Nonadiabatic corrections to electric current in molecular junction due to nuclear motion at the molecule-electrode interfaces

Abstract

We present quantum electron transport theory that incorporates dynamical effects of motion of atoms on electrode-molecule interfaces in the calculations of the electric current. The theory is based on non-equilibrium Green's functions. We separate time scales in the Green's functions on fast relative time and slow central time. The derivative with respect to the central time serves as a small parameter in the theory. We solve the real-time Kadanoff-Baym equations for molecular Green's functions using Wigner representation and keep terms up to the second order with respect to the central time derivatives. Molecular Green's functions and consequently the electric current are expressed as functions of molecular junction coordinates as well as velocities and accelerations of molecule-electrode interface nuclei. We apply the theory to model a molecular system and study the effects of non-adiabatic nuclear motion on molecular junction conductivity.

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Cited by in corpus (5)

• Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions
• Timescale separation solution of Kadanoff-Baym equations for quantum transport in time-dependent fields
• First-passage time theory of activated rate chemical processes in electronic molecular junctions
• Non-Adiabatic Effects of Nuclear Motion in Quantum Transport of Electrons: A Self-Consistent Keldysh-Langevin Study
• Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport: inclusion of electron-electron interactions