12,626 research outputs found
Ideal, Defective, and Gold--Promoted Rutile TiO2(110) Surfaces: Structures, Energies, Dynamics, and Thermodynamics from PBE+U
Extensive first principles calculations are carried out to investigate
gold-promoted TiO2(110) surfaces in terms of structure optimizations,
electronic structure analyses, ab initio thermodynamics calculations of surface
phase diagrams, and ab initio molecular dynamics simulations. All computations
rely on density functional theory in the generalized gradient approximation
(PBE) and account for on-site Coulomb interactions via inclusion of a Hubbard
correction, PBE+U, where U is computed from linear response theory. This
approach is validated by investigating the interaction between TiO2(110)
surfaces and typical probe species (H, H2O, CO). Relaxed structures and binding
energies are compared to both data from the literature and plain PBE results.
The main focus of the study is on the properties of gold-promoted titania
surfaces and their interactions with CO. Both PBE+U and PBE optimized
structures of Au adatoms adsorbed on stoichiometric and reduced TiO2 surfaces
are computed, along with their electronic structure. The charge rearrangement
induced by the adsorbates at the metal/oxide contact are also analyzed and
discussed. By performing PBE+U ab initio molecular dynamics simulations, it is
demonstrated that the diffusion of Au adatoms on the stoichiometric surface is
highly anisotropic. The metal atoms migrate either along the top of the
bridging oxygen rows, or around the area between these rows, from one bridging
position to the next along the [001] direction. Approximate ab initio
thermodynamics predicts that under O-rich conditions, structures obtained by
substituting a Ti5c atom with an Au atom are thermodynamically stable over a
wide range of temperatures and pressures.Comment: 20 pages, 12 figures, accepted for publication in Phys. Rev.
Alternative axiomatics and complexity of deliberative STIT theories
We propose two alternatives to Xu's axiomatization of the Chellas STIT. The
first one also provides an alternative axiomatization of the deliberative STIT.
The second one starts from the idea that the historic necessity operator can be
defined as an abbreviation of operators of agency, and can thus be eliminated
from the logic of the Chellas STIT. The second axiomatization also allows us to
establish that the problem of deciding the satisfiability of a STIT formula
without temporal operators is NP-complete in the single-agent case, and is
NEXPTIME-complete in the multiagent case, both for the deliberative and the
Chellas' STIT.Comment: Submitted to the Journal of Philosophical Logic; 13 pages excluding
anne
Parameterized Approximation Schemes using Graph Widths
Combining the techniques of approximation algorithms and parameterized
complexity has long been considered a promising research area, but relatively
few results are currently known. In this paper we study the parameterized
approximability of a number of problems which are known to be hard to solve
exactly when parameterized by treewidth or clique-width. Our main contribution
is to present a natural randomized rounding technique that extends well-known
ideas and can be used for both of these widths. Applying this very generic
technique we obtain approximation schemes for a number of problems, evading
both polynomial-time inapproximability and parameterized intractability bounds
Wavefunction extended Lagrangian Born-Oppenheimer molecular dynamics
Extended Lagrangian Born-Oppenheimer molecular dynamics [Niklasson, Phys.
Rev. Lett. 100 123004 (2008)] has been generalized to the propagation of the
electronic wavefunctions. The technique allows highly efficient first
principles molecular dynamics simulations using plane wave pseudopotential
electronic structure methods that are stable and energy conserving also under
incomplete and approximate self-consistency convergence. An implementation of
the method within the planewave basis set is presented and the accuracy and
efficiency is demonstrated both for semi-conductor and metallic materials.Comment: 6 pages, 3 figure
Quantum Fluctuations Driven Orientational Disordering: A Finite-Size Scaling Study
The orientational ordering transition is investigated in the quantum
generalization of the anisotropic-planar-rotor model in the low temperature
regime. The phase diagram of the model is first analyzed within the mean-field
approximation. This predicts at a phase transition from the ordered to
the disordered state when the strength of quantum fluctuations, characterized
by the rotational constant , exceeds a critical value . As a function of temperature, mean-field theory predicts a range of
values of where the system develops long-range order upon cooling, but
enters again into a disordered state at sufficiently low temperatures
(reentrance). The model is further studied by means of path integral Monte
Carlo simulations in combination with finite-size scaling techniques,
concentrating on the region of parameter space where reentrance is predicted to
occur. The phase diagram determined from the simulations does not seem to
exhibit reentrant behavior; at intermediate temperatures a pronounced increase
of short-range order is observed rather than a genuine long-range order.Comment: 27 pages, 8 figures, RevTe
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