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Enhancing Magnetic Hysteresis in Single-Molecule Magnets by Ligand Functionalisation

85 Pages Posted: 20 Nov 2019 Sneak Peek Status: Under Review

See all articles by Ke-Xin Yu

Ke-Xin Yu

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology

Jon G. C. Kragskow

University of Manchester - Department of Chemistry

You-Song Ding

University of Manchester - Department of Chemistry; Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology

Yuan-Qi Zhai

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology

Daniel Reta

University of Manchester - Department of Chemistry

Nicholas Chilton

University of Manchester - Department of Chemistry

Yan-Zhen Zheng

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology

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Abstract

The design criteria for single-molecule magnets (SMMs) of dysprosium(III) to show large thermal energy barriers to magnetic reversal have been established and proven, and the challenge to enhance their performance is understanding and control of vibrational modes that govern slow relaxation. We have prepared a new SMM, [Dy(L)2(py)5][BPh4] 1 (where HL = (S)-(-)-1-phenylethanol), which is based on the archetype [Dy(OtBu)2(py)5][BPh4] 2. Compounds 1 and 2 have similarly large energy barriers of Ueff = 1130(20) cm-1 and Ueff = 1250(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 spin dynamics show that substitution of the alkoxide ligand in fact enhances relaxation over the energy barrier for 1 over 2, in agreement with experiment, and that the higher temperature of magnetic hysteresis owes to reduced quantum tunnelling at low temperatures.

Keywords: Molecular Magnetism, Memory, Spin Dynamics, Coordination Chemistry, Vibronic Coupling

Suggested Citation

Yu, Ke-Xin and Kragskow, Jon G. C. and Ding, You-Song and Zhai, Yuan-Qi and Reta, Daniel and Chilton, Nicholas and Zheng, Yan-Zhen, Enhancing Magnetic Hysteresis in Single-Molecule Magnets by Ligand Functionalisation (November 11, 2019). CHEMJOURNAL-D-19-01184. Available at SSRN: https://ssrn.com/abstract=3485162 or http://dx.doi.org/10.2139/ssrn.3485162
This is a paper under consideration at Cell Press and has not been peer-reviewed.

Ke-Xin Yu

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology ( email )

China

Jon G. C. Kragskow

University of Manchester - Department of Chemistry ( email )

United Kingdom

You-Song Ding

University of Manchester - Department of Chemistry ( email )

United Kingdom

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology ( email )

China

Yuan-Qi Zhai

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology ( email )

China

Daniel Reta

University of Manchester - Department of Chemistry ( email )

United Kingdom

Nicholas Chilton (Contact Author)

University of Manchester - Department of Chemistry

United Kingdom

Yan-Zhen Zheng

Xi'an Jiaotong University (XJTU) - Frontier Institute of Science and Technology ( email )

China

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