Dynamical correction to linear Kohn-Sham conductances from static density functional theory.

For molecules weakly coupled to leads the exact linear Kohn-Sham (KS) conductance can be orders of magnitude larger than the true linear conductance due to the lack of dynamical exchange-correlation (xc) corrections. In this work we show how to incorporate dynamical effects in KS transport calculations. The only quantity needed is the static xc potential in the molecular junction. Our scheme provides a comprehensive description of Coulomb blockade without breaking the spin symmetry. This is explicitly demonstrated in single-wall nanotubes where the corrected conductance is in good agreement with experimental data whereas the KS conductance fails dramatically.

[1]  J. Perdew,et al.  Density-Functional Theory for Fractional Particle Number: Derivative Discontinuities of the Energy , 1982 .

[2]  A. M. Tsvelick,et al.  Exact solution of the Anderson model: I , 1983 .

[3]  E. Gross,et al.  Density-Functional Theory for Time-Dependent Systems , 1984 .

[4]  The European Science Foundation (ESF) , 1994, Environmental science and pollution research international.

[5]  Spin configurations of a carbon nanotube in a nonuniform external potential , 1999, Physical review letters.

[6]  C. Ta.  Kondo effect in a magnetic field and the magnetoresistivity of kondo alloys , 2000 .

[7]  S. Tarucha,et al.  Few-electron quantum dots , 2001 .

[8]  Multiwall carbon nanotubes as quantum dots. , 2002, Physical review letters.

[9]  Hongkun Park,et al.  Shell filling and exchange coupling in metallic single-walled carbon nanotubes. , 2002, Physical review letters.

[10]  Luiz N. Oliveira,et al.  Density-functional study of the Mott gap in the Hubbard model , 2002 .

[11]  N A Lima,et al.  Density functionals not based on the electron gas: local-density approximation for a Luttinger liquid. , 2003, Physical review letters.

[12]  Gianluca Stefanucci,et al.  Time-dependent partition-free approach in resonant tunneling systems , 2003, cond-mat/0310084.

[13]  Hartmut Haug,et al.  Quantum Kinetics in Transport and Optics of Semiconductors , 2004 .

[14]  G. Stefanucci,et al.  Time-dependent quantum transport: An exact formulation based on TDDFT , 2004, cond-mat/0402094.

[15]  Conductance through Quantum Dots Studied by Finite Temperature DMRG , 2004, cond-mat/0406594.

[16]  Electronic excitation spectrum of metallic carbon nanotubes , 2004, cond-mat/0411530.

[17]  Dynamical corrections to the DFT-LDA electron conductance in nanoscale systems. , 2004, Physical review letters.

[18]  Kieron Burke,et al.  Self-interaction errors in density-functional calculations of electronic transport. , 2005, Physical review letters.

[19]  Zero-bias molecular electronics: Exchange-correlation corrections to Landauer's formula , 2005, cond-mat/0502385.

[20]  Claudio Verdozzi,et al.  Time-dependent density-functional theory and strongly correlated systems: insight from numerical studies. , 2007, Physical review letters.

[21]  G. Vignale,et al.  Incompleteness of the Landauer formula for electronic transport , 2008, 0810.2857.

[22]  G. Stefanucci,et al.  Generalized waveguide approach to tight-binding wires: Understanding large vortex currents in quantum rings , 2009, 0903.0557.

[23]  Weitao Yang,et al.  Discontinuous nature of the exchange-correlation functional in strongly correlated systems. , 2008, Physical review letters.

[24]  K. Thygesen,et al.  The relation between structure and quantum interference in single molecule junctions. , 2010, Nano letters.

[25]  E K U Gross,et al.  Dynamical Coulomb blockade and the derivative discontinuity of time-dependent density functional theory. , 2009, Physical review letters.

[26]  H. Mera,et al.  Are Kohn-Sham conductances accurate? , 2010, Physical review letters.

[27]  G. Stefanucci,et al.  Assessing the accuracy of Kohn-Sham conductances using the Friedel sum rule , 2010 .

[28]  G. Stefanucci,et al.  Towards a description of the Kondo effect using time-dependent density-functional theory. , 2011, Physical review letters.

[29]  M. Ratner,et al.  Novel quantum interference effects in transport through molecular radicals. , 2011, Nano letters.

[30]  F. Evers,et al.  Broadening of the derivative discontinuity in density functional theory. , 2011, Physical chemistry chemical physics : PCCP.

[31]  S. Kurth,et al.  Comparative study of many-body perturbation theory and time-dependent density functional theory in the out-of-equilibrium Anderson model , 2011, 1107.0162.

[32]  Missing derivative discontinuity of the exchange-correlation energy for attractive interactions: The charge Kondo effect , 2012, 1208.3042.

[33]  J. Lorenzana,et al.  Density-functional theory with adaptive pair density: The Gutzwiller approximation as a density functional , 2012 .

[34]  Á. Rubio,et al.  Universal dynamical steps in the exact time-dependent exchange-correlation potential. , 2012, Physical review letters.

[35]  Integer particle preference during charge transfer in Kohn-Sham theory , 2012 .

[36]  K. Burke,et al.  Bethe ansatz approach to the Kondo effect within density-functional theory. , 2012, Physical review letters.

[37]  F. Evers,et al.  Transport calculations based on density functional theory, Friedel's sum rule, and the Kondo effect , 2012 .

[38]  Paola Gori-Giorgi,et al.  Strong correlation in Kohn-Sham density functional theory. , 2012, Physical review letters.

[39]  S. Kurth,et al.  Lattice density functional theory at finite temperature with strongly density-dependent exchange-correlation potentials , 2012, 1209.3145.

[40]  Discontinuities of the exchange-correlation kernel and charge-transfer excitations in time-dependent density-functional theory , 2011, 1108.3100.

[41]  M. Ruggenthaler,et al.  Many-body quantum dynamics from the density , 2013 .

[42]  L. Kronik,et al.  Piecewise linearity of approximate density functionals revisited: implications for frontier orbital energies. , 2012, Physical review letters.