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Charge transport through single molecules can be influenced by the charge andspin states of redox-active metal centres placed in the transport pathway.These molecular intrinsic properties are usually addressed by varying themolecules electrochemical and magnetic environment, a procedure that requirescomplex setups with multiple terminals. Here we show that oxidation andreduction of organometallic compounds containing either Fe, Ru or Mo centrescan solely be triggered by the electric field applied to a two-terminalmolecular junction. Whereas all compounds exhibit bias-dependent hysteresis,the Mo-containing compound additionally shows an abrupt voltage-inducedconductance switching, yielding high to low current ratios exceeding 1000 atvoltage stimuli of less than 1.0 V. DFT calculations identify a localized,redox active molecular orbital that is weakly coupled to the electrodes andclosely aligned with the Fermi energy of the leads because of thespin-polarised ground state unique to the Mo centre. This situation opens anadditional slow and incoherent hopping channel for transport, triggering atransient charging effect of the entire molecule and a strong hysteresis withunprecedented high low-to-high current ratios.

Field-induced Conductance Switching by Charge-state Alternation in Organometallic Single-Molecule Junctions