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We investigate electron transport through a mixed-valence molecular complexin which an excess electron can tunnel between hetero-valent transition metalions, each having a fixed localized spin. We show that in this class ofmolecules the interplay of the spins and the vibrational breathing modes of theionic ligand-shells allows the total molecular spin to be detected as well ascontrolled by nonequilibrium transport. Due to a spin-dependent pseudoJahn-Teller effect electronic transitions with different spin values can bedistinguished by their vibronic conductance side peaks, without using anexternal magnetic field. Conversely, we show that the spin state of the entiremolecule can also be controlled via the nonequilibrium quantized molecularvibrations due to a vibration-induced spin-blockade.

Vibrational detection and control of spin in mixed-valence molecular transistors