Investigating complex magnetic anisotropy in a Co(II) molecular compound: a charge density and correlated ab initio electronic structure study

Damgaard-Møller, E., Krause, L., Lassen, H., Malaspina, L. A., Grabowsky, S., Bamberger, H., McGuire, J., Miras, H. N. , Sproules, S. and Overgaard, J. (2020) Investigating complex magnetic anisotropy in a Co(II) molecular compound: a charge density and correlated ab initio electronic structure study. Inorganic Chemistry, 59(18), pp. 13190-13200. (doi: 10.1021/acs.inorgchem.0c01489) (PMID:32869986)

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Abstract

Understanding magnetic anisotropy and specifically how to tailor it is crucial in the search for high-temperature single-ion magnets. Herein, we investigate the magnetic anisotropy in a six-coordinated cobalt(II) compound that has a complex geometry and distinct triaxial magnetic anisotropy from the perspective of the electronic structure, using electronic spectra, ab initio calculations, and an experimental charge density, of which the latter two provides insight into the d-orbital splitting. The analysis showed that the d-orbital splitting satisfactorily predicted the complex triaxial magnetic anisotropy exhibited by the compound. Furthermore, a novel method to directly compare the ab initio results and the d-orbital populations obtained from the experimental charge density was developed, while a topological analysis of the density provided insights into the metal–ligand bonding. This work thus further establishes the validity of using d-orbitals for predicting magnetic anisotropy in transition metal compounds while also pointing out the need for a more frequent usage of the term triaxial anisotropy in the field of single-molecule magnetism.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Sproules, Dr Stephen and Moiras, Dr Haralampos and McGuire, Mr Jake
Authors: Damgaard-Møller, E., Krause, L., Lassen, H., Malaspina, L. A., Grabowsky, S., Bamberger, H., McGuire, J., Miras, H. N., Sproules, S., and Overgaard, J.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Inorganic Chemistry
Publisher:American Chemical Society
ISSN:0020-1669
ISSN (Online):1520-510X
Published Online:01 September 2020
Copyright Holders:Copyright © 2020 American Chemical Society
First Published:First published in Inorganic Chemistry 59(18):13190-13200
Publisher Policy:Reproduced in accordance with the publisher copyright policy

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