Enhancing Magnetic Hysteresis in Single-Molecule Magnets by Ligand Functionalization

Ke-xin Yu, Jon G.c. Kragskow, You-song Ding, Yuan-qi Zhai, Daniel Reta, Nicholas F. Chilton, Yan-zhen Zheng

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102 Citations (SciVal)


Design criteria for dysprosium(III) single-molecule magnets (SMMs) with large thermal energy barriers to magnetic reversal have been established and proven, and the challenge to enhance performance is in understanding and controlling electron-vibration coupling that is the origin of magnetic reversal. We have prepared an SMM, [Dy(L)2(py)5][BPh4] 1 (HL = (S)-(-)-1-phenylethanol), based on the archetype [Dy(OtBu)2(py)5][BPh4] 2. Compounds 1 and 2 have similarly large energy barriers of Ueff = 1,130(20) cm−1 and Ueff = 1,250(10) cm−1, and yet 1 shows magnetic hysteresis at a far higher temperature of 22 K cf. TH = 4 K for 2. Ab initio calculation of the electron-vibration coupling and spin dynamics shows that substitution of the alkoxide ligand in fact enhances relaxation over the energy barrier for 1 compared with 2, in agreement with experiment, and that the higher temperature of magnetic hysteresis likely owes to reduced quantum tunneling at low temperatures.
Original languageEnglish
Pages (from-to)1777-1793
Issue number7
Publication statusPublished - 28 May 2020
Externally publishedYes

Bibliographical note

We acknowledge the Natural Science Foundation of China (21620102002 and
21773130), Xi’an Municipal Bureau of Science and Technology (201805056ZD7CG40), Cyrus Chung Ying Tang Foundation, State Key Laboratory for Mechanical Behavior of Materials, the Fundamental Research Funds for the Central Universities (P.R.C.), EPSRC (U.K., EP/P002560/1), and the University of Manchester for funding and support. We also thank the Instrument Analysis Centre of Xi’an Jiaotong University for the measurement on dilution ratio and the Computational Shared Facility at The University of Manchester. K.-X.Y. thanks the China Scholarship Council for a research scholarship and N.F.C. thanks the University of Manchester for a Presidential Fellowship and the Royal Society for a University Research Fellowship. We thank Prof. Richard Winpenny and Dr David
Mills for useful discussions


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