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      Magnetic Slow Relaxation in a Metal-Organic Framework Made of Chains of Ferromagnetically Coupled Single-Molecule Magnets

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          Lanthanide double-decker complexes functioning as magnets at the single-molecular level.

          Double-decker phthalocyanine complexes with Tb3+ or Dy3+ showed slow magnetization relaxation as a single-molecular property. The temperature ranges in which the behavior was observed were far higher than that of the transition-metal-cluster single-molecule magnets (SMMs). The significant temperature rise results from a mechanism in the relaxation process different from that in the transition-metal-cluster SMMs. The effective energy barrier for reversal of the magnetic moment is determined by the ligand field around a lanthanide ion, which gives the lowest degenerate substate a large |Jz| value and large energy separations from the rest of the substates in the ground-state multiplets.
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            Lanthanide single-molecule magnets.

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              Molecular magnetic hysteresis at 60 kelvin in dysprosocenium

              Lanthanides have been investigated extensively for potential applications in quantum information processing and high-density data storage at the molecular and atomic scale. Experimental achievements include reading and manipulating single nuclear spins, exploiting atomic clock transitions for robust qubits and, most recently, magnetic data storage in single atoms. Single-molecule magnets exhibit magnetic hysteresis of molecular origin—a magnetic memory effect and a prerequisite of data storage—and so far lanthanide examples have exhibited this phenomenon at the highest temperatures. However, in the nearly 25 years since the discovery of single-molecule magnets, hysteresis temperatures have increased from 4 kelvin to only about 14 kelvin using a consistent magnetic field sweep rate of about 20 oersted per second, although higher temperatures have been achieved by using very fast sweep rates (for example, 30 kelvin with 200 oersted per second). Here we report a hexa-tert-butyldysprosocenium complex—[Dy(Cpttt)2][B(C6F5)4], with Cpttt = {C5H2tBu3-1,2,4} and tBu = C(CH3)3—which exhibits magnetic hysteresis at temperatures of up to 60 kelvin at a sweep rate of 22 oersted per second. We observe a clear change in the relaxation dynamics at this temperature, which persists in magnetically diluted samples, suggesting that the origin of the hysteresis is the localized metal–ligand vibrational modes that are unique to dysprosocenium. Ab initio calculations of spin dynamics demonstrate that magnetic relaxation at high temperatures is due to local molecular vibrations. These results indicate that, with judicious molecular design, magnetic data storage in single molecules at temperatures above liquid nitrogen should be possible.
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                Author and article information

                Journal
                Chemistry - A European Journal
                Chem. Eur. J.
                Wiley
                09476539
                May 11 2018
                May 11 2018
                March 24 2018
                : 24
                : 27
                : 6983-6991
                Affiliations
                [1 ]Univ. Rennes, INSA Rennes, CNRS; ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226; 35000 Rennes France
                [2 ]Univ. Rennes, CNRS; ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226; 35000 Rennes France
                [3 ]Laboratory of Molecular Magnetism (LaMM); Università degli studi di Firenze, INSTM unit; Via della lastruccia 3 50019 Sesto Fiorentino Italy
                [4 ]LCPM-Groupe “Matériaux Inorganiques: Chimie Douce et Cristallographie”; Université Assane Seck de Ziguinchor; BP 523 Ziguinchor Sénégal
                Article
                10.1002/chem.201800095
                29436739
                65408449-6a17-4f88-9067-8cce0eeb31a0
                © 2018

                http://doi.wiley.com/10.1002/tdm_license_1.1

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