Four-atom period in the conductance of monatomic Al wires

We present first principles calculations based on density functional theory for the conductance of monatomic Al wires between Al(111) electrodes. In contrast to the even-odd oscillations observed in other metallic wires, the conductance of the Al wires is found to oscillate with a period of 4 atoms as the length of the wire is varied. Although local charge neutrality can account for the observed period it leads to an incorrect phase. We explain the conductance behavior using a resonant transport model based on the electronic structure of the infinite wire.Comment: 4 pages, 5 figure

Interference and k-point sampling in the supercell approach to phase-coherent transport

We present a systematic study of interference and k-point sampling effects in the supercell approach to phase-coherent electron transport. We use a representative tight-binding model to show that interference between the repeated images is a small effect compared to the error introduced by using only the Gamma-point for a supercell containing (3,3) sites in the transverse plane. An insufficient k-point sampling can introduce strong but unphysical features in the transmission function which can be traced to the presence of van Hove singularities in the lead. We present a first-principles calculation of the transmission through a Pt contact which shows that the k-point sampling is also important for realistic systems.Comment: 4 pages, 5 figures. Accepted for Phys. Rev. B (Brief Report

Conduction Mechanism in a Molecular Hydrogen Contact

We present first principles calculations for the conductance of a hydrogen molecule bridging a pair of Pt electrodes. The transmission function has a wide plateau with T~1 which extends across the Fermi level and indicates the existence of a single, robust conductance channel with nearly perfect transmission. Through a detailed Wannier function analysis we show that the H2 bonding state is not involved in the transport and that the plateau forms due to strong hybridization between the H2 anti-bonding state and states on the adjacent Pt atoms. The Wannier functions furthermore allow us to derive a resonant-level model for the system with all parameters determined from the fully self-consistent Kohn-Sham Hamiltonian.Comment: 5 pages, 4 figure

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

Continuous Variable Quantum Key Distribution with a Noisy Laser

Existing experimental implementations of continuous-variable quantum key distribution require shot-noise limited operation, achieved with shot-noise limited lasers. However, loosening this requirement on the laser source would allow for cheaper, potentially integrated systems. Here, we implement a theoretically proposed prepare-and-measure continuous-variable protocol and experimentally demonstrate the robustness of it against preparation noise stemming for instance from technical laser noise. Provided that direct reconciliation techniques are used in the post-processing we show that for small distances large amounts of preparation noise can be tolerated in contrast to reverse reconciliation where the key rate quickly drops to zero. Our experiment thereby demonstrates that quantum key distribution with non-shot-noise limited laser diodes might be feasible.Comment: 10 pages, 6 figures. Corrected plots for reverse reconciliatio

Single-Quadrature Continuous-Variable Quantum Key Distribution

Most continuous-variable quantum key distribution schemes are based on the Gaussian modulation of coherent states followed by continuous quadrature detection using homodyne detectors. In all previous schemes, the Gaussian modulation has been carried out in conjugate quadratures thus requiring two independent modulators for their implementations. Here, we propose and experimentally test a largely simplified scheme in which the Gaussian modulation is performed in a single quadrature. The scheme is shown to be asymptotically secure against collective attacks, and considers asymmetric preparation and excess noise. A single-quadrature modulation approach renders the need for a costly amplitude modulator unnecessary, and thus facilitates commercialization of continuous-variable quantum key distribution.Comment: 13 pages, 7 figure

Spatially resolved quantum plasmon modes in metallic nano-films from first principles

Electron energy loss spectroscopy (EELS) can be used to probe plasmon excitations in nanostructured materials with atomic-scale spatial resolution. For structures smaller than a few nanometers quantum effects are expected to be important, limiting the validity of widely used semi-classical response models. Here we present a method to identify and compute spatially resolved plasmon modes from first principles based on a spectral analysis of the dynamical dielectric function. As an example we calculate the plasmon modes of 0.5-4 nm thick Na films and find that they can be classified as (conventional) surface modes, sub-surface modes, and a discrete set of bulk modes resembling standing waves across the film. We find clear effects of both quantum confinement and non-local response. The quantum plasmon modes provide an intuitive picture of collective excitations of confined electron systems and offer a clear interpretation of spatially resolved EELS spectra.Comment: 7 pages, 7 figure

Fully selfconsistent GW calculations for molecules

We calculate single-particle excitation energies for a series of 33 molecules using fully selfconsistent GW, one-shot G$_0$W$_0$, Hartree-Fock (HF), and hybrid density functional theory (DFT). All calculations are performed within the projector augmented wave (PAW) method using a basis set of Wannier functions augmented by numerical atomic orbitals. The GW self-energy is calculated on the real frequency axis including its full frequency dependence and off-diagonal matrix elements. The mean absolute error of the ionization potential (IP) with respect to experiment is found to be 4.4, 2.6, 0.8, 0.4, and 0.5 eV for DFT-PBE, DFT-PBE0, HF, G$_0$W$_0$[HF], and selfconsistent GW, respectively. This shows that although electronic screening is weak in molecular systems its inclusion at the GW level reduces the error in the IP by up to 50% relative to unscreened HF. In general GW overscreens the HF energies leading to underestimation of the IPs. The best IPs are obtained from one-shot G$_0$W$_0$ calculations based on HF since this reduces the overscreening. Finally, we find that the inclusion of core-valence exchange is important and can affect the excitation energies by as much as 1 eV.Comment: 10 pages, 5 figure

Plasmons on the edge of MoS2 nanostructures

Using ab initio calculations we predict the existence of one-dimensional (1D), atomically confined plasmons at the edges of a zigzag MoS2 nanoribbon. The strongest plasmon originates from a metallic edge state localized on the sulfur dimers decorating the Mo edge of the ribbon. A detailed analysis of the dielectric function reveals that the observed deviations from the ideal 1D plasmon behavior result from single-particle transitions between the metallic edge state and the valence and conduction bands of the MoS2 sheet. The Mo and S edges of the ribbon are clearly distinguishable in calculated spatially resolved electron energy loss spectrum owing to the different plasmonic properties of the two edges. The edge plasmons could potentially be utilized for tuning the photocatalytic activity of MoS2 nanoparticles

Dynamic rotor mode in antiferromagnetic nanoparticles

We present experimental, numerical, and theoretical evidence for a new mode of antiferromagnetic dynamics in nanoparticles. Elastic neutron scattering experiments on 8 nm particles of hematite display a loss of diffraction intensity with temperature, the intensity vanishing around 150 K. However, the signal from inelastic neutron scattering remains above that temperature, indicating a magnetic system in constant motion. In addition, the precession frequency of the inelastic magnetic signal shows an increase above 100 K. Numerical Langevin simulations of spin dynamics reproduce all measured neutron data and reveal that thermally activated spin canting gives rise to a new type of coherent magnetic precession mode. This "rotor" mode can be seen as a high-temperature version of superparamagnetism and is driven by exchange interactions between the two magnetic sublattices. The frequency of the rotor mode behaves in fair agreement with a simple analytical model, based on a high temperature approximation of the generally accepted Hamiltonian of the system. The extracted model parameters, as the magnetic interaction and the axial anisotropy, are in excellent agreement with results from Mossbauer spectroscopy