Please use this identifier to cite or link to this item: http://hdl.handle.net/2381/44277
Title: Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet.
Authors: Ding, Y-S
Yu, K-X
Reta, D
Ortu, F
Winpenny, REP
Zheng, Y-Z
Chilton, NF
First Published: 7-Aug-2018
Publisher: Nature Research (part of Springer Nature)
Citation: Nat Commun, 2018, 9 (1), 3134
Abstract: 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.
DOI Link: 10.1038/s41467-018-05587-6
eISSN: 2041-1723
Links: https://www.nature.com/articles/s41467-018-05587-6
http://hdl.handle.net/2381/44277
Version: Publisher Version
Status: Peer-reviewed
Type: Journal Article
Rights: Copyright © the authors, 2018. This is an open-access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.
Description: CCDC 1450752 (1), and 1566471 (2) contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/conts/retrieving.html (or from the Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: (+44)1223- 336-033; or deposit@ccdc.cam.ac.uk). Magnetic data is available from N.F.C. on request.
Appears in Collections:Published Articles, Dept. of Chemistry

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