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.
Highlights
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
For Single-molecule magnets (SMMs) to be economically viable in magnetic data storage, hysteresis should be observable at temperatures greater than that of liquid nitrogen (77 K)[2]; it has become clear that a large Ueff barrier is not the sole requirement for this to be achieved[6,7]
QTM can manifest when SMMs are adsorbed to surfaces[22], and understanding this process is crucial for commercialising SMM research; recent studies have highlighted the importance of extrinsic effects such as conduction electrons[23] and the spin-phonon coupling[24] on QTM
Summary
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.
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