Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet.pdf (939.03 kB)
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Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet.

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journal contribution
posted on 05.06.2019, 08:49 by Y-S Ding, K-X Yu, D Reta, F Ortu, REP Winpenny, Y-Z Zheng, NF Chilton
Understanding quantum tunnelling of the magnetisation (QTM) in single-molecule magnets (SMMs) is crucial for improving performance and achieving molecule-based information storage above liquid nitrogen temperatures. Here, through a field- and temperature-dependent study of the magnetisation dynamics of [Dy(tBuO)Cl(THF)5][BPh4]·2THF, we elucidate the different relaxation processes: field-independent Orbach and Raman mechanisms dominate at high temperatures, a single-phonon direct process dominates at low temperatures and fields >1 kOe, and a field- and temperature-dependent QTM process operates near zero field. Accounting for the exponential temperature dependence of the phonon collision rate in the QTM process, we model the magnetisation dynamics over 11 orders of magnitude and find a QTM tunnelling gap on the order of 10-4 to 10-5 cm-1. We show that removal of Dy nuclear spins does not suppress QTM, and argue that while internal dipolar fields and hyperfine coupling support QTM, it is the dynamic crystal field that drives efficient QTM.


This work was supported by the EPSRC (EP/P002560/1), the Ramsay Memorial Trust (fellowship to N.F.C.), The University of Manchester, the NSFC (nos. 21473129, 21620102002 and 21773130), “National Young 1000-Plan” program, State Key Laboratory for Mechanical Behaviour of Materials, the Fundamental Research Funds for the Central Universities and the Cyrus Chung Ying Tang Foundation.



Nat Commun, 2018, 9 (1), 3134

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/Organisation/COLLEGE OF SCIENCE AND ENGINEERING/Department of Chemistry


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CCDC 1450752 (1), and 1566471 (2) contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via (or from the Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: (+44)1223- 336-033; or Magnetic data is available from N.F.C. on request.



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