464 research outputs found
Independent particle descriptions of tunneling from a many-body perspective
Currents across thin insulators are commonly taken as single electrons moving
across classically forbidden regions; this independent particle picture is
well-known to describe most tunneling phenomena. Examining quantum transport
from a different perspective, i.e., by explicit treatment of electron-electron
interactions, we evaluate different single particle approximations with
specific application to tunneling in metal-molecule-metal junctions. We find
maximizing the overlap of a Slater determinant composed of single particle
states to the many-body current-carrying state is more important than energy
minimization for defining single particle approximations in a system with open
boundary conditions. Thus the most suitable single particle effective potential
is not one commonly in use by electronic structure methods, such as the
Hartree-Fock or Kohn-Sham approximations.Comment: 4+ pages, 4 figures; accepted to Phys. Rev. B Rapid Communication
Atomic resolution scanning tunneling microscopy images of Au(111) surfaces in air and polar organic solvents
Atomic features of a close‐packed metal surface have been observed for the first time by scanning tunneling microscopy in organic polar solvents. Evaporated gold films, exhibiting large reconstructed (111) terraces, have been imaged with a resolution far superior to previous results in aqueous environments
Surface stress of Ni adlayers on W(110): the critical role of the surface atomic structure
Puzzling trends in surface stress were reported experimentally for Ni/W(110)
as a function of Ni coverage. In order to explain this behavior, we have
performed a density-functional-theory study of the surface stress and atomic
structure of the pseudomorphic and of several different possible 1x7
configurations for this system. For the 1x7 phase, we predict a different, more
regular atomic structure than previously proposed based on surface x-ray
diffraction. At the same time, we reproduce the unexpected experimental change
of surface stress between the pseudomorphic and 1x7 configuration along the
crystallographic surface direction which does not undergo density changes. We
show that the observed behavior in the surface stress is dominated by the
effect of a change in Ni adsorption/coordination sites on the W(110) surface.Comment: 14 pages, 3 figures Published in J. Phys.: Condens. Matter 24 (2012)
13500
Effects of asymmetric contacts on single molecule conductances of HS(CH2)nCOOH in nano-electrical junctions
A scanning tunnelling microscope has been used to determine the conductance of single molecular wires with the configuration X-bridge-X, X-bridge-Y and Y-bridge-Y (X = thiol terminus and Y = COOH). We find that for molecular wires with mixed functional groups (X-bridge-Y) the single molecule conductance decreases with respect to the comparable symmetric molecules. These differences are confirmed by theoretical computations based on a combination of density functional theory and the non-equilibrium Green functions formalism. This study demonstrates that the apparent contact resistance, as well as being highly sensitive to the type of the anchoring group is also strongly influenced by contact-asymmetry of the single molecular junction which in this case decreases the transmission. This highlights that contact asymmetry is a significant factor to be considered when evaluating nano-electrical junctions incorporating single molecules
Large-Scale Atomistic Simulations of Environmental Effects on the Formation and Properties of Molecular Junctions
Using an updated simulation tool, we examine molecular junctions comprised of
benzene-1,4-dithiolate bonded between gold nanotips, focusing on the importance
of environmental factors and inter-electrode distance on the formation and
structure of bridged molecules. We investigate the complex relationship between
monolayer density and tip separation, finding that the formation of
multi-molecule junctions is favored at low monolayer density, while
single-molecule junctions are favored at high density. We demonstrate that tip
geometry and monolayer interactions, two factors that are often neglected in
simulation, affect the bonding geometry and tilt angle of bridged molecules. We
further show that the structures of bridged molecules at 298 and 77 K are
similar.Comment: To appear in ACS Nano, 30 pages, 5 figure
Stabilizing single atom contacts by molecular bridge formation
Gold-molecule-gold junctions can be formed by carefully breaking a gold wire
in a solution containing dithiolated molecules. Surprisingly, there is little
understanding on the mechanical details of the bridge formation process and
specifically on the role that the dithiol molecules play themselves. We propose
that alkanedithiol molecules have already formed bridges between the gold
electrodes before the atomic gold-gold junction is broken. This leads to
stabilization of the single atomic gold junction, as observed experimentally.
Our data can be understood within a simple spring model.Comment: 14 pages, 3 figures, 1 tabl
Finite size effects on transport coefficients for models of atomic wires coupled to phonons
We consider models of quasi-1-d, planar atomic wires consisting of several,
laterally coupled rows of atoms, with mutually non-interacting electrons. This
electronic wire system is coupled to phonons, corresponding, e.g., to some
substrate. We aim at computing diffusion coefficients in dependence on the wire
widths and the lateral coupling. To this end we firstly construct a numerically
manageable linear collision term for the dynamics of the electronic occupation
numbers by following a certain projection operator approach. By means of this
collision term we set up a linear Boltzmann equation. A formula for extracting
diffusion coefficients from such Boltzmann equations is given. We find in the
regime of a few atomic rows and intermediate lateral coupling a significant and
non-trivial dependence of the diffusion coefficient on both, the width and the
lateral coupling. These results, in principle, suggest the possible
applicability of such atomic wires as electronic devices, such as, e.g.,
switches.Comment: 9 pages, 5 figures, accepted for publication in Eur. Phys. J.
Conductance statistics from a large array of sub-10 nm molecular junctions
Devices made of few molecules constitute the miniaturization limit that both
inorganic and organic-based electronics aspire to reach. However, integration
of millions of molecular junctions with less than 100 molecules each has been a
long technological challenge requiring well controlled nanometric electrodes.
Here we report molecular junctions fabricated on a large array of sub-10 nm
single crystal Au nanodots electrodes, a new approach that allows us to measure
the conductance of up to a million of junctions in a single conducting Atomic
Force Microscope (C-AFM) image. We observe two peaks of conductance for
alkylthiol molecules. Tunneling decay constant (beta) for alkanethiols, is in
the same range as previous studies. Energy position of molecular orbitals,
obtained by transient voltage spectroscopy, varies from peak to peak, in
correlation with conductance values.Comment: ACS Nano (in press
Relaxation and reconstruction on (111) surfaces of Au, Pt, and Cu
We have theoretically studied the stability and reconstruction of (111)
surfaces of Au, Pt, and Cu. We have calculated the surface energy, surface
stress, interatomic force constants, and other relevant quantities by ab initio
electronic structure calculations using the density functional theory (DFT), in
a slab geometry with periodic boundary conditions. We have estimated the
stability towards a quasi-one-dimensional reconstruction by using the
calculated quantities as parameters in a one-dimensional Frenkel-Kontorova
model. On all surfaces we have found an intrinsic tensile stress. This stress
is large enough on Au and Pt surfaces to lead to a reconstruction in which a
denser surface layer is formed, in agreement with experiment. The
experimentally observed differences between the dense reconstruction pattern on
Au(111) and a sparse structure of stripes on Pt(111) are attributed to the
details of the interaction potential between the first layer of atoms and the
substrate.Comment: 8 pages, 3 figures, submitted to Physical Review
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
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