Quantitative Current-Voltage Characteristics in Molecular Junctions from First Principles

Abstract

Using self-energy-corrected density functional theory (DFT) and a coherent scattering-state approach, we explain current-voltage (IV) measurements of four pyridine-Au and amine-Au linked molecular junctions with quantitative accuracy. Parameter-free many-electron self-energy corrections to DFT Kohn-Sham eigenvalues are demonstrated to lead to excellent agreement with experiments at finite bias, improving upon order-of-magnitude errors in currents obtained with standard DFT approaches. We further propose an approximate route for prediction of quantitative IV characteristics for both symmetric and asymmetric molecular junctions based on linear response theory and knowledge of the Stark shifts of junction resonance energies. Our work demonstrates that a quantitative, computationally inexpensive description of coherent transport in molecular junctions is readily achievable, enabling new understanding and control of charge transport properties of molecular-scale interfaces at large bias voltages.

6 pages, 3 figures

References in corpus (19)

• Density functional method for nonequilibrium electron transport
• Selfconsistent order-N density-functional calculations for very large systems
• Dependence of Single Molecule Junction Conductance on Molecular Conformation
• Renormalization of Molecular Electronic Levels at Metal-Molecule Interfaces
• First-Principles Based Matrix-Green's Function Approach to Molecular Electronic Devices: General Formalism
• Mechanically-Controlled Binary Conductance Switching of a Single-Molecule Junction
• Observation of Quantum Interference in Molecular Charge Transport
• Amine-Gold Linked Single-Molecule Junctions: Experiment and Theory
• The Kondo effect in C${}_{60}$ single-molecule transistors
• Magnetoresistance through a single molecule
• Self-interaction errors in density functional calculations of electronic transport
• Simultaneous Determination of Conductance and Thermopower of Single Molecule Junctions
• Formation and Evolution of Single Molecule Junctions
• Polarization-induced renormalization of molecular levels at metallic and semiconducting surfaces
• First-principles phase-coherent transport in metallic nanotubes with realistic contacts
• The bandstructure of gold from many-body perturbation theory
• Relating Energy Level Alignment and Amine-Linked Single Molecule Junction Conductance
• Electronic energy level alignment at metal-molecule interfaces with a GW approach
• Tunneling conductance of amine linked alkyl chains

Cited by in corpus (13)

• Heat dissipation and its relation to thermopower in single-molecule junctions
• Impact of electrode density of states on transport through pyridine-linked single molecule junctions
• Voltage tuning of vibrational mode energies in single-molecule junctions
• Generalized projected dynamics for non-system observables of non-equilibrium quantum impurity models
• Towards a full ab initio theory of strong electronic correlations in nanoscale devices
• Quantum transport simulation scheme including strong correlations and its application to organic radicals adsorbed on gold
• Lead Geometry and Transport Statistics in Molecular Junctions
• Energy-dependent resonance broadening in symmetric and asymmetric molecular junctions from an ab initio non-equilibrium Green's function approach
• Shot noise variation within ensembles of gold atomic break junctions at room temperature
• Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2
• Dynamical coupling and negative differential resistance from interactions across the molecule-electrode interface in molecular junctions
• A multiconfigurational pair-density functional theory approach to molecular junctions
• Interplay of electron and phonon channels in the refrigeration through molecular junctions