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Manipulation of organic polyradicals in a single-molecule transistor

Inspired by cotunneling spectroscopy of spin-states in a single OPE5-based molecule, we investigate the prospects for electric control of magnetism in purely organic molecules contacted in a three-terminal geometry. Using the gate electrode, the molecule is reversibly switched between three different redox states, with magnetic spectra revealing both ferromagnetic and antiferromagnetic exchange couplings on the molecule. These observations are shown to be captured by an effective low-energy Heisenberg model, which we substantiate microscopically by a simple valence bond description of the molecule. These preliminary findings suggest an interesting route towards functionalized all-organic molecular magnetism.