Screening effects in a density functional theory based description of molecular junctions in the Coulomb blockade regime

We recently introduced a method based on density functional theory (DFT) and non-equilibrium Green's function techniques (NEGF) for calculating the addition energies of single molecule nano-junctions in the Coulomb blockade (CB) regime. Here we apply this approach to benzene molecules lying parallel and at various distances from two aluminum fcc (111) surfaces, and discuss the distance dependence in our calculations in terms of electrostatic screening effects. The addition energies near the surface are reduced by about a factor of two, which is comparable to previously reported calculations employing a computationally far more demanding quasi-particle description

Electron transfer through a single barrier inside a molecule: from strong to weak coupling

In all theoretical treatments of electron transport through single molecules between two metal electrodes, a clear distinction has to be made between a coherent transport regime with a strong coupling throughout the junction and a Coulomb blockade regime in which the molecule is only weakly coupled to both leads. The former case where the tunnelling barrier is considered to be delocalized across the system can be well described with common mean-field techniques based on density functional theory (DFT), while the latter case with its two distinct barriers localized at the interfaces usually requires a multideterminant description. There is a third scenario with just one barrier localized inside the molecule which we investigate here using a variety of quantum-chemical methods by studying partial charge shifts in biphenyl radical ions induced by an electric field at different angles to modulate the coupling and thereby the barrier within the $\pi$-system. We find steps rounded off at the edges in the charge versus field curves for weak and intermediate coupling, whose accurate description requires a correct treatment of both exchange and dynamical correlation effects is essential. We establish that DFT standard functionals fail to reproduce this feature, while a long range corrected hybrid functional fares much better, which makes it a reasonable choice for a proper DFT-based transport description of such single barrier systemsComment: 8 pages, 4 figures; J. Chem. Phys., in print (2012

Streakline-based closed-loop control of a bluff body flow

A novel closed-loop control methodology is introduced to stabilize a cylinder wake flow based on images of streaklines. Passive scalar tracers are injected upstream the cylinder and their concentration is monitored downstream at certain image sectors of the wake. An AutoRegressive with eXogenous inputs mathematical model is built from these images and a Generalized Predictive Controller algorithm is used to compute the actuation required to stabilize the wake by adding momentum tangentially to the cylinder wall through plasma actuators. The methodology is new and has real-world applications. It is demonstrated on a numerical simulation and the provided results show that good performances are achieved.Fil: Roca, Pablo Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Mecánica. Laboratorio de Fluidodinámica; ArgentinaFil: Cammilleri, Ada. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Mecánica. Laboratorio de Fluidodinámica; ArgentinaFil: Duriez, Thomas Pierre Cornil. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Mecánica. Laboratorio de Fluidodinámica; ArgentinaFil: Mathelin, Lionel. Centre National de la Recherche Scientifique. Laboratoire d'Informatique pour la Mécanique et les Sciences de l'Ingénieur; FranciaFil: Artana, Guillermo Osvaldo. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Mecánica. Laboratorio de Fluidodinámica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentin

Anisotropy of the Mobility of Pentacene from Frustration

The bandstructure of pentacene is calculated using first-principles density functional theory. A large anisotropy of the hole and electron effective masses within the molecular planes is found. The band dispersion of the HOMO and the LUMO is analyzed with the help of a tight-binding fit. The anisotropy is shown to be intimately related to the herringbone structure.Comment: Accepted for publication in Synthetic Metal

Towards a theoretical description of molecular junctions in the Coulomb blockade regime based on density functional theory

Non-equilibrium Greens function techniques (NEGF) combined with Density Functional Theory (DFT) calculations have become a standard tool for the description of electron transport through single molecule nano-junctions in the coherent tunneling regime. However, the applicability of these methods for transport in the Coulomb blockade (CB) regime is still under debate. We present here NEGF-DFT calculations performed on simple model systems in the presence of an effective gate potential. The results show that: i) the CB addition energies can be predicted with such an approach with reasonable accuracy; ii) neither the magnitude of the Kohn-Sham gap nor the lack of a derivative discontinuity in the exchange-correlation functional represent a problem for this purpose

A multideterminant assessment of mean field methods for the description of electron transfer in the weak coupling regime

Multideterminant calculations have been performed on model systems to emphasize the role of many-body effects in the general description of charge quantization experiments. We show numerically and derive analytically that a closed-shell ansatz, the usual ingredient of mean-field methods, does not properly describe the step-like electron transfer characteristic in weakly coupled systems. With the multideterminant results as a benchmark, we have evaluated the performance of common ab initio mean field techniques, such as Hartree Fock (HF) and Density Functional Theory (DFT) with local and hybrid exchange correlation functionals, with a special focus on spin-polarization effects. For HF and hybrid DFT, a qualitatively correct open-shell solution with distinct steps in the electron transfer behaviour can be obtained with a spin-unrestricted (i.e., spin-polarized) ansatz though this solution differs quantitatively from the multideterminant reference. We also discuss the relationship between the electronic eigenvalue gap and the onset of charge transfer for both HF and DFT and relate our findings to recently proposed practical schemes for calculating the addition energies in the Coulomb blockade regime for single molecule junctions from closed-shell DFT within the local density approximation

Effect of magnetic field on the strange star

We study the effect of a magnetic field on the strage quark matter and apply to strange star. We found that the strange star becomes more compact in presence of strong magnetic field.Comment: 10 pages (LaTex) and 3 postscript figures available on reques

Theoretical Characterization of the Electronic Properties of Heterogeneous Vertical Stacks of 2D Metal Dichalcogenides Containing one Doped Layer

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