Room-temperature ferrimagnetism and size-modulated electronic structures in two-dimensional cluster-based metal-organic frameworks  

作　　者：Jing Cheng Xingxing Li Jinlong Yang 

机构地区：[1]Key Laboratory of Precision and Intelligent Chemistry,University of Science and Technology of China,Hefei 230026,China [2]Department of Chemical Physics,University of Science and Technology of China,Hefei 230026,China [3]Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,China [4]Hefei National Laboratory,University of Science and Technology of China,Hefei 230088,China

出　　处：《Science China Chemistry》2024年第4期1334-1340,共7页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(22288201,22273092,22322304);the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450101);the Youth Innovation Promotion Association CAS(2019441);the Innovation Program for Quantum Science and Technology(2021ZD0303306);USTC Tang Scholar。

摘　　要：Cluster-assembled materials have attracted particular attention for their complex hierarchical structures and unique properties.However,the majority of cluster-based assemblies developed so far are either non-magnetic or only exhibit magnetic ordering with a relatively low Curie temperature,limiting their applications in spintronics.Thus,two-dimensional(2D)cluster-assembled materials with room-temperature magnetism remain highly desirable.For this purpose,based on first principles calculations,we design a series of thermodynamically stable 2D cluster-based metal-organic frameworks(MOFs)Fe_(n)-(pyz)(n=1-6)by utilizing Fenmetal clusters as nodes and nitrogen-containing pyrazine ligands as organic linkers.These 2D cluster-based MOFs exhibit robust ferrimagnetic ordering due to the strong d-p direct exchange interaction between d-electron spin of Fe_(n)(n=1-6)clusters and charge transfer-induced p-electron spin of pyrazine ligands.In particular,the ferrimagnetic Curie temperatures are well above room temperature(up to 836 K).Additionally,altering the size of Fe_(n)clusters in Fe_(n)-(pyz)(n=1-6)MOFs results in diverse functional spintronic properties,including bipolar magnetic semiconductors,half semiconductors and Dirac half metals.Moreover,these 2D assembled MOFs possess sizable magnetic anisotropy energies,up to 9.16 me V per formula.

关 键 词：metal-organic framework two-dimensional material half metal bipolar magnetic semiconductor MAGNET 

分 类 号：O641.4[理学—物理化学]