Chiral-phonons Control of Molecular Spins

Magnetic molecules are at the forefront of the next technological revolution, offering the unique possibility to control and manipulate quantum spin states at the nanoscale. However, although long relaxation times have been achieved up to 80 K, there are currently no practical ways to initialize molecular spins in a pure quantum state, e.g. the fully polarized one. This is a critical roadblock to the development of any application based on magnetic molecules.Chiral phonons hold the potential to provide new ways to manipulate spin states by exchanging angular momentum, which in turn can be pumped into the vibrations degrees of freedom through circularly polarized THz light. Although this proposal for controlling spin has been experimentally demonstrated for condensed-matter systems like 2D materials, evidence for molecules still needs to be provided. At the same time, the understanding of this process is still minimal, and there is no first principles evidence on how chiral phonons emerge in a material and how they influence spin dynamics.CHIC will break new ground in this emerging field by delivering the first fully ab initio investigation of chiral phonons in molecular materials, going from showing its origin in spin-phonon coupling, to quantitatively predicting the efficiency of spin population pumping through THz light, and individuating novel chemical strategies towards the enhanced control of spin polarization.The project builds on the synergy between my previous experience with chiral chemical systems, molecular magnetism, and electronic structure theory, and the expertise of Prof. Lunghi, the supervisor, on ab initio spin relaxation and open quantum systems dynamics. Thanks to this orthogonal knowledge transfer and a comprehensive set of training activities, I will be able to make a long-lasting contribution to the field of molecular quantum technologies with far-reaching consequences for the establishment of a quantum industry in the EU.