Many-body correlations and coupling in benzene-dithiol junctions
arXiv:1612.06780 · doi:10.1103/PhysRevB.95.115137
Abstract
Most theoretical studies of nanoscale transport in molecular junctions rely on the combination of the Landauer formalism with Kohn-Sham density functional theory (DFT) using standard local and semilocal functionals to approximate exchange and correlation effects. In many cases, the resulting conductance is overestimated with respect to experiments. Recent works have demonstrated that this discrepancy may be reduced when including many-body corrections on top of DFT. Here we study benzene-dithiol (BDT) gold junctions and analyze the effect of many-body perturbation theory (MBPT) on the calculation of the conductance with respect to different bonding geometries. We find that the many-body corrections to the conductance strongly depend on the metal-molecule coupling strength. In the BDT junction with the lowest coupling, many-body corrections reduce the overestimation on the conductance to a factor two, improving the agreement with experiments. In contrast, in the strongest coupling cases, many-body corrections on the conductance are found to be sensibly smaller and standard DFT reveals a valid approach.
9 pages, 4 figures
References in corpus (29)
- Density functional method for nonequilibrium electron transport
- A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
- Dependence of Single Molecule Junction Conductance on Molecular Conformation
- Hubbard-corrected DFT energy functionals: the LDA+U description of correlated systems
- Mechanically-Controlled Binary Conductance Switching of a Single-Molecule Junction
- Amine-Gold Linked Single-Molecule Junctions: Experiment and Theory
- Time-dependent quantum transport: A practical scheme using density functional theory
- Simultaneous Determination of Conductance and Thermopower of Single Molecule Junctions
- Conserving GW scheme for nonequilibrium quantum transport in molecular contacts
- Zero-bias molecular electronics: Exchange-correlation corrections to Landauer's formula
- Dynamical corrections to the DFT-LDA electron conductance in nanoscale systems
- n-Alkyl Thiol Head Group Interactions with the Au(111) Surface
- Effects of self-interaction corrections on the transport properties of phenyl-based molecular junctions
- Molecular transport calculations with Wannier functions
- Influence of Functional Groups on Charge Transport in Molecular Junctions
- The bandstructure of gold from many-body perturbation theory
- Ab initio GW electron-electron interaction effects in Quantum Transport
- Towards a description of the Kondo effect using time-dependent density functional theory
- A variational pseudo-self-interaction correction approach: ab-initio description of correlated oxides and molecules
- Maximally-localized Wannier functions for GW quasiparticles
- Incompleteness of the Landauer Formula for Electronic Transport
- Ab initio correlation effects on the electronic and transport properties of metal(II)-phthalocyanine based devices
- Do methanethiol adsorbates on the Au(111) surface dissociate?
- Ab initio complex band structure of conjugated polymers: Effects of hydrid DFT and GW schemes
- Donor and acceptor levels of organic photovoltaic compounds from first principles
- Efficient DFT+U calculations of ballistic electron transport: Application to Au monatomic chains with a CO impurity
- Identification of the Atomic Scale Structures of the Gold-Thiol Interfaces of Molecular Nanowires by Inelastic Tunneling Spectroscopy
- Dynamical Image Charge Effect in Molecular Tunnel Junctions: Beyond Energy Level Alignment
- Correlation of interfacial bonding mechanism and equilibrium conductance of molecular junctions