Determining Key Local Vibrations in the Relaxation of Molecular Spin Qubits and Single-Molecule Magnets

To design molecular spin qubits and nanomagnets operating at high temperatures, there is an urgent need to understand the relationship between vibrations and spin relaxation processes. Herein we develop a simple first-principles methodology to determine the modulation that vibrations exert on spin energy levels. This methodology is applied to [Cu­(mnt)₂]^2– (mnt^2– = 1,2-dicyano­ethylene-1,2-dithiolate), a highly coherent complex. By theoretically identifying the most relevant vibrational modes, we are able to offer general strategies to chemically design more resilient magnetic molecules, where the energy of the spin states is not coupled to vibrations.