Nonequilibrium Green's function theory for nonadiabatic effects in quantum electron transport
arXiv:1710.00195 · doi:10.1063/1.5007071
Abstract
We develop nonequilibribrium Green's function based transport theory, which includes effects of nonadiabatic nuclear motion in the calculation of the electric current in molecular junctions. Our approach is based on the separation of slow and fast timescales in the equations of motion for the Green's functions by means of the Wigner representation. Time derivatives with respect to central time serves as a small parameter in the perturbative expansion enabling the computation of nonadiabatic corrections to molecular Green's functions. Consequently, we produce series of analytic expressions for non-adiabatic electronic Green's functions (up to the second order in the central time derivatives); which depend not solely on instantaneous molecular geometry but likewise on nuclear velocities and accelerations. Extended formula for electric current is derived which accounts for the non-adiabatic corrections. This theory is concisely illustrated by the calculations on a model molecular junction.
References in corpus (14)
- Franck-Condon blockade and giant Fano factors in transport through single molecules
- Inelastic transport theory from first-principles: methodology and applications for nanoscale devices
- Real-time path integral approach to nonequilibrium many-body quantum system
- Resonant Electron Transport in Single-Molecule Junctions: Vibrational Excitation, Rectification, Negative Differential Resistance and Local Cooling
- Hierarchical Quantum Master Equation Approach to Electronic-Vibrational Coupling in Nonequilibrium Transport through Nanosystems
- Cooling mechanisms in molecular conduction junctions
- Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
- Current Noise in Single-Molecule Junctions Induced by Electronic-Vibrational Coupling
- Effect of nonadiabatic electronic-vibrational interactions on the transport properties of single-molecule junctions
- Nonequilibrium resonant spectroscopy of molecular vibrons
- Waiting time distribution for electron transport in a molecular junction with electron-vibration interaction
- Vibrational inelastic scattering effects in molecular electronics
- Superoperator coupled cluster method for nonequilibrium density matrix
- Non-renewal statistics for electron transport in a molecular junction with electron-vibration interaction