Studies of the Temperature Dependence of the Structure and Magnetism of a Hexagonal-Bipyramidal Dysprosium(III) Single-Molecule Magnet

Ding, You-Song1,2,3,4; Blackmore, William J. A.3; Zhai, Yuan-Qi1,2; Giansiracusa, Marcus J.3; Reta, Daniel3,5,6,7; Vitorica-Yrezabal, Inigo3; Winpenny, Richard E. P.3; Chilton, Nicholas F.3; Zheng, Yan-Zhen1,2

2021-12-01

10.1021/acs.inorgchem.1c02779

INORGANIC CHEMISTRY   影响因子和分区

0020-1669

1520-510X

The hexagonal-bipyramidal lanthanide(III) complex [Dy((OBu)-Bu-t)Cl(18-C-6)][BPh4] (1; 18-C-6 = 1,4,7,10,13,16-hexaoxacyclooctadecane ether) displays an energy barrier for magnetization reversal (U-eff) of ca. 1000 K in a zero direct-current field. Temperature-dependent X-ray diffraction studies of 1 down to 30 K reveal bending of the Cl-Ln-OtBu angle at low temperature. Using ab initio calculations, we show that significant bending of the O-Dy-Cl angle upon cooling from 273 to 100 K leads to a ca. 10% decrease in the energy of the excited electronic states. A thorough exploration of the temperature and field dependencies of the magnetic relaxation rate reveals that magnetic relaxation is dictated by five mechanisms in different regimes: Orbach, Raman-I, quantum tunnelling of magnetization, and Raman-II, in addition to the observation of a phonon bottleneck effect.

SCI ; EI

英语

NI期刊

其他

NSFC[21620102002,21773130,21971203,22101116] ; Key Scientific and Technological Innovation Team of Shaanxi Province[2020TD-001] ; Key Laboratory Construction Program of Xi'an Municipal Bureau of Science and Technology[201805056ZD7CG40] ; EPSRC["EP/P002560/1","EP/R011079/1"] ; European Research Council["ERC-2017-ADG-786734","ERC-2019-STG-851504"]

Chemistry

Chemistry, Inorganic & Nuclear

WOS:000736851900001

AMER CHEMICAL SOC

20220211454158

Calculations ; Dysprosium compounds ; Electronic cooling ; Magnetization reversal

Thermodynamics:641.1 ; Heat Transfer:641.2 ; Magnetism: Basic Concepts and Phenomena:701.2 ; Mathematics:921

CHEMISTRY

Web of Science

1.Xi An Jiao Tong Univ, MOE Key Lab Nonequilibrium Synth & Modulat Conden, Xian Key Lab Sustainable Energy & Mat Chem,Sch Ch, Frontier Inst Sci & Technol,State Key Lab Mech Be, Xian 710049, Peoples R China
2.Xi An Jiao Tong Univ, Sch Phys, Xian 710049, Peoples R China
3.Univ Manchester, Sch Nat Sci, Dept Chem, Manchester M13 9PL, Lancs, England
4.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
5.Euskal Herriko Unibertsitatea, Kimika Fak, Donostia, Euskadi, Peoples R China
6.Dostia Int Phys Ctr DIPC, Donostia, Euskadi, Peoples R China
7.Basque Fdn Sci, Ikerbasque, Bilbao, Spain

Ding, You-Song,Blackmore, William J. A.,Zhai, Yuan-Qi,et al. Studies of the Temperature Dependence of the Structure and Magnetism of a Hexagonal-Bipyramidal Dysprosium(III) Single-Molecule Magnet[J]. INORGANIC CHEMISTRY,2021,61:227-235.

Ding, You-Song.,Blackmore, William J. A..,Zhai, Yuan-Qi.,Giansiracusa, Marcus J..,Reta, Daniel.,...&Zheng, Yan-Zhen.(2021).Studies of the Temperature Dependence of the Structure and Magnetism of a Hexagonal-Bipyramidal Dysprosium(III) Single-Molecule Magnet.INORGANIC CHEMISTRY,61,227-235.

Ding, You-Song,et al."Studies of the Temperature Dependence of the Structure and Magnetism of a Hexagonal-Bipyramidal Dysprosium(III) Single-Molecule Magnet".INORGANIC CHEMISTRY 61(2021):227-235.