Ab initio GW electron-electron interaction effects in Quantum Transport

We present an ab initio approach to electronic transport in nanoscale systems which includes electronic correlations through the GW approximation. With respect to Landauer approaches based on density-functional theory (DFT), we introduce a physical quasiparticle electronic-structure into a non-equilibrium Green's function theory framework. We use an equilibrium non-selfconsistent $G^0W^0$ self-energy considering both full non-hermiticity and dynamical effects. The method is applied to a real system, a gold mono-atomic chain. With respect to DFT results, the conductance profile is modified and reduced by to the introduction of diffusion and loss-of-coherence effects. The linear response conductance characteristic appear to be in agreement with experimental results.Comment: 5 pages, 4 figures, refused by PR

Monolayer and Bilayer Perfluoropentacene on Cu(111)

Perfluoropentacene (PFP), an n-type organic semiconductor, is deposited at monolayer and bilayer coverages on Cu(111). Scanning tunneling microscopy at various bias voltages is used to investigate the geometric and electronic structures of the layer. The appearances of the first layer and second layer differ, likely due to perturbation of the first layer electronic structure by the substrate. This has been previously observed for pentacene (Pn), the isostructural p-type organic semiconductor. The PFP film has a unit cell of (4, −3,3 4) relative to the substrate, which is larger than that of Pn/Cu(111), representing a half-integer increment in each direction

Amine-Gold Linked Single-Molecule Junctions: Experiment and Theory

The measured conductance distribution for single molecule benzenediamine-gold junctions, based on 59,000 individual conductance traces recorded while breaking a gold point contact in solution, has a clear peak at 0.0064 G$_{0}$ with a width of $\pm$ 40%. Conductance calculations based on density functional theory (DFT) for 15 distinct junction geometries show a similar spread. Differences in local structure have a limited influence on conductance because the amine-Au bonding motif is well-defined and flexible. The average calculated conductance (0.046 G$_{0}$) is seven times larger than experiment, suggesting the importance of many-electron corrections beyond DFT

Orbital textures and charge density waves in transition metal dichalcogenides

Low-dimensional electron systems, as realized naturally in graphene or created artificially at the interfaces of heterostructures, exhibit a variety of fascinating quantum phenomena with great prospects for future applications. Once electrons are confined to low dimensions, they also tend to spontaneously break the symmetry of the underlying nuclear lattice by forming so-called density waves; a state of matter that currently attracts enormous attention because of its relation to various unconventional electronic properties. In this study we reveal a remarkable and surprising feature of charge density waves (CDWs), namely their intimate relation to orbital order. For the prototypical material 1T-TaS2 we not only show that the CDW within the two-dimensional TaS2-layers involves previously unidentified orbital textures of great complexity. We also demonstrate that two metastable stackings of the orbitally ordered layers allow to manipulate salient features of the electronic structure. Indeed, these orbital effects enable to switch the properties of 1T-TaS2 nanostructures from metallic to semiconducting with technologically pertinent gaps of the order of 200 meV. This new type of orbitronics is especially relevant for the ongoing development of novel, miniaturized and ultra-fast devices based on layered transition metal dichalcogenides

Infrared Nanoimaging of Hydrogenated Perovskite Nickelate Synaptic Devices

Solid-state devices made from correlated oxides such as perovskite nickelates are promising for neuromorphic computing by mimicking biological synaptic function. However, comprehending dopant action at the nanoscale poses a formidable challenge to understanding the elementary mechanisms involved. Here, we perform operando infrared nanoimaging of hydrogen-doped correlated perovskite, neodymium nickel oxide (H-NdNiO3) devices and reveal how an applied field perturbs dopant distribution at the nanoscale. This perturbation leads to stripe phases of varying conductivity perpendicular to the applied field, which define the macroscale electrical characteristics of the devices. Hyperspectral nano-FTIR imaging in conjunction with density functional theory calculations unveil a real-space map of multiple vibrational states of H-NNO associated with OH stretching modes and their dependence on the dopant concentration. Moreover, the localization of excess charges induces an out-of-plane lattice expansion in NNO which was confirmed by in-situ - x-ray diffraction and creates a strain that acts as a barrier against further diffusion. Our results and the techniques presented here hold great potential to the rapidly growing field of memristors and neuromorphic devices wherein nanoscale ion motion is fundamentally responsible for function.Comment: 30 pages, 5 figures in the main text and 5 figures in the Supplementary Materia

Goos-H\"{a}nchen-like shifts for Dirac fermions in monolayer graphene barrier

We investigate the Goos-H\"{a}nchen-like shifts for Dirac fermions in transmission through a monolayer graphene barrier. The lateral shifts, as the functions of the barrier's width and the incidence angle, can be negative and positive in Klein tunneling and classical motion, respectively. Due to their relations to the transmission gap, the lateral shifts can be enhanced by the transmission resonances when the incidence angle is less than the critical angle for total reflection, while their magnitudes become only the order of Fermi wavelength when the incidence angle is larger than the critical angle. These tunable beam shifts can also be modulated by the height of potential barrier and the induced gap, which gives rise to the applications in graphene-based devices.Comment: 5 pages, 5 figure

Highly Conducting pi-Conjugated Molecular Junctions Covalently Bonded to Gold Electrodes

We measure electronic conductance through single conjugated molecules bonded to Au metal electrodes with direct Au-C covalent bonds using the scanning tunneling microscope based break-junction technique. We start with molecules terminated with trimethyltin end groups that cleave off in situ resulting in formation of a direct covalent sigma bond between the carbon backbone and the gold metal electrodes. The molecular carbon backbone used in this study consist of a conjugated pi-system that has one terminal methylene group on each end, which bonds to the electrodes, achieving large electronic coupling of the electrodes to the pi-system. The junctions formed with the prototypical example of 1,4-dimethylenebenzene show a conductance approaching one conductance quantum (G0 = 2e2/h). Junctions formed with methylene terminated oligophenyls with two to four phenyl units show a hundred-fold increase in conductance compared with junctions formed with amine-linked oligophenyls. The conduction mechanism for these longer oligophenyls is tunneling as they exhibit an exponential dependence of conductance with oligomer length. In addition, density functional theory based calculations for the Au-xylylene-Au junction show near-resonant transmission with a cross-over to tunneling for the longer oligomers.Comment: Accepted to the Journal of the American Chemical Society as a Communication

Quantum Resistance Standard Based on Epitaxial Graphene

We report development of a quantum Hall resistance standard accurate to a few parts in a billion at 300 mK and based on large area epitaxial graphene. The remarkable precision constitutes an improvement of four orders of magnitude over the best results obtained in exfoliated graphene and is similar to the accuracy achieved in well-established semiconductor standards. Unlike the traditional resistance standards the novel graphene device is still accurately quantized at 4.2 K, vastly simplifying practical metrology. This breakthrough was made possible by exceptional graphene quality achieved with scalable silicon carbide technology on a wafer scale and shows great promise for future large scale applications in electronics.Comment: Submitte

Spin Channels in Functionalized Graphene Nanoribbons

We characterize the transport properties of functionalized graphene nanoribbons using extensive first-principles calculations based on density functional theory (DFT) that encompass both monovalent and divalent ligands, hydrogenated defects and vacancies. We find that the edge metallic states are preserved under a variety of chemical environments, while bulk conducting channels can be easily destroyed by either hydrogenation or ion or electron beams, resulting in devices that can exhibit spin conductance polarization close to unity.Comment: 14 pages, 5 figure