The ability to electrically-drive spin excitations in molecules with magnetic anisotropy is key for high-density storage and quantum-information technology. Electrons, however, also tunnel via the vibrational excitations unique to a molecule. The interplay of spin and vibrational excitations offers novel routes to study and, ultimately, electrically manipulate molecular magnetism. Here we use a scanning tunneling microscope to electrically induce spin and vibrational excitations in a single molecule consisting of a nickelocene magnetically coupled to a Ni atom. We evidence a vibron-assisted spin excitation at an energy one order of magnitude higher compared to the usual spin excitations of nickelocene and explain it using first-principles calculations that include electron correlations. Furthermore, we observe that spin excitations can be quenched by modifying the Ni-nickelocene coupling. Our study suggests that nickelocene-based complexes constitute a model playground for exploring the interaction of spin and vibrations in the electron transport through single magnetic molecules.
