4,484 research outputs found
Time-dependent i-DFT exchange-correlation potentials with memory: Applications to the out-of-equilibrium Anderson model
We have recently put forward a steady-state density functional theory (i-DFT)
to calculate the transport coefficients of quantum junctions. Within i-DFT it
is possible to obtain the steady density on and the steady current through an
interacting junction using a fictitious noninteracting junction subject to an
effective gate and bias potential. In this work we extend i-DFT to the time
domain for the single-impurity Anderson model. By a reverse engineering
procedure we extract the exchange-correlation (xc) potential and xc bias at
temperatures above the Kondo temperature . The derivation is based
on a generalization of a recent paper by Dittmann et al. [arXiv:1706.04547].
Interestingly the time-dependent (TD) i-DFT potentials depend on the system's
history only through the first time-derivative of the density. We perform
numerical simulations of the early transient current and investigate the role
of the history dependence. We also empirically extend the history-dependent TD
i-DFT potentials to temperatures below . For this purpose we use a
recently proposed parametrization of the i-DFT potentials which yields highly
accurate results in the steady state.Comment: 7 pages, 4 figure
AC transport in Correlated Quantum Dots: From Kondo to Coulomb blockade regime
We explore the finite bias DC differential conductance of a correlated
quantum dot under the influence of an AC field, from the low-temperature Kondo
to the finite temperature Coulomb blockade regime. Real-time simulations are
performed using a time-dependent generalization of the steady-state density
functional theory (i-DFT) [Nano Lett. {\bf 15}, 8020 (2015)]. The numerical
simplicity of i-DFT allows for unprecedented long time evolutions. Accurate
values of average current and density are obtained by integrating over several
periods of the AC field. We find that (i) the zero-temperature Kondo plateau is
suppressed, (ii) the photon-assisted conductance peaks are shifted due to
correlations and (iii) the Coulomb blockade is lifted with a concomitant
smoothening of the sharp diamond edges.Comment: 5 pages, 4 figure
Dynamical correction to linear Kohn-Sham conductances from static density functional theory
For molecules weakly coupled to leads the exact linear Kohn-Sham (KS)
conductance can be orders of magnitude larger than the true linear conductance
due to the lack of dynamical exchange-correlation (xc) corrections. In this
work we show how to incorporate dynamical effects in KS transport calculations.
The only quantity needed is the static xc potential in the molecular junction.
Our scheme provides a comprehensive description of Coulomb blockade without
breaking the spin symmetry. This is explicitly demonstrated in single-wall
nanotubes where the corrected conductance is in good agreement with
experimental data whereas the KS conductance fails dramatically.Comment: 5 pages (4 figures) + 3 pages (2 figures) Supplemental Materia
Transport through correlated systems with density functional theory
We present recent advances in Density Functional Theory (DFT) for
applications to the field of quantum transport, with particular emphasis on
transport through strongly correlated systems. We review the foundations of the
popular Landauer-B\"uttiker(LB)+DFT approach. This formalism, when using
approximations to the exchange-correlation (xc) potential with steps at integer
occupation, correctly captures the Kondo plateau in the zero bias conductance
at zero temperature but completely fails to capture the transition to the
Coulomb blockade (CB) regime as temperature increases. To overcome the
limitations of LB+DFT the quantum transport problem is treated from a
time-dependent (TD) perspective using TDDFT, an exact framework to deal with
nonequilibrium situations. The steady-state limit of TDDFT shows that in
addition to an xc potential in the junction, there also exists an xc correction
to the applied bias. Open shell molecules in the CB regime provide the most
striking examples of the importance of the xc bias correction. Using the
Anderson model as guidance we estimate these corrections in the limit of zero
bias. For the general case we put forward a steady-state DFT which is based on
the one-to-one correspondence between the pair of basic variables steady
density on and steady current across the junction and the pair local potential
on and bias across the junction. Like TDDFT, this framework also leads to both
an xc potential in the junction and an xc correction to the bias. Unlike in
TDDFT, these potentials are independent of history. We highlight the universal
features of both xc potential and xc bias corrections for junctions in the CB
regime and provide an accurate parametrization for the Anderson model at
arbitrary temperatures and interaction strengths thus providing a unified DFT
description for both Kondo and CB regimes and the transition between them.Comment: 29 pages, 22 Figure
Monomolecular layers and thin films of silane coupling agents by vapor-phase adsorption on oxidized aluminum
Thin films of tetraethoxysilane [TEOS], (3-bromopropyl)trimethoxysilane [BPS], trimethoxyvinylsilane [VS], and 3-(tri-methoxysily1)propyl methacrylate [TPM] on oxidized aluminum surfaces have been investigated by reflection-absorption FTIR spectroscopy, ellipsometry, contact angle, and quartz crystal microbalance (QCM) measurements. Gravimetric measurements with the QCM can reveal quantitative aspects of adsorption and film formation, even for films as thin as monolayers. Adsorption of these silane coupling agents from solution typically produces multilayer films. Vapor-phase adsorption of TEOS and TPM at room temperature results in monomolecular layers. The coupling agents VS and BPS require additional heating after the vapor-phase adsorption to initiate the hydrolysis and condensation reactions necessary for the surface attachment, which produces one to three layers. For vapor adsorbed films a packing density of 4-7 molecules/nm2 was found. The data strongly suggest that the organic moieties in several of these films have a preferential orientation on the surface; they can be viewed as two-dimensional, oligomeric siloxane networks with oriented organic chains. Subsequent heating of TPM films results in structural rearrangements; heating of TEOS results in complete condensation to Si02 films
Quantifizierung der Reaktivität von 3-Aminopropyltriethoxysilan-Monoschichten mit der Quarzmikrowaage
A time-dependent approach to electron pumping in open quantum systems
We propose a time-dependent approach to investigate the motion of electrons
in quantum pump device configurations. The occupied one-particle states are
propagated in real time and used to calculate the local electron density and
current. An advantage of the present computational scheme is that the same
computational effort is required to simulate monochromatic, polychromatic and
nonperiodic drivings. Furthermore, initial state dependence and history effects
are naturally accounted for. This approach can also be embedded in the
framework of time-dependent density functional theory to include
electron-electron interactions. In the special case of periodic drivings we
combine the Floquet theory with nonequilibrium Green's functions and obtain a
general expression for the pumped current in terms of inelastic transmission
probabilities. This latter result is used for benchmarking our propagation
scheme in the long-time limit. Finally, we discuss the limitations of
Floquet-based schemes and suggest our approach as a possible way to go beyond
them.Comment: 14 pages, 8 figure
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