Cis-trans isomerism modulates the magnetic relaxation of dysprosium single-molecule magnets

被引:140
作者
Wu, Jianfeng [1 ,3 ]
Jung, Julie [2 ]
Zhang, Peng [1 ]
Zhang, Haixia [1 ]
Tang, Jinkui [1 ]
Le Guennic, Boris [2 ]
机构
[1] Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Peoples R China
[2] Univ Rennes 1, CNRS, UMR 6226, Inst Sci Chim Rennes, 263 Ave Gen Leclerc, F-35042 Rennes, France
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
SPIN-LATTICE-RELAXATION; DY-III; ION MAGNET; ANISOTROPY; COMPLEXES; BARRIERS; BLOCKING; HYSTERESIS; EXCHANGE; MEMORY;
D O I
10.1039/c5sc04510j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Geometry and magnetic relaxation modulations in a series of mononuclear dysprosium complexes, [DyLz(2)(o-vanilin)(2)]center dot X center dot solvent (Lz = 6-pyridin-2-yl-[1,3,5]triazine-2,4-diamine; X = Br- (1), NO3- (2), CF3SO3- (3)), were realized by changing the nature of the counter-anion. The Dy-III ions in all complexes are eight-coordinate and in approximate D-4d symmetry environments. The magnetic relaxation and anisotropy of these complexes were systematically investigated, both experimentally and from ab initio calculations. All complexes exhibit excellent single-molecule magnetic behavior. Remarkably, magneto-structural studies show that the rotation of the coordinating plane of the square-antiprismatic environment in complex 2 induces a magnetic relaxation path through higher excited states, yielding a high anisotropy barrier of 615 K (696 K for a diluted sample). Additionally, obvious opening of the hysteresis loop is observed up to 7 K, which is the highest blocking temperature ever reported for dysprosium single-molecule magnets.
引用
收藏
页码:3632 / 3639
页数:8
相关论文
共 53 条
[1]   Mononuclear lanthanide single-molecule magnets based on polyoxometalates [J].
AlDamen, Murad A. ;
Clemente-Juan, Juan M. ;
Coronado, Eugenio ;
Marti-Gastaldo, Carlos ;
Gaita-Arino, Alejandro .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (28) :8874-+
[2]   Cholesky decomposition-based multiconfiguration second-order perturbation theory (CD-CASPT2):: Application to the spin-state energetics of CoIII(diiminato)(NPh) [J].
Aquilante, Francesco ;
Malmqvist, Per-Ake ;
Pedersen, Thomas Bondo ;
Ghosh, Abhik ;
Roos, Bjoern Olof .
JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2008, 4 (05) :694-702
[3]   Software News and Update MOLCAS 7: The Next Generation [J].
Aquilante, Francesco ;
De Vico, Luca ;
Ferre, Nicolas ;
Ghigo, Giovanni ;
Malmqvist, Per-Ake ;
Neogrady, Pavel ;
Pedersen, Thomas Bondo ;
Pitonak, Michal ;
Reiher, Markus ;
Roos, Bjorn O. ;
Serrano-Andres, Luis ;
Urban, Miroslav ;
Veryazov, Valera ;
Lindh, Roland .
JOURNAL OF COMPUTATIONAL CHEMISTRY, 2010, 31 (01) :224-247
[4]   Reduced anionic Mn12 molecules with half-integer ground states as single-molecule magnets [J].
Aubin, SMJ ;
Sun, ZM ;
Pardi, L ;
Krzystek, J ;
Folting, K ;
Brunel, LC ;
Rheingold, AL ;
Christou, G ;
Hendrickson, DN .
INORGANIC CHEMISTRY, 1999, 38 (23) :5329-5340
[5]   Capping Ligand Perturbed Slow Magnetic Relaxation in Dysprosium Single-Ion Magnets [J].
Bi, Ye ;
Guo, Yun-Nan ;
Zhao, Lang ;
Guo, Yang ;
Lin, Shuang-Yan ;
Jiang, Shang-Da ;
Tang, Jinkui ;
Wang, Bing-Wu ;
Gao, Song .
CHEMISTRY-A EUROPEAN JOURNAL, 2011, 17 (44) :12476-12481
[6]  
Blagg RJ, 2013, NAT CHEM, V5, P673, DOI [10.1038/nchem.1707, 10.1038/NCHEM.1707]
[7]   Single Pyramid Magnets: Dy5 Pyramids with Slow Magnetic Relaxation to 40 K [J].
Blagg, Robin J. ;
Muryn, Christopher A. ;
McInnes, Eric J. L. ;
Tuna, Floriana ;
Winpenny, Richard E. P. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (29) :6530-6533
[8]  
Boudreaux E.A., 1976, Theory and Applications of Molecular Paramagnetism
[9]   THE SYNTHESIS OF CERTAIN SUBSTITUTED 1,3,5-TRIAZINES CONTAINING THE FERROIN GROUP [J].
CASE, FH ;
KOFT, E .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1959, 81 (04) :905-906
[10]   Enhancing Anisotropy Barriers of Dysprosium(III) Single-Ion Magnets [J].
Chen, Gong-Jun ;
Guo, Yun-Nan ;
Tian, Jin-Lei ;
Tang, Jinkui ;
Gu, Wen ;
Liu, Xin ;
Yan, Shi-Ping ;
Cheng, Peng ;
Liao, Dai-Zheng .
CHEMISTRY-A EUROPEAN JOURNAL, 2012, 18 (09) :2484-2487