Understanding resonant charge transport through weakly coupled single-molecule junctions

Abstract

Off-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and it is now well understood within the framework of the non-interacting Landauer approach. Conversely, gaining a qualitative and quantitative understanding of the resonant transport regime has proven more elusive. Here, we study resonant charge transport through graphene-based zinc-porphyrin junctions. We experimentally demonstrate an inadequacy of the non-interacting Landauer theory as well as the conventional single-mode Franck-Condon model. Instead, we model the overall charge transport as a sequence of non-adiabatic electron transfers, the rates of which depend on both outer and inner-sphere vibrational interactions. We show that the transport properties of our molecular junctions are determined by a combination of electron-electron and electron-vibrational coupling, and are sensitive to the interactions with the wider local environment. Furthermore, we assess the importance of nuclear tunnelling and examine the suitability of semi-classical Marcus theory as a description of charge transport in molecular devices.

version accepted in Nature Communications; SI available at https://researchportal.hw.ac.uk/en/publications/understanding-resonant-charge-transport-through-weakly-coupled-si

References in corpus (10)

• Electron transmission through molecules and molecular interfaces
• Franck-Condon blockade and giant Fano factors in transport through single molecules
• Room-temperature gating of molecular junctions using few-layer graphene nanogap electrodes
• Vibrational sidebands and dissipative tunneling in molecular transistors
• Spin-based all-optical quantum computation with quantum dots: understanding and suppressing decoherence
• Franck-Condon Blockade in a Single-Molecule Transistor
• Beyond Marcus theory and the Landauer-Büttiker approach in molecular junctions: A unified framework
• Irreversibility and hysteresis in redox molecular conduction junctions
• Vibrational Excitations in Weakly Coupled Single-Molecule Junctions: A Computational Analysis
• Sequential electron transport and vibrational excitations in an organic molecule coupled to few-kayer graphene electrodes

Cited by in corpus (14)

• Phase-Coherent Charge Transport through a Porphyrin Nanoribbon
• Semiclassical instanton formulation of Marcus-Levich-Jortner theory
• Beyond Marcus theory and the Landauer-Buttiker approach in molecular junctions. II. A self-consistent Born approach
• OQuPy: A Python package to efficiently simulate non-Markovian open quantum systems with process tensors
• Single-electron transport in a molecular Hubbard dimer
• ACE: A general-purpose non-Markovian open quantum systems simulation toolkit based on process tensors
• Generalized input-output method: A new route to quantum transport junctions
• On the theory of charge transport and entropic effects in solvated molecular junctions
• Electronic measurements of entropy in meso- and nanoscale systems
• Charge-state dependent vibrational relaxation in a single-molecule junction
• Enhanced entanglement in multi-bath spin-boson models
• Spin-orbit interaction induces charge beatings in a lightwave-STM single molecule junction
• Crucial effect of transverse vibrations on the transport through polymer chains
• Interference and shot noise in a degenerate Anderson-Holstein model