Vibron-assisted spin excitation in a magnetically anisotropic molecule

The electrical control and readout of molecular spin states are key for high-density storage. Expectations are that electrically-driven spin and vibrational excitations in a molecule should give rise to new conductance features in the presence of magnetic anisotropy, offering alternative routes to study and, ultimately, manipulate molecular magnetism. Here, we use inelastic electron tunneling spectroscopy to promote and detect the excited spin states of a prototypical molecule with magnetic anisotropy. We demonstrate the existence of a vibron-assisted spin excitation that can exceed in energy and in amplitude a simple excitation among spin states. This excitation, which can be quenched by structural changes in the magnetic molecule, is explained using first-principles calculations that include dynamical electroniccorrelations.We thank M. Ternes for providing his fitting program. This work was supported by the Agence Nationale de la Recherche (grants No. ANR-13-BS10-0016, ANR-11-LABX-0058 NIE and ANR-10-LABX-0026 CSC) and by the Agencia Española de Investigación (grants Nos. MAT2016-78293-C6-1-R and MDM-2016-0618). D.-J.C. and N.L. thank the MICINN (project RTI2018-097895-B-C44). M.-L.B. thanks the national computational center CINES and TGCC (GENCI project: A0030807364)