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Forbidden transitions between energy levels typically involve violation ofselection rules imposed by symmetry and/or conservation laws. A nanomagnettunneling between up and down states violates angular momentum conservationbecause of broken rotational symmetry. Here we report observations of highlyforbidden transitions between spin states in a Ni$_4$ single-molecule magnet inwhich a single photon can induce the spin to change by several times $\hbar$,nearly reversing the direction of the spin. These observations are understoodas tunneling-assisted transitions that lift the standard $\Delta m = \pm 1$selection rule for single-photon transitions. These transitions are observed atlow applied fields, where tunneling is dominated by the molecule's intrinsicanisotropy and the field acts as a perturbation. Such transitions can beexploited to create macroscopic superposition states that are not typicallyaccessible through single-photon $\Delta m = \pm 1$ transitions.

Observation of tunneling-assisted highly forbidden single-photon transitions in a Ni$_4$ single-molecule magnet