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The effect of doped ions on single-molecule magnets of the Mn_(12)-Ac family

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Chinese Physics B 2008年第11期17卷 4318-4322页

作者：张俊荣何伦华曹慧波王芳卫张泮霖 State Key Laboratory of Magnetism Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of Sciences Laboratoire Léon Brillouin CEA-CNRS CE-Saclay 91191 Gif-sur-Yvette France

This paper investigates the single-molecule magnets of pure and Cr/Fe-doped Mn12-Ac. The components of the mixed crystals are identified by AC susceptibility technique. The ground-state spin and anisotropy parameters of doped Mn12-Ac are obtained：（i） MnllCr-Ac （S=19/2, D=0.62K, B=0.0009K, A=63K）, and （ii） Mn11Fe-Ac （S=21/2, D=0.39 K, B=0.001 K, △=55 K）. The single-ion origin of the magnetic anisotropy is discussed.

关键词： single-molecule magnets magnetic anisotropy macroscopic quantum tunnelling

Enhancing blocking temperature using inverse hydrogen bonds for non-radical bridged dimeric Dy(Ⅲ)single-molecule magnets

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Science China Chemistry 2024年第10期67卷 3328-3338页

作者： Peng-Bo Jin Qian-Cheng Luo Ye-Ye Liu Yan-Zhen Zheng Frontier Institute of Science and Technology State Key Laboratory of Electrical Insulation and Power EquipmentMOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed MatterXi’an Key Laboratory of Electronic Devices and Material Chemistry and School of ChemistryXi’an Jiaotong UniversityXi’an 710054China

single-molecule magnets(SMMs)are a kind of nanosized magnetic materials that are capable of storing massive bytes of *** coupling the spin centers in a proper manner is a usual approach to promote the working temperature(or blocking temperature)for *** delocalized radicals have been widely employed to accomplish this ***,we show a new manner by using weak but multiple B–H^(δ-)···Dy^(3+)inverse hydrogen bonding(IHB)interactions to control the magnetic couplings in a series of dimeric dysprosiacaborane *** approach leads to a record high T_(B)^(100s)of 10 K among non-radical bridged dimeric SMMs,which is mainly ascribed to strong ferromagnetic coupling(4.38 cm^(-1))and the proper alignment of the magnetic principle axes of the adjacent dysprosium(Ⅲ)*** verifying by theoretical calculations,these results demonstrate that IHB interactions can be used to construct strong axial ferromagnetic coupling and enhancing magnetic blocking temperature for SMMs.

关键词： single-molecule magnets carborane dysprosium ferromagnetic coupling inverse hydrogen bond

Chelating Guanidinates for Dysprosium(Ⅲ) single-molecule magnets

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Chinese Journal of Chemistry 2021年第6期39卷 1635-1640页

作者： Peng-Bo Jin Ke-Xin Yu Yuan-Qi Zhai Qian-Cheng Luo Yi-Dian Wang Xu-Feng Zhang Yi Lv Yan-Zhen Zheng Xi'an Jiaotong University Shenzhen Research School Frontier Institute of Science and Technology(FIST)State Key Laboratory of Mechanical Behavior for MaterialsMOE Key Laboratory for Nonequilibrium Synthesis of Condensed MatterXi’an Key Laboratory of Sustainable Energy and Materials ChemistrySchool of Physics and School of ChemistryXi’an Jiaotong University99 Yanxiang RoadXi’anShaanxi 710054China Department of Hepatobiliary Surgery The First Affiliated Hospital of Xi'an Jiootong University277 West Yanta RoadXi'anShaanxi 710061China

Two chelating guanidinate-based dysprosium(Ⅲ)complexes,namely the monomeric{(Me_(3)Si)_(2)NC(N^(i)Pr)_(2)}_(2)Dy(μ-CI)_(2)Li(THF)_(2) 1 and the dimeric[{(Me_(3)Si)_(2)NC(N^(i)Pr)_(2)}_(2)Dy(μ-CI)]_(2) 2,have been confirmed to be single-molecule ***,the alteration from 1 to 2 leads to an obvious mitigated quantum tunnelling of magnetization at zero field of the hysteresis loop and much enhanced magnetic relaxation barrier(up to 312 K).5%dilution with the yttrium(Ⅲ)analogue for 2 shows no clear change for the hysteresis,indicating the single-ion nature of the magnetic behavior.

关键词： Guanidinate ligand Magnetic properties Lanthanides single-molecule magnets Ab initio calculations

Structures and magnetic relaxation properties of cyclopentadienyl/β-diketonate/trispyrazolylborate hybridized dysprosium single-molecule magnets

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Chinese Chemical Letters 2023年第8期34卷 467-471页

作者： Lu Zhang Jin Xiong Yin-Shan Meng Tao Liu State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116024China Department of Chemistry Carnegie Mellon UniversityPittsburghPA 15213United States

The combination of cyclopentadiene,β-diketonate and tripyrazoylborate ligands with dysprosium ion afforded five mononuclear compounds:[(Cp)2Dy(Tp∗)](1Dy),[(Cp)Dy(Tp∗)Cl(THF)](2Dy),[(Cp)Dy(Tp)Cl(THF)](3Dy),[(DBM)Dy(Tp)Cl(THF)](4Dy),[{(Tp)Dy(DBM)_(2)(H_(2)O)}·THF](5Dy)(Cp=cyclopentadiene;Tp∗=hydrotris(3,5-dimethyl-1-pyrazolyl)borate;Tp=hydrotris(1-pyrazolyl)borate;DBM=dibenzoylmethanoate).Magnetic study revealed that 1Dy and 3Dy exhibited typical butterfly-type *** susceptibility study combined with ab initio calculations indicated that the magnetic relaxation behaviors of 1Dy–4Dy were governed by the Orbach and Raman processes under applied DC ***,3Dy showed two-step magnetic relaxation,which was attributed to the static disordering of the coordinated THF *** anisotropy analysis indicated that it was the relative strength of the interactions between DyIII and surrounding ligands that determined the orientation of the magnetic easy axis.

