707 research outputs found
Hydroxylation Structure and Proton Transfer Reactivity at the Zinc Oxide-Water Interface
The hydroxylation structural features of the first
adsorption layer and its connection to proton transfer reactivity have been studied for the ZnO-liquid water interface at room temperature. Molecular dynamics simulations employing the ReaxFF forcefield were performed for water on seven ZnO surfaces with varying step concentrations. At higher water coverage a higher level of hydroxylation was found, in agreement with previous experimental results. We have also calculated the free energy barrier for transferring a proton to the surface, showing that stepped surfaces stabilize the hydroxylated
state and decrease the water dissociation barrier. On highly stepped surfaces the barrier is only 2 kJ/mol or smaller. Outside the first adsorption layer no dissociation events were found during almost 100 ns of simulation time; this indicates that these reactions are much more likely if catalyzed by the metal oxide surface. Also, when exposed to a vacuum, the less stepped surfaces stabilize adsorption beyond monolayer coverage
Development and Validation of a ReaxFF Reactive Force Field for Cu Cation/Water Interactions and Copper Metal/Metal Oxide/Metal Hydroxide Condensed Phases
To enable large-scale reactive dynamic simulations of copper oxide/water and copper ion/water interactions we have extended the ReaxFF reactive force field framework to Cu/O/H interactions. To this end, we employed a multistage force field development strategy, where the initial training set (containing metal/metal oxide/metal hydroxide condensed phase data and [Cu(H_2O)_n]^(2+) cluster structures and energies) is augmented by single-point quantum mechanices (QM) energies from [Cu(H_2O)_n]^(2+) clusters abstracted from a ReaxFF molecular dynamics simulation. This provides a convenient strategy to both enrich the training set and to validate the final force field. To further validate the force field description we performed molecular dynamics simulations on Cu^(2+)/water systems. We found good agreement between our results and earlier experimental and QM-based molecular dynamics work for the average Cu/water coordination, JahnâTeller distortion, and inversion in [Cu(H_2O)_6]^(2+) clusters and first- and second-shell OâCuâO angular distributions, indicating that this force field gives a satisfactory description of the Cu-cation/water interactions. We believe that this force field provides a computationally convenient method for studying the solution and surface chemistry of metal cations and metal oxides and, as such, has applications for studying protein/metal cation complexes, pH-dependent crystal growth/dissolution, and surface catalysis
Electromagnetic finite-size effects to the hadronic vacuum polarization
In order to reduce the current hadronic uncertainties in the theory
prediction for the anomalous magnetic moment of the muon, lattice calculations
need to reach sub-percent accuracy on the hadronic-vacuum-polarization
contribution. This requires the inclusion of
electromagnetic corrections. The inclusion of electromagnetic interactions in
lattice simulations is known to generate potentially large finite-size effects
suppressed only by powers of the inverse spatial extent. In this paper we
derive an analytic expression for the finite-volume
corrections to the two-pion contribution to the hadronic vacuum polarization at
next-to-leading order in the electromagnetic coupling in scalar QED. The
leading term is found to be of order where is the spatial extent.
A term is absent since the current is neutral and a photon far away
thus sees no charge and we show that this result is universal. Our analytical
results agree with results from the numerical evaluation of loop integrals as
well as simulations of lattice scalar gauge theory with stochastically
generated photon fields. In the latter case the agreement is up to
exponentially suppressed finite-volume effects. For completeness we also
calculate the hadronic vacuum polarization in infinite volume using a basis of
2-loop master integrals.Comment: 42 pages, 11 figure
Interacting supernovae and supernova impostors. SN 2007sv: the major eruption of a massive star in UGC 5979
We report the results of the photometric and spectroscopic monitoring
campaign of the transient SN 2007sv. The observables are similar to those of
type IIn supernovae, a well-known class of objects whose ejecta interact with
pre-existing circum-stellar material. The spectra show a blue continuum at
early phases and prominent Balmer lines in emission, however, the absolute
magnitude at the discovery of SN 2007sv (M_R = - 14.25 +/- 0.38) indicate it to
be most likely a supernova impostor. This classification is also supported by
the lack of evidence in the spectra of very high velocity material as expected
in supernova ejecta. In addition we find no unequivocal evidence of broad lines
of alpha - and/or Fe-peak elements. The comparison with the absolute light
curves of other interacting objects (including type IIn supernovae) highlights
the overall similarity with the prototypical impostor SN 1997bs. This supports
our claim that SN 2007sv was not a genuine supernova, and was instead a
supernova impostor, most likely similar to the major eruption of a luminous
blue variable.Comment: Accepted for publication in MNRAS. 15 pages, 11 figures, 5 table
Aspirin and extended-release dipyridamole versus clopidogrel for recurrent stroke
Background
Recurrent stroke is a frequent, disabling event after ischemic stroke. This study compared
the efficacy and safety of two antiplatelet regimens â aspirin plus extendedrelease
dipyridamole (ASAâERDP) versus clopidogrel.
Methods
In this double-blind, 2-by-2 factorial trial, we randomly assigned patients to receive
25 mg of aspirin plus 200 mg of extended-release dipyridamole twice daily or to receive
75 mg of clopidogrel daily. The primary outcome was first recurrence of stroke.
The secondary outcome was a composite of stroke, myocardial infarction, or death
from vascular causes. Sequential statistical testing of noninferiority (margin of 1.075),
followed by superiority testing, was planned.
Results
A total of 20,332 patients were followed for a mean of 2.5 years. Recurrent stroke
occurred in 916 patients (9.0%) receiving ASAâERDP and in 898 patients (8.8%) receiving
clopidogrel (hazard ratio, 1.01; 95% confidence interval [CI], 0.92 to 1.11). The
secondary outcome occurred in 1333 patients (13.1%) in each group (hazard ratio for
ASAâERDP, 0.99; 95% CI, 0.92 to 1.07). There were more major hemorrhagic events
among ASAâERDP recipients (419 [4.1%]) than among clopidogrel recipients (365
[3.6%]) (hazard ratio, 1.15; 95% CI, 1.00 to 1.32), including intracranial hemorrhage
(hazard ratio, 1.42; 95% CI, 1.11 to 1.83). The net risk of recurrent stroke or major
hemorrhagic event was similar in the two groups (1194 ASAâERDP recipients [11.7%],
vs. 1156 clopidogrel recipients [11.4%]; hazard ratio, 1.03; 95% CI, 0.95 to 1.11).
Conclusions
The trial did not meet the predefined criteria for noninferiority but showed similar rates
of recurrent stroke with ASAâERDP and with clopidogrel. There is no evidence that either
of the two treatments was superior to the other in the prevention of recurrent
stroke. (ClinicalTrials.gov number, NCT00153062.
Transformation kinetics of alloys under non-isothermal conditions
The overall solid-to-solid phase transformation kinetics under non-isothermal
conditions has been modeled by means of a differential equation method. The
method requires provisions for expressions of the fraction of the transformed
phase in equilibrium condition and the relaxation time for transition as
functions of temperature. The thermal history is an input to the model. We have
used the method to calculate the time/temperature variation of the volume
fraction of the favored phase in the alpha-to-beta transition in a zirconium
alloy under heating and cooling, in agreement with experimental results. We
also present a formulation that accounts for both additive and non-additive
phase transformation processes. Moreover, a method based on the concept of path
integral, which considers all the possible paths in thermal histories to reach
the final state, is suggested.Comment: 16 pages, 7 figures. To appear in Modelling Simul. Mater. Sci. En
Isospin-breaking corrections to light leptonic decays in lattice QCD+QED at the physical point
We report on the physical-point RBC/UKQCD calculation of the leading
isospin-breaking corrections to light-meson leptonic decays. This is highly
relevant for future precision tests in the flavour physics sector, in
particular the first-row unitarity of the Cabibbo-Kobayashi-Maskawa matrix
containing the elements and . The simulations were performed
using Domain-Wall fermions for flavours, and with isospin-breaking
effects included perturbatively in the path integral through order and
. We use QED for the
inclusion of electromagnetism, and discuss here the non-locality of this
prescription which has significant impact on the infinite-volume extrapolation.Comment: Proceedings for The 39th International Symposium on Lattice Field
Theory, 8th-13th August, 2022, Rheinische Friedrich-Wilhelms-Universit\"at
Bonn, Bonn, German
The acceleration and storage of radioactive ions for a neutrino factory
The term beta-beam has been coined for the production of a pure beam of
electron neutrinos or their antiparticles through the decay of radioactive ions
circulating in a storage ring. This concept requires radioactive ions to be
accelerated to a Lorentz gamma of 150 for 6He and 60 for 18Ne. The neutrino
source itself consists of a storage ring for this energy range, with long
straight sections in line with the experiment(s). Such a decay ring does not
exist at CERN today, nor does a high-intensity proton source for the production
of the radioactive ions. Nevertheless, the existing CERN accelerator
infrastructure could be used as this would still represent an important saving
for a beta-beam facility. This paper outlines the first study, while some of
the more speculative ideas will need further investigations.Comment: Accepted for publication in proceedings of Nufact02, London, 200
X-ray Diffraction and Molecular Dynamics Study of Medium-range Order in Ambient and Hot Water
We have developed x-ray diffraction measurements with high energy-resolution
and accuracy to study water structure at three different temperatures (7, 25
and 66 C) under normal pressure. Using a spherically curved Ge crystal an
energy resolution better than 15 eV has been achieved which eliminates
influence from Compton scattering. The high quality of the data allows a
precise oxygen-oxygen pair correlation function (PCF) to be directly derived
from the Fourier transform of the experimental data resolving shell structure
out to ~12 {\AA}, i.e. 5 hydration shells. Large-scale molecular dynamics (MD)
simulations using the TIP4P/2005 force-field reproduce excellently the
experimental shell-structure in the range 4-12 {\AA} although less agreement is
seen for the first peak in the PCF. The Local Structure Index [J. Chem. Phys.
104, 7671 (1996)] identifies a tetrahedral minority giving the
intermediate-range oscillations in the PCF and a disordered majority providing
a more featureless background in this range. The current study supports the
proposal that the structure of liquid water, even at high temperatures, can be
described in terms of a two-state fluctuation model involving local structures
related to the high-density and low-density forms of liquid water postulated in
the liquid-liquid phase transition hypothesis.Comment: Submitted to Phys. Chem. Chem. Phy
Real-space local polynomial basis for solid-state electronic-structure calculations: A finite-element approach
We present an approach to solid-state electronic-structure calculations based
on the finite-element method. In this method, the basis functions are strictly
local, piecewise polynomials. Because the basis is composed of polynomials, the
method is completely general and its convergence can be controlled
systematically. Because the basis functions are strictly local in real space,
the method allows for variable resolution in real space; produces sparse,
structured matrices, enabling the effective use of iterative solution methods;
and is well suited to parallel implementation. The method thus combines the
significant advantages of both real-space-grid and basis-oriented approaches
and so promises to be particularly well suited for large, accurate ab initio
calculations. We develop the theory of our approach in detail, discuss
advantages and disadvantages, and report initial results, including the first
fully three-dimensional electronic band structures calculated by the method.Comment: replacement: single spaced, included figures, added journal referenc
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