Fermi level alignment in single molecule junctions and its dependence on interface structure

The alignment of the Fermi level of a metal electrode within the gap of the highest occupied and lowest unoccupied orbital of a molecule is a key quantity in molecular electronics. Depending on the type of molecule and the interface structure of the junction, it can vary the electron transparency of a gold/molecule/gold junction by at least one order of magnitude. In this article we will discuss how Fermi level alignment is related to surface structure and bonding configuration on the basis of density functional theory calculations for bipyridine and biphenyl dithiolate between gold leads. We will also relate our findings to quantum-chemical concepts such as electronegativity.Comment: 5 pages, 2 figures, presented at the ICN+T 2006 conferenc

Conformation dependence of charge transfer and level alignment in nitrobenzene junctions with pyridyl anchor groups

The alignment of molecular levels with the Fermi energy in single molecule junctions is a crucial factor in determining their conductance or the observability of quantum interference effects. In the present study which is based on density functional theory calculations, we explore the zero-bias charge transfer and level alignment for nitro-bipyridyl-phenyl adsorbed between two gold surfaces which we find to vary significantly with the molecular conformation. The net charge transfer is the result of two opposing effects, namely Pauli repulsion at the interface between the molecule and the leads, and the electron accepting nature of the NO$_2$ group, where only the latter which we analyze in terms of the electronegativity of the isolated molecules depends on the two intra-molecular torsion angles. We provide evidence that the conformation dependence of the alignment of molecular levels and peaks in the transmission function can indeed be understood in terms of charge transfer for this system, and that other properties such as molecular dipoles do not play a significant role. Our study is relevant for device design in molecular electronics where nitrobenzene appears as a component in proposals for rectification, quantum interference or chemical gating.Comment: 10 pages, 6 figure

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

Forces and conductances in a single-molecule bipyridine junction

Inspired by recent measurements of forces and conductances of bipyridine nano-junctions, we have performed density functional theory calculations of structure and electron transport in a bipyridine molecule attached between gold electrodes for seven different contact geometries. The calculations show that both the bonding force and the conductance are sensitive to the surface structure, and that both properties are in good agreement with experiment for contact geometries characterized by intermediate coordination of the metal atoms corresponding to a stepped surface. The conductance is mediated by the lowest unoccupied molecular orbital, which can be illustrated by a quantitative comparison with a one-level model. Implications for the interpretation of the experimentally determined force and conductance distributions are discussed

High-precision covariant one-boson-exchange potentials for np scattering below 350 MeV

All realistic potential models for the two-nucleon interaction are to some extent based on boson exchange. However, in order to achieve an essentially perfect fit to the scattering data, characterized by a chi2/Ndata ~ 1, previous potentials have abandoned a pure one boson-exchange mechanism (OBE). Using a covariant theory, we have found a OBE potential that fits the 2006 world np data below 350 MeV with a chi2/Ndata = 1.06 for 3788 data. Our potential has fewer adjustable parameters than previous high-precision potentials, and also reproduces the experimental triton binding energy without introducing additional irreducible three-nucleon forces.Comment: 4 pages; revised version with augmented data sets; agrees with published versio

Integrated Vertical Bloch Line (VBL) memory

Vertical Bloch Line (VBL) Memory is a recently conceived, integrated, solid state, block access, VLSI memory which offers the potential of 1 Gbit/sq cm areal storage density, data rates of hundreds of megabits/sec, and submillisecond average access time simultaneously at relatively low mass, volume, and power values when compared to alternative technologies. VBLs are micromagnetic structures within magnetic domain walls which can be manipulated using magnetic fields from integrated conductors. The presence or absence of BVL pairs are used to store binary information. At present, efforts are being directed at developing a single chip memory using 25 Mbit/sq cm technology in magnetic garnet material which integrates, at a single operating point, the writing, storage, reading, and amplification functions needed in a memory. The current design architecture, functional elements, and supercomputer simulation results are described which are used to assist the design process

Oriented components and their separations

[EN] There is a tight connection between connectedness, connected components, and certain types of separation spaces. Recently, axiom systems for oriented connectedness were proposed leading to the notion of reaches. Here, we introduce production relations as a further generalization of connectivity spaces and reaches and derive associated systems of oriented components that generalize connected components in a natural manner. The main result is a characterization of generalized reaches in terms of equivalent separation spaces.Stadler, BMR.; Stadler, PF. (2017). Oriented components and their separations. Applied General Topology. 18(2):255-275. doi:10.4995/agt.2017.5868SWORD25527518

Error Propagation in the Hypercycle

We study analytically the steady-state regime of a network of n error-prone self-replicating templates forming an asymmetric hypercycle and its error tail. We show that the existence of a master template with a higher non-catalyzed self-replicative productivity, a, than the error tail ensures the stability of chains in which m<n-1 templates coexist with the master species. The stability of these chains against the error tail is guaranteed for catalytic coupling strengths (K) of order of a. We find that the hypercycle becomes more stable than the chains only for K of order of a2. Furthermore, we show that the minimal replication accuracy per template needed to maintain the hypercycle, the so-called error threshold, vanishes like sqrt(n/K) for large K and n<=4

Metastable States in High Order Short-Range Spin Glasses

The mean number of metastable states in higher order short-range spin glasses is estimated analytically using a variational method introduced by Tanaka and Edwards for very large coordination numbers. For lattices with small connectivities, numerical simulations do not show any significant dependence on the relative positions of the interacting spins on the lattice, indicating thus that these systems can be described by a few macroscopic parameters. As an extremely anisotropic model we consider the low autocorrelated binary spin model and we show through numerical simulations that its landscape has an exceptionally large number of local optima