Non-adiabatic corrections to electric current in molecular junctions due to nuclear motion at the molecule-electrode interfaces

Kershaw, Vincent F., and Kosov, Daniel S. (2018) Non-adiabatic corrections to electric current in molecular junctions due to nuclear motion at the molecule-electrode interfaces. Journal of Chemical Physics, 149 (4). 044121.

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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 as 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.

Item ID: 55902
Item Type: Article (Research - C1)
ISSN: 1089-7690
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A version of this publication was included as Chapter 3 of the following PhD thesis: Kershaw, Vincent Francis (2020) Non-adiabatic quantum transport and atomic motion in molecular-sized electronic systems. PhD thesis, James Cook University, which is available Open Access in ResearchOnline@JCU. Please see the Related URLs for access.

Date Deposited: 18 Oct 2018 21:54
FoR Codes: 34 CHEMICAL SCIENCES > 3407 Theoretical and computational chemistry > 340704 Theoretical quantum chemistry @ 100%
SEO Codes: 97 EXPANDING KNOWLEDGE > 970102 Expanding Knowledge in the Physical Sciences @ 100%
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