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Controlling Magnetic Anisotropy in a Zero-Dimensional S=1 Magnet Using Isotropic Cation Substitution

Manson, JL; Curley, SPM; Williams, RC; Walker, D; Goddard, PA; Ozarowski, A; Johnson, RD; ... Singleton, J; + view all (2021) Controlling Magnetic Anisotropy in a Zero-Dimensional S=1 Magnet Using Isotropic Cation Substitution. Journal of the American Chemical Society , 143 (12) pp. 4633-4638. 10.1021/jacs.0c12516. Green open access

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Abstract

The [Zn_{1–x}_Ni-{x}(HF_{2})(pyz)_{2}]SbF_{6} (x = 0.2; pyz = pyrazine) solid solution exhibits a zero-field splitting (D) that is 22% larger [D = 16.2(2) K (11.3(2) cm^{–1})] than that observed in the x = 1 material [D = 13.3(1) K (9.2(1) cm^{–1)}]. The substantial change in D is accomplished by an anisotropic lattice expansion in the MN_{4} (M = Zn or Ni) plane, wherein the increased concentration of isotropic Zn(II) ions induces a nonlinear variation in M-F and M-N bond lengths. In this, we exploit the relative donor atom hardness, where M-F and M-N form strong ionic and weak coordinate covalent bonds, respectively, the latter being more sensitive to substitution of Ni by the slightly larger Zn(II) ion. In this way, we are able to tune the single-ion anisotropy of a magnetic lattice site by Zn-substitution on nearby sites. This effect has possible applications in the field of single-ion magnets and the design of other molecule-based magnetic systems.

Type: Article
Title: Controlling Magnetic Anisotropy in a Zero-Dimensional S=1 Magnet Using Isotropic Cation Substitution
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/jacs.0c12516
Publisher version: https://doi.org/10.1021/jacs.0c12516
Language: English
Additional information: © 2021 The Authors. Published by American Chemical Society under a Creative Commons license (https://creativecommons.org/licenses/by-nc-nd/4.0/).
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/10125922
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