An ab initio study of magnetic relaxation in a dysprosocenium single-molecule magnet

The development of technologies exploiting molecular spins, such as single-molecule magnets (SMMs) and molecular qubits, requires detailed knowledge of the microscopic spin-dynamics, which in turn relies on understanding the spin-phonon coupling. Building on our recent work, we perform ab initio calculations of the phonon modes, anharmonic phonon scattering and spin-phonon coupling in a molecular crystal of the dysprosocenium SMM [DyCpttt2][B(C6F5)4]. Spin-dynamics simulations give excellent agreement with experiment and provide further insight into the high-performance of the dysprosocenium class of SMMs. We find that strong phonon scattering in the (pseudo-)acoustic regime leads to very short phonon lifetimes, large phonon linewidths, and, consequently, slower spin relaxation.