Dy-based single-molecule magnet as a case study for magnetization relaxation under applied pressure

Molecular nanomagnets have garnered significant attention in recent years thanks to their unique potential in quantum information processing as molecular qudits and in high-density memory encoding as single-molecule magnets. However, fully unlocking the potential of these systems requires a comprehensive understanding of the interplay between the various mechanisms that govern their relaxation dynamics, which remains a noncompletely understood phenomenon. In this work, we employ a cost-effective semi-ab initio approach to model the magnetization relaxation dynamics in a testbed Dy-based single-molecule magnet and determine the effects of applied external pressure on the interplay between various mechanisms, such as coupling with molecular vibrations and quantum tunneling. Ab initio phonon calculations are validated by direct comparison with inelastic neutron scattering experiments, which are used for the first time to investigate pressure-induced modifications of phonons and vibrations in a molecular nanomagnet. The combination of our theoretical approach with different experimental techniques allows us to predict an overall acceleration of the relaxation dynamics under pressure, disentangling the role of different ingredients, such as crystal field axiality and phonons.