1,700 research outputs found
Non-adiabatic Effects in the Dissociation of Oxygen Molecules at the Al(111) Surface
The measured low initial sticking probability of oxygen molecules at the
Al(111) surface that had puzzled the field for many years was recently
explained in a non-adiabatic picture invoking spin-selection rules [J. Behler
et al., Phys. Rev. Lett. 94, 036104 (2005)]. These selection rules tend to
conserve the initial spin-triplet character of the free O2 molecule during the
molecule's approach to the surface. A new locally-constrained
density-functional theory approach gave access to the corresponding
potential-energy surface (PES) seen by such an impinging spin-triplet molecule
and indicated barriers to dissociation which reduce the sticking probability.
Here, we further substantiate this non-adiabatic picture by providing a
detailed account of the employed approach. Building on the previous work, we
focus in particular on inaccuracies in present-day exchange-correlation
functionals. Our analysis shows that small quantitative differences in the
spin-triplet constrained PES obtained with different gradient-corrected
functionals have a noticeable effect on the lowest kinetic energy part of the
resulting sticking curve.Comment: 17 pages including 11 figures; related publications can be found at
http://www.fhi-berlin.mpg.de/th/th.htm
Mouse precision-cut liver slices as an ex vivo model to study drug-induced cholestasis
Drugs are often withdrawn from the market due to the manifestation of drug-induced liver injury (DILI) in patients. Drug-induced cholestasis (DIC), defined as obstruction of hepatic bile flow due to medication, is one form of DILI. Because DILI is idiosyncratic, and the resulting cholestasis complex, there is no suitable in vitro model for early DIC detection during drug development. Our goal was to develop a mouse precision-cut liver slice (mPCLS) model to study DIC and to assess cholestasis development using conventional molecular biology and analytical chemistry methods. Cholestasis was induced in mPCLS through a 48-h-incubation with three drugs known to induce cholestasis in humans, namely chlorpromazine (15, 20, and 30 µM), cyclosporin A (1, 3, and 6 µM) or glibenclamide (25, 50, and 65 µM). A bile-acid mixture (16 µM) that is physiologically representative of the human bile-acid pool was added to the incubation medium with drug, and results were compared to incubations with no added bile acids. Treatment of PCLS with cholestatic drugs increased the intracellular bile-acid concentration of deoxycholic acid and modulated bile-transporter genes. Chlorpromazine led to the most pronounced cholestasis in 48 h, observed as increased toxicity; decreased protein and gene expression of the bile salt export pump; increased gene expression of multidrug resistance-associated protein 4; and accumulation of intracellular bile acids. Moreover, chlorpromazine-induced cholestasis exhibited some transition into fibrosis, evidenced by increased gene expression of collagen 1A1 and heatshock protein 47. In conclusion, we demonstrate that mPCLS can be used to study human DIC onset and progression in a 48 h period. We thus propose this model is suited for other similar studies of human DIC
Remark on Pauli-Villars Lagrangian on the Lattice
It is interesting to superimpose the Pauli-Villars regularization on the
lattice regularization. We illustrate how this scheme works by evaluating the
axial anomaly in a simple lattice fermion model, the Pauli-Villars Lagrangian
with a gauge non-invariant Wilson term. The gauge non-invariance of the axial
anomaly, caused by the Wilson term, is remedied by a compensation among
Pauli-Villars regulators in the continuum limit. A subtlety in Frolov-Slavnov's
scheme for an odd number of chiral fermions in an anomaly free complex gauge
representation, which requires an infinite number of regulators, is briefly
mentioned.Comment: 14 pages, Phyzzx. The final version to appear in Phys. Rev.
Constraints on the Existence of Chiral Fermions in Interacting Lattice Theories
It is shown that an interacting theory, defined on a regular lattice, must
have a vector-like spectrum if the following conditions are satisfied:
(a)~locality, (b)~relativistic continuum limit without massless bosons, and
(c)~pole-free effective vertex functions for conserved currents.
The proof exploits the zero frequency inverse retarded propagator of an
appropriate set of interpolating fields as an effective quadratic hamiltonian,
to which the Nielsen-Ninomiya theorem is applied.Comment: LaTeX, 9 pages, WIS--93/56--JUNE--P
A New Look at the Axial Anomaly in Lattice QED with Wilson Fermions
By carrying out a systematic expansion of Feynman integrals in the lattice
spacing, we show that the axial anomaly in the U(1) lattice gauge theory with
Wilson fermions, as determined in one-loop order from an irrelevant lattice
operator in the Ward identity, must necessarily be identical to that computed
from the dimensionally regulated continuum Feynman integrals for the triangle
diagrams.Comment: 1 figure, LaTeX, 18 page
Room temperature structure and energetics of water-hydroxyl layers on Pt(111)
The interactions between water and hydroxyl species on Pt(111) surfaces have
been intensely investigated due to their importance to fuel cell
electrocatalysis. Here we present a room temperature molecular dynamics study
of their structure and energetics using an ensemble of neural network
potentials, which allow us to obtain unprecedented statistical sampling. We
first study the energetics of hydroxyl formation, where we find a near-linear
adsorption energy profile, which exhibits a soft and gradual increase in the
differential adsorption energy at high hydroxyl coverages. This is strikingly
different from the predictions of the conventional bilayer model, which
displays a kink at 1/3ML OH coverage indicating a sizeable jump in differential
adsorption energy, but within the statistical uncertainty of previously
reported ab initio molecular dynamics studies. We then analyze the structure of
the interface, where we provide evidence for the water-OH/Pt(111) interface
being hydrophobic at high hydroxyl coverages. We furthermore explain the
observed adsorption energetics by analyzing the hydrogen bonding in the
water-hydroxyl adlayers, where we argue that the increase in differential
adsorption energy at high OH coverage can be explained by a reduction in the
number of hydrogen bonds from the adsorbed water molecules to the hydroxyls
Local-metrics