Beyond Marcus theory and the Landauer-Buttiker approach in molecular junctions. II. A self-consistent Born approach
arXiv:1912.11003 · doi:10.1063/1.5143146
Abstract
Marcus and Landauer-Buttiker approaches to charge transport through molecular junctions describe two contrasting mechanisms of electronic conduction. In previous work, we have shown how these charge transport theories can be unified in the single-level case by incorporating lifetime broadening into the second-order quantum master equation. Here, we extend our previous treatment by incorporating lifetime broadening in the spirit of the self-consistent Born approximation. By comparing both theories to numerically converged hierarchical-equations-of-motion (HEOM) results, we demonstrate that our novel self-consistent approach rectifies shortcomings of our earlier framework which are present especially in the case of relatively strong electron-vibrational coupling. We also discuss circumstances under which the theory developed here simplifies to the generalised theory developed in our earlier work. Finally, by considering the high-temperature limit of our new self-consistent treatment, we show how lifetime broadening can also be self-consistently incorporated into Marcus theory. Overall, we demonstrate that the self-consistent approach constitutes a more accurate description of molecular conduction while retaining most of the conceptual simplicity of our earlier framework.
Version accepted in J. Chem. Phys
References in corpus (15)
- Molecular Transport Junctions: Vibrational Effects
- Franck-Condon blockade and giant Fano factors in transport through single molecules
- Real-time path integral approach to nonequilibrium many-body quantum system
- Theory of the Franck-Condon blockade regime
- Resonant Electron Transport in Single-Molecule Junctions: Vibrational Excitation, Rectification, Negative Differential Resistance and Local Cooling
- Full counting statistics of nano-electromechanical systems
- Hierarchical Quantum Master Equation Approach to Electronic-Vibrational Coupling in Nonequilibrium Transport through Nanosystems
- Transport in molecular states language: Generalized quantum master equation approach
- Vibrational Excitations in Weakly Coupled Single-Molecule Junctions: A Computational Analysis
- A self-consistent quantum master equation approach to molecular transport
- Hierarchical quantum master equation approach to current fluctuations in nonequilibrium charge transport through nanosystems
- Vibrational effects in charge transport through a molecular double quantum dot
- Vibrationally-mediated molecular transistors
- Environment-Assisted Quantum Transport through Single-Molecule Junctions
- Marcus Theory of Thermoelectricity in Molecular Junctions