Characterization of the isolated [ Co 3 Ni ( EtOH ) ] + cluster by IR spectroscopy and spin-dynamics calculations

We experimentally and theoretically study the geometry, as well as the electronic and vibrational properties, of the heterotetranuclear magnetic cluster [Co3Ni(EtOH)]+, which is prepared in the gas phase with molecular beam expansion. We characterize the cluster and identify possible isomers through the comparison of experimentally observed infrared spectra with state-of-the-art quantum chemistry calculations, more specifically by focusing on the OH stretching frequency. Furthermore, we suggest ultrafast, laser-induced, local spin-flip scenarios on every Co atom, and report a cooperative effect, in which the spin density is localized on one Co atom, gets transiently transferred to another, and then bounces back pointing in the opposite direction. Finally, we predict a tolerance of the suggested scenarios with respect to the laser detuning of about 20 meV, which lies within an experimentally applicable range. Our joint investigation is an additional step toward the implementation of laser-controlled nanospintronic devices.