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Putting the Squeeze on Molecule-Based Magnets: Exploiting Pressure to Develop Magneto-Structural Correlations in Paramagnetic Coordination Compounds

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EaStCHEM School of Chemistry and Centre for Science at Extreme Conditions, The University of Edinburgh, David Brewster Road, Edinburgh EH9 3FJ, UK
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School of Engineering and Centre for Science at Extreme Conditions, The University of Edinburgh, Peter Guthrie Tait Road, Edinburgh EH9 3FD, UK
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School of Natural and Environmental Sciences, Newcastle University, Kings Road, Newcastle NE1 7RU, UK
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School of Molecular Sciences and Centre for Microscopy, Characterisation and Analysis, University of Western Australia, 35 Stirling Highway, Crawley, Perth 6005, Australia
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School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, UK
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Authors to whom correspondence should be addressed.
Magnetochemistry 2020, 6(3), 32; https://doi.org/10.3390/magnetochemistry6030032
Received: 20 July 2020 / Revised: 5 August 2020 / Accepted: 10 August 2020 / Published: 12 August 2020
(This article belongs to the Special Issue Magnetic Properties at Extreme Conditions)
The cornerstone of molecular magnetism is a detailed understanding of the relationship between structure and magnetic behaviour, i.e., the development of magneto-structural correlations. Traditionally, the synthetic chemist approaches this challenge by making multiple compounds that share a similar magnetic core but differ in peripheral ligation. Changes in the ligand framework induce changes in the bond angles and distances around the metal ions, which are manifested in changes to magnetic susceptibility and magnetisation data. This approach requires the synthesis of a series of different ligands and assumes that the chemical/electronic nature of the ligands and their coordination to the metal, the nature and number of counter ions and how they are positioned in the crystal lattice, and the molecular and crystallographic symmetry have no effect on the measured magnetic properties. In short, the assumption is that everything outwith the magnetic core is inconsequential, which is a huge oversimplification. The ideal scenario would be to have the same complex available in multiple structural conformations, and this is something that can be achieved through the application of external hydrostatic pressure, correlating structural changes observed through high-pressure single crystal X-ray crystallography with changes observed in high-pressure magnetometry, in tandem with high-pressure inelastic neutron scattering (INS), high-pressure electron paramagnetic resonance (EPR) spectroscopy, and high-pressure absorption/emission/Raman spectroscopy. In this review, which summarises our work in this area over the last 15 years, we show that the application of pressure to molecule-based magnets can (reversibly) (1) lead to changes in bond angles, distances, and Jahn–Teller orientations; (2) break and form bonds; (3) induce polymerisation/depolymerisation; (4) enforce multiple phase transitions; (5) instigate piezochromism; (6) change the magnitude and sign of pairwise exchange interactions and magnetic anisotropy, and (7) lead to significant increases in magnetic ordering temperatures. View Full-Text
Keywords: high pressure X-ray crystallography; high pressure magnetometry; high pressure absorption spectroscopy; molecule-based magnets; single-molecule magnets; single-ion magnets high pressure X-ray crystallography; high pressure magnetometry; high pressure absorption spectroscopy; molecule-based magnets; single-molecule magnets; single-ion magnets
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MDPI and ACS Style

Etcheverry-Berrios, A.; Parsons, S.; Kamenev, K.V.; Probert, M.R.; Moggach, S.A.; Murrie, M.; Brechin, E.K. Putting the Squeeze on Molecule-Based Magnets: Exploiting Pressure to Develop Magneto-Structural Correlations in Paramagnetic Coordination Compounds. Magnetochemistry 2020, 6, 32. https://doi.org/10.3390/magnetochemistry6030032

AMA Style

Etcheverry-Berrios A, Parsons S, Kamenev KV, Probert MR, Moggach SA, Murrie M, Brechin EK. Putting the Squeeze on Molecule-Based Magnets: Exploiting Pressure to Develop Magneto-Structural Correlations in Paramagnetic Coordination Compounds. Magnetochemistry. 2020; 6(3):32. https://doi.org/10.3390/magnetochemistry6030032

Chicago/Turabian Style

Etcheverry-Berrios, Alvaro; Parsons, Simon; Kamenev, Konstantin V.; Probert, Michael R.; Moggach, Stephen A.; Murrie, Mark; Brechin, Euan K. 2020. "Putting the Squeeze on Molecule-Based Magnets: Exploiting Pressure to Develop Magneto-Structural Correlations in Paramagnetic Coordination Compounds" Magnetochemistry 6, no. 3: 32. https://doi.org/10.3390/magnetochemistry6030032

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