Assembling High-Temperature Single-Molecule Magnets with Low-Coordinate Bis(amido)Dysprosium Unit[DyN_(2)]^(+)via Cl-K-Cl Linkage  

作　　者：Chen Wang Rong Sun Yaofeng Chen Bing-Wu Wang Zhe-Ming Wang Song Gao 

机构地区：[1]Beijing National Laboratory of Molecular Science,Beijing Key Laboratory for Magnetoeletric Materials and Devices,College of Chemistry and Molecular Engineering,Peking University,Beijing 100871(China) [2]State Key Laboratory of Organometallic Chemistry,Shanghai Institute of Organic Chemistry,University of Chinese Academy of Sciences,Chinese Academy of Sciences,Shanghai 200032(China) [3]School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640(China)

出　　处：《CCS Chemistry》2020年第5期362-368,共7页中国化学会会刊（英文）

基　　金：supported by the National Natural Science Foundation of China(21971006);National Key R&D Program of China(2018YFA0306003,2017YFA0206301,and 2017YFA0204903);High-Performance Computing Platform at Peking University.

摘　　要：Symmetryandaxialityarethought tobeguides toward the pursuit of high energy barrier and blocking temperature for thedysprosium(Ⅲ)(Dy^(Ⅲ))single-molecule magnets(SMMs).The Dy^(Ⅲ)complexeswith low coordination numbers are intended to satisfy axial symmetry.Here,we report four four-coordinate Dy^(Ⅲ)SMMs based on bis(arylamido)dysprosium building block{Dy(N^(RR’))2(μ-Cl)_(2)K}(N^(RR’)={N(SiMe_(3))(C_(6)H_(3)iPr_(2)-2,6)}^(−)),with two strong Dy–N and twoweak Dy–Cl bonds.Through fine-tuning of axial anisotropy,the SMM with the largest N–Dy–N angle of 139.24(15)°displayed magnetic hysteresis with a coercive field(H_(c))of 18.6 kOe at 2 K,which kept opening up to 35 K.Alternating current susceptibility measurement showed that the relaxation energy barrier reached as high as 1578 K,which is among the highest reported Dy^(Ⅲ)SMMs.Ab initio calculations revealed strong anisotropy and crystal-field axiality of the compound,despite the low symmetry,and provided a synthetically workable approach to construct high-performance SMMs useful in applications such as digital processing,transport electronics,quantumcomputing,and ultra-high-density data storage.

关 键 词：low-coordinate strategy low symmetry bulky amido ligand magnetic anisotropy single-molecule magnets 

分 类 号：O469[理学—凝聚态物理]