Molecular magnetic hysteresis at 60 kelvin in dysprosocenium

• Published in: Nature (London) 2017-08, Vol.548 (7668), p.439-442
• Main Authors: Goodwin, Conrad A. P., Ortu, Fabrizio, Reta, Daniel, Chilton, Nicholas F., Mills, David P.
• Format: Article
• Language: English
• Subjects: 119/118; 140/131; 140/133; 639/638/440; 639/638/911/406; 639/766/94; Data processing; Data storage; High temperature; Humanities and Social Sciences; Hysteresis; Information processing; Lanthanides; letter; Ligands; Liquid nitrogen; Magnetic fields; Magnetic hysteresis; Magnetic induction; Magnetic relaxation; Magnets; multidisciplinary; Physics research; Quantum phenomena; Qubits (quantum computing); Rare earth metals; Science; Spin dynamics; Temperature; Temperature effects; Vibrations
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/nature23447

Magnetic hysteresis is observed in a dysprosocenium complex at temperatures of up to 60 kelvin, the origin of which is the localized metal–ligand vibrational modes unique to dysprosocenium. Molecular memories heat up The discovery of molecules that exhibit magnetic bistability raised hopes for the use of such molecular systems as tiny building blocks for magnetic data storage. Despite a quarter of a century of research, however, the temperatures at which these molecules display their desirable magnetic properties remain frustratingly low. Conrad Goodwin et al . report the synthesis and characterization of a molecular dysprosocenium complex that shows magnetic bistability up to 60 kelvin—tantalizingly close to liquid nitrogen temperatures, the point at which applications would start to become a realistic possibility. 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 1 , 2 , exploiting atomic clock transitions for robust qubits 3 and, most recently, magnetic data storage in single atoms 4 , 5 . Single-molecule magnets exhibit magnetic hysteresis of molecular origin 6 —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 7 , hysteresis temperatures have increased from 4 kelvin to only about 14 kelvin 8 , 9 , 10 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 11 , 12 (for example, 30 kelvin with 200 oersted per second) 12 . Here we report a hexa- tert -butyldysprosocenium complex—[Dy(Cp ttt ) 2 ][B(C 6 F 5 ) 4 ], with Cp ttt  = {C 5 H 2 t Bu 3 -1,2,4} and t Bu = C(CH 3 ) 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 indic