6,815 research outputs found
Charge-transfer in time-dependent density-functional theory via spin-symmetry-breaking
Long-range charge-transfer excitations pose a major challenge for
time-dependent density functional approximations. We show that
spin-symmetry-breaking offers a simple solution for molecules composed of
open-shell fragments, yielding accurate excitations at large separations when
the acceptor effectively contains one active electron. Unrestricted
exact-exchange and self-interaction-corrected functionals are performed on
one-dimensional models and the real LiH molecule within the pseudopotential
approximation to demonstrate our results.Comment: 5 pages, 4 figure
Self-consistent DFT+U method for real-space time-dependent density functional theory calculations
We implemented various DFT+U schemes, including the ACBN0 self-consistent
density-functional version of the DFT+U method [Phys. Rev. X 5, 011006 (2015)]
within the massively parallel real-space time-dependent density functional
theory (TDDFT) code Octopus. We further extended the method to the case of the
calculation of response functions with real-time TDDFT+U and to the description
of non-collinear spin systems. The implementation is tested by investigating
the ground-state and optical properties of various transition metal oxides,
bulk topological insulators, and molecules. Our results are found to be in good
agreement with previously published results for both the electronic band
structure and structural properties. The self consistent calculated values of U
and J are also in good agreement with the values commonly used in the
literature. We found that the time-dependent extension of the self-consistent
DFT+U method yields improved optical properties when compared to the empirical
TDDFT+U scheme. This work thus opens a different theoretical framework to
address the non equilibrium properties of correlated systems
Universal Dynamical Steps in the Exact Time-Dependent Exchange-Correlation Potential
We show that the exact exchange-correlation potential of time-dependent
density-functional theory displays dynamical step structures that have a
spatially non-local and time non-local dependence on the density. Using
one-dimensional two-electron model systems, we illustrate these steps for a
range of non-equilibrium dynamical situations relevant for modeling of
photo-chemical/physical processes: field-free evolution of a non-stationary
state, resonant local excitation, resonant complete charge-transfer, and
evolution under an arbitrary field. Lack of these steps in usual approximations
yield inaccurate dynamics, for example predicting faster dynamics and
incomplete charge transfer
Importance of Acid–Base Equilibrium in Electrocatalytic Oxidation of Formic Acid on Platinum
This work was supported by Japanese Society for the Promotion of Science (JSPS) KAKENHI Grants Nos. 24550143 and 24750117 and MEXT Project of Integrated Research on Chemical Synthesis. M.T.M.K. gratefully acknowledges the award of Long-Term Fellowship of JSPS (No. L-11527) and Visiting Professorship of Hokkaido University. T.U. acknowledges Grants-in-Aid for Regional R&D Proposal-Based Program from Northern Advancement Center for Science & Technology of Hokkaido, Japan. J.J. acknowledges scholarship of Asian Graduate School, Hokkaido University.Peer reviewedPostprin
On the use of Neumann's principle for the calculation of the polarizability tensor of nanostructures
The polarizability measures how the system responds to an applied electrical
field. Computationally, there are many different ways to evaluate this
tensorial quantity, some of which rely on the explicit use of the external
perturbation and require several individual calculations to obtain the full
tensor. In this work, we present some considerations about symmetry that allow
us to take full advantage of Neumann's principle and decrease the number of
calculations required by these methods. We illustrate the approach with two
examples, the use of the symmetries in real space and in spin space in the
calculation of the electrical or the spin response.Comment: 7 pages, 5 figures, accepted for publication in the Journal of
Nanoscience and Nanotechnolog
Condensation transitions in a model for a directed network with weighted links
An exactly solvable model for the rewiring dynamics of weighted, directed
networks is introduced. Simulations indicate that the model exhibits two types
of condensation: (i) a phase in which, for each node, a finite fraction of its
total out-strength condenses onto a single link; (ii) a phase in which a finite
fraction of the total weight in the system is directed into a single node. A
virtue of the model is that its dynamics can be mapped onto those of a
zero-range process with many species of interacting particles -- an exactly
solvable model of particles hopping between the sites of a lattice. This
mapping, which is described in detail, guides the analysis of the steady state
of the network model and leads to theoretical predictions for the conditions
under which the different types of condensation may be observed. A further
advantage of the mapping is that, by exploiting what is known about exactly
solvable generalisations of the zero-range process, one can infer a number of
generalisations of the network model and dynamics which remain exactly
solvable.Comment: 23 pages, 8 figure
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