Molecular Nanomagnets Probed by Inelastic Neutron Scattering

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Abstract

Molecular nanomagnets have the potential to address many technological challenges whilst also giving insights into fundamental quantum behaviours. In order to accomplish this it is crucial that a determination of the magnetic properties of these nanoscopic objects is established. Inelastic neutron scattering (INS) is at the forefront of these investigations and is a technique capable of unravelling vast amounts of information that can enable a detailed understanding and tailoring of the properties of these molecules. This thesis demonstrates the application of this state-of-the-art technique to a number of different yet important nanomagnets in the field, pushing the technique to the limit to yield new insights into the underlying physics in these systems. The potential of this technique is finely displayed in the unravelling of the spin dynamics in a supramolecular (Cr7Ni)2 dimer, where the intermolecular entanglement is portrayed in the vast 4D phase space extracted. This work also harnesses the full power of the 4D-INS technique to resolve the long standing issue of the spin Hamiltonian in the archetypal single molecule magnet (SMM) Mn12, which after hundreds of papers since the realisation of its magnetic properties some 25 years ago had still not been convincingly settled. A little utilised avenue to building on Mn12 and generating better SMMs is also suggested and the evolution of the technique demonstrated by 8 characterising the magnetic properties in a tiny quantity of nanomagnet dimers.

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