Coherent and incoherent dynamics of molecular nanomagnets investigated by magnetic resonances and inelastic neutron and x-ray scattering

Abstract

The focus of this thesis is the characterization of the coherent and incoherent dynamics of molecular nanomagnets. For this purpose, we will exploit several state-of-the-art experimental techniques, such as magnetic resonances and inelastic scattering of neutrons and X-rays. By means of nuclear magnetic resonances we will characterize the nuclear relaxation times and the parameters of the spin Hamiltonian of two V-based molecular qudits, demonstrating, in addition, the capability to coherently manipulate their nuclear states. This proof-of-concepts experiments represent an important first step towards the implementation of molecular qudits in quantum information processing. Moreover, by X-ray inelastic scattering, we will investigate the phonon dispersions of one benchmark molecular qudit and their role in its relaxation dynamics. We will also focus on the key factors governing the phonon-induced relaxation in Dy-based single molecule magnets by studying, through inelastic neutron scattering, the changes induced in their phonon density of states by chemical substitutions or structural deformations. Finally, a synergistic approach combining electron and nuclear magnetic resonance will give us insights on the electronic relaxation dynamics of a supramolecular assembly linking an isolated nuclear qudit and an electronic spin qubit.