Predicting the conductance of strongly correlated molecules: the Kondo effect in perchlorotriphenylmethyl/Au junctions

Abstract

Stable organic radicals integrated into molecular junctions represent a practical realization of the single-orbital Anderson impurity model. Motivated by recent experiments for perchlorotriphenylmethyl (PTM) molecules contacted to gold electrodes, we develop a method that combines density functional theory (DFT), quantum transport theory, numerical renormalization group (NRG) calculations and renormalized super-perturbation theory (rSPT) to compute both equilibrium and non-equilibrium properties of strongly correlated nanoscale systems at low temperatures effectively from first principles. We determine the possible atomic structures of the interfaces between the molecule and the electrodes, which allow us to estimate the Kondo temperature and the characteristic transport properties, which compare well with experiments. By using the non-equilibrium rSPT results we assess the range of validity of equilibrium DFT+NRG-based transmission calculations for the evaluation of the finite voltage conductance. The results demonstrate that our method can provide qualitative insights into the properties of molecular junctions when the molecule-metal contacts are amorphous or generally ill-defined, and that it can further give a fully quantitative description when the experimental contact structures are well characterized.

arXiv commentNanoscale, 2018

References in corpus (29)

• Density functional method for nonequilibrium electron transport
• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• The numerical renormalization group method for quantum impurity systems
• Half-metallic ferromagnets: From band structure to many-body effects
• Hubbard-corrected DFT energy functionals: the LDA+U description of correlated systems
• From the Kondo Regime to the Mixed-Valence Regime in a Single-Electron Transistor
• Correlated metals and the LDA+U method
• Quantum embedding theories
• A first-principles approach to electrical transport in atomic-scale nanostructures
• Temperature and magnetic field dependence of a Kondo system in the weak coupling regime
• Robust organic radical molecular junctions using acetylene terminated groups for C-Au bond formation
• Towards a description of the Kondo effect using time-dependent density functional theory
• Dynamical Mean-Field Theory for Molecular Electronics: Electronic Structure and Transport Properties
• Kondo Conductance in an Atomic Nanocontact from First Principles
• Constrained-DFT method for accurate energy level alignment of metal/molecule interfaces
• Universal out-of-equilibrium Transport in Kondo-correlated quantum dots: Renormalized dual Fermions on the Keldysh contour
• Steady-State Density Functional Theory for Finite Bias Conductances
• Kondo effect and conductance of nanocontacts with magnetic impurities
• Kondo effect and spin quenching in high-spin molecules on metal substrates
• Quantum transport simulation scheme including strong correlations and its application to organic radicals adsorbed on gold
• Kondo conductance across the smallest spin 1/2 radical molecule
• Atomistic Simulations of Highly Conductive Molecular Transport Junctions Under Realistic Conditions
• Structural Origins of Conductance Fluctuations in Gold-Thiolate Molecular Transport Junctions
• Many-body spectral functions from steady state density functional theory
• Orbital Kondo effect in Cobalt-Benzene sandwich molecules
• Conductance scaling in Kondo correlated quantum dots: role of level asymmetry and charging energy
• Nonequilibrium Anderson model made simple with density functional theory
• Transmission through correlated Cu${}_n$CoCu${}_n$ heterostructures
• Kondo impurities in nanotubes: the importance of being "in"

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• Chemical sensing with graphene: A quantum field theory perspective
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