Related papers: Self-interaction errors in density functional calc…
Molecular signalling in living cells occurs at low copy numbers and is thereby inherently limited by the noise imposed by thermal diffusion. The precision at which biochemical receptors can count signalling molecules is intimately related…
Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…
We study the model of a molecular switch comprised of a molecule with a soft vibrational degree of freedom coupled to metallic leads. In the presence of strong electron-ion interaction, different charge states of the molecule correspond to…
We generalize the exact strong-interaction limit of the exchange-correlation energy of Kohn-Sham density functional theory to open systems with fluctuating particle numbers. When used in the self-consistent Kohn-Sham procedure on…
Recent experiments demonstrate a temperature control of the electric conduction through a ferrocene-based molecular junction. Here we examine the results in view of determining means to distinguish between transport through single-particle…
A review of the approximations in any time-dependent density functional calculation of excitation energies is given. The single-pole approximation for the susceptibility is used to understand errors in popular approximations for the…
Electronic conductance through a single molecule is sensitive towards its structural orientation between two electrodes, owing to the distribution of molecular orbitals and their coupling to the electrode levels, that are governed by…
For adjusting the charging state of a molecular metal complex in the context of a density functional theory description of coherent electron transport through single molecule junctions, we correct for self interaction effects by fixing the…
It is shown that the DFT exchange and correlation functionals satisfy an expression that couples exchange and correlation functionals and functional derivatives evaluated at three different densities and for two particle numbers. This…
Within the framework of nonequilibrium Green's functions, we investigate the thermoelectric transport in a single molecular junction with electron-phonon and electron-electron interactions. By transforming into a displaced phonon basis, we…
Density-functional theory simplifies many-electron calculations by approximating the exchange and correlation interactions with a one-electron operator that is a functional of the density. Hybrid functionals incorporate some amount of exact…
Most density functionals have been developed by imposing the known exact constraints on the exchange-correlation energy, or by a fit to a set of properties of selected systems, or by both. However, accurate modeling of the conventional…
The calculation of the nonlinear conductance of a single-molecule junction is revisited. The self energy on the junction resulting from the electron-phonon interaction has at low temperatures logarithmic singularities (in the real part) and…
The transport properties of a octane-dithiol (ODT) molecule coupled to Au(001) leads are analyzed using density functional theory and non-equilibrium Green functions. It is shown that a symmetric molecule can turn into a diode under…
Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…
Ab initio calculations of phenyl dithiol connected to Au, Ag, Pd, and Pt electrodes are performed using non-equilibrium Green's functions and density functional theory. For each metal, the properties of the molecular junction are considered…
We investigate the effect on molecular transport due to the different structural aspects of metal-molecule interfaces. The example system chosen is the prototypical molecular device formed by sandwiching the phenyl dithiolate molecule (PDT)…
Charge and heat transport through a single molecule tunnel-coupled to external normal electrodes have been studied. The molecule with sufficiently strong interaction between lectrons and vibrational internal degrees of freedom can be…
The performance of several common approximations for the exchange-correlation kernel within time-dependent density-functional theory is tested for elementary excitations in the homogeneous electron gas. Although the adiabatic local-density…
Non-equilibrium Green's functions (NEGF) formalism combined with extended Huckel (EHT) and charging model are used to study electrical conduction through single-molecule junctions. Analyzed molecular complex is composed of asymmetric…