The evolution of chemical ordering and property in Fe1+xSe2 upon intercalation ratios

作     者：Zijing Zhao Xiaocang Han Shengcai Zhu Zhi Fang Ziyi Han Zhongyu Liang Bailing Li Biao Zhang Wei Li Zhaochu Luo Licong Peng Xiaoxu Zhao Xiangguo Li Jiadong Zhou Song Gao Chengxin Wang Mathias Kl?ui Yanglong Hou Zijing Zhao;Xiaocang Han;Shengcai Zhu;Zhi Fang;Ziyi Han;Zhongyu Liang;Bailing Li;Biao Zhang;Wei Li;Zhaochu Luo;Licong Peng;Xiaoxu Zhao;Xiangguo Li;Jiadong Zhou;Song Gao;Chengxin Wang;Mathias Kläui;Yanglong Hou

作者机构：School of Materials Science and Engineering Beijing Key Laboratory for Magnetoelectric Materials and DevicesPeking University School of MaterialsShenzhen Campus of Sun Yat-sen University School of Physics and Optoelectronic Engineering Beijing University of Technology State Key Laboratory for Artificial Microstructure&Mesoscopic PhysicsSchool of PhysicsPeking University Key Lab of Advanced Optoelectronic Quantum Architecture and Measurement(MOE) School of Physics Beijing Institute of Technology School of ChemistrySun Yat-sen University School of Materials Science and Engineering Sun Yat-sen University Institute of Physics Johannes Gutenberg University Mainz 

出 版 物：《National Science Review》 (国家科学评论(英文版))

年 卷 期：2025年第12卷第2期

页      面：165-176页

核心收录：

学科分类：08[工学] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Key Research and Development Program of China (2022YFA1204003 and 2022YFA1203902) the National Natural Science Foundation of China (92263203, 52027801 and 52301300) the China-Germany Collaboration Project (M-0199) 

主　　题：intercalation Fe-intercalated 2D materials room-temperature magnetism 

摘      要：Intercalation has been considered as an effective method to explore innovative two-dimensional（2D）materials and modify their properties. However, the relationship between intercalation concentration,structure, and property remains a largely uncharted territory, and the controllable synthesis of desired intercalated phases faces challenges. Here, a general intercalated rule for the effect of self-intercalation ratio on atomic arrangements is revealed. Then, the controllable synthesis of a series of Fe-intercalated 2D materials is realized. Scanning transmission electron microscopy illustrates that their intercalation structures undergo disordered/ordered/half-ordered/ordered transformation, which confirms the intercalated rule and proposes a new structure termed half-ordered intercalation. Notably, their magnetic and electrical properties can be significantly modulated by intercalation. Orderly intercalated nanoflakes possess room-temperature magnetism with composition-regulated magnetic domains. Moreover, Fe1.5Se2and Fe1.6Se2are scarce half-metallic materials showing different magneto-resistance behaviors. This work would guide the design and synthesis of new intercalated materials, and deepen the understanding of the relationship between structure and properties.