercalated atoms that may exhibit ferromagnetism, while weak interactions lead to a trimer phase with attenuated or quenched magnetism, which further evolves into tetramer and hexagonal phases at increasing intercalant density. These findings elucidate the mechanism underpinning experimental observations and paves the way for rational design and precise control of self-intercalation in layered materials.
最近的实验突破展示了一种强大的合成方法，用于插入层状材料的范德华间隙以实现性能调制，从而为探索新物理和设计新应用开辟了一条途径，但控制插层剂组装模式和性能的机制仍不清楚。基于大量的结构搜索和计算能量学分析，我们揭示了一种类似萨巴蒂尔原理，它决定了过渡金属二硫属化物中自插层原子的空间排列。我们进一步构建了一个稳健的描述符，量化了强插层剂 - 主体相互作用有利于插层原子的单分散相，该相可能表现出铁磁性，而弱相互作用导致具有减弱或淬灭磁性的三聚体相，随着插层剂密度的增加，该相进一步演变为四聚体和六方相。这些发现阐明了支撑实验观察结果的机制，并为层状材料中自插层的合理设计和精确控制铺平了道路。