关键词： single-molecule magnets Lanthanide complexes Magnetic anisotropy Magnetic relaxations Quantum tunneling of magnetization

Switching the coordination geometry to enhance erbium(Ⅲ)single-molecule magnets

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Chinese Chemical Letters 2023年第5期34卷 535-538页

作者： Qian-Cheng Luo Ning Ge Yuan-Qi Zhai Tengbo Wang Lin Sun Qi Sun Fanni Li Zhendong Fu Yan-Zhen Zheng Frontier Institute of Science and Technology School of Chemistry and School of PhysicsXi'an Jiaotong UniversityXi'an 710054China The School of Automation Science and Technology Xi'an Jiaotong UniversityXi'an 712000China Institute of Molecular and Crystal Engineering College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China Department of General Surgery The First Affiliated Hospital of Xi'an Jiaotong UniversityXi'an 710061China Department of Talent Highland The First Affiliated Hospital of Xi'an Jiaotong UniversityXi'an 710061China Neutron Platform Songshan Lake Materials LaboratoryDongguan 523808China

Two erbium(Ⅲ)complexes[ErCl(OAr^(Ad))_(3)][Na(THF)_(6)](1)and Er(OAr^(Ad))_(3)(2)are successfully prepared by using one variety of"hard"base ligand with large steric *** coordination geometry around the Er(Ⅲ)site changes from distorted tetrahedral to flat trigonal pyramid geometry in different solvent environment due to the removal of the coordinated *** an alternation significantly enhances the single-molecule magnet(SMM)behavior and makes the field-induced effective energy barrier(Ueff)arrive at 43(1)cm-1for the *** with theoretical calculations,this study shows that strong equatorial ligand field and high local symmetry are critical to suppress the quantum tunneling of the magnetization(QTM)and achieve high-performance erbium(Ⅲ)based SMMs.

关键词： single-molecule magnets Erbium Lanthanide complexes Magnetic anisotropy Slow magnetic relaxation

Frequency-domain terahertz transmission spectra of Mn_3 and Mn_(12) single-molecule magnets

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Science China(Physics,Mechanics & Astronomy) 2012年第7期55卷 1245-1248页

作者： LIU RuiYuan ZUO JunWei LI YanRong ZHOU YuRong WANG YunPing Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesP.O.Box 603Beijing 100190China

Frequency-domain terahertz transmission spectra of Mn3 and Mn12 single molecule magnets （SMMs） have been measured at different temperatures, and hence the anisotropic parameters O2 and D4 of the spin Hamiltonian H = D2Sz^2 ＋ D4Sz^4 have been calculated. For Mn12 SMM, D2=-10.9 GHz and D4=-2.59×10^-2 GHz, while for Mn3 SMM, D2=-22.0 GHz and D4 can be con- sidered negligible. This suggests Mn3 SMM can be considered as a simpler and more suitable candidate for magnetic quantum tunneling research.

关键词： terahertz single-molecule magnets transmission

Tuning Magnetic Relaxation in Square-Pyramidal Dysprosium single-molecule magnets Using Apical Alkoxide Ligands

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CCS Chemistry 2021年第12期3卷 388-398页

作者： Zhenhua Zhu Yi-Quan Zhang Xiao-Lei Li Mei Guo Jingjing Lu Shuting Liu Richard A.Layfield Jinkui Tang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 University of Chinese Academy of Sciences Beijing 100049 Jiangsu Key Lab for NSLSCS School of Physical Science and TechnologyNanjing Normal UniversityNanjing 210023 University of Science and Technology of China Hefei 230026 Department of Chemistry School of Life SciencesUniversity of SussexBrighton BN19QR

Eight square-pyramidal dysprosium complexes of the type[Dy(X)(DBP)_(2){TMG(H)}_(2)]were synthesized,where TMG(H)denotes 1,1,3,3-tetramethylguanidine,X denotes an alkoxide ligand or anionic guanidinate in the apical position,and DBP denotes 2,*** complexes,expressed as 5-Dy-X,are single-molecule magnets(SMMs)with properties dependent on the nature of the apical X ligand.

关键词： single-molecule magnets dysprosium magnetic relaxation energy barrier twocoordination design

Assembling High-Temperature single-molecule magnets with Low-Coordinate Bis(amido)Dysprosium Unit[DyN_(2)]^(+)via Cl-K-Cl Linkage

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CCS Chemistry 2020年第5期2卷 362-368页

作者： Chen Wang Rong Sun Yaofeng Chen Bing-Wu Wang Zhe-Ming Wang Song Gao Beijing National Laboratory of Molecular Science Beijing Key Laboratory for Magnetoeletric Materials and DevicesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871(China) State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032(China) School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640(China)

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 ***,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 *** 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 *** current susceptibility measurement showed that the relaxation energy barrier reached as high as 1578 K,which is among the highest reported Dy^(Ⅲ)*** 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

Magnetic Interactions Switching in Two Dinuclear Dy（Ⅲ） single-molecule magnets via Subtle Structural Distortion

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Magnetic Interactions Switching in Two Dinuclear Dy（Ⅲ） Si...