Molecular magnetic hysteresis at 60 K in dysprosocenium

Conrad Goodwin, Fabrizio Ortu, Daniel Reta, Nicholas Chilton, David Mills

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    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 spins1, 2, exploiting atomic clock transitions for robust qubits3 and, most recently, magnetic data storage in single atoms4, 5. Single-molecule magnets exhibit magnetic hysteresis of molecular origin6—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 magnets7, hysteresis temperatures have increased from 4 kelvin to only about 14 kelvin8, 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 rates11, 12 (for example, 30 kelvin with 200 oersted per second)12. 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.
    Original languageEnglish
    Pages (from-to)439-442
    Early online date23 Aug 2017
    Publication statusPublished - 24 Aug 2017


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