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Recent experiments have shown that transport properties of molecular-scaledevices can be reversibly altered by the surrounding solvent. Here, we use acombination of first-principles calculations and experiment to explain thischange in transport properties through a shift in the local electrostaticpotential at the junction caused by nearby conducting and solvent moleculeschemically bound to the electrodes. This effect is found to alter theconductance of bipyridine - gold junctions by more than 50%. Moreover, wedevelop a general electrostatic model that quantitatively predicts therelationship between conductance and the binding energies and dipoles of thesolvent and conducting molecules. Our work shows that solvent induced effectsare a viable route for controlling charge and energy transport atmolecular-scale interfaces.

Adsorption-Induced Solvent-Based Electrostatic Gating of Charge Transport through Molecular Junctions