title: Adsorption-Induced Solvent-Based Electrostatic Gating of Charge Transport through Molecular Junctions.
abstract: Recent experiments have shown that transport properties of molecular-scale devices can be reversibly altered by the surrounding solvent. Here, we use a combination of first-principles calculations and experiment to explain this change in transport properties through a shift in the local electrostatic potential at the junction caused by nearby conducting and solvent molecules chemically bound to the electrodes. This effect is found to alter the conductance of 4,4'-bipyridine-gold junctions by more than 50%. Moreover, we develop a general electrostatic model that quantitatively relates the conductance and dipoles associated with the bound solvent and conducting molecules. Our work shows that solvent-induced effects can be used to control charge and energy transport at molecular-scale interfaces.
authors.affiliation: †Department of Physics, University of California, Berkeley, California 94720, United States.|‡Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
authors.forename: Michele
authors.initials: M
authors.lastname: Kotiuga
authors.affiliation: ‡Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.|§Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States.
authors.forename: Pierre
authors.initials: P
authors.lastname: Darancet
authors.affiliation: §Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States.|△Centro de Nanociencia y Nanotecnologia, Universidad de las Fuerzas Armadas-ESPE, Sangolqui, P.O. Box 171-5-231B, Ecuador.
authors.forename: Carlos R
authors.initials: CR
authors.lastname: Arroyo
authors.affiliation: §Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States.
authors.forename: Latha
authors.initials: L
authors.lastname: Venkataraman
authors.affiliation: †Department of Physics, University of California, Berkeley, California 94720, United States.|‡Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.|∥Kavli Energy NanoSciences Institute at Berkeley, University of California, Berkeley, California 94720, United States.
authors.forename: Jeffrey B
authors.initials: JB
authors.lastname: Neaton
keywords: density functional theory; molecular conductance; single molecule electronics; solvent effects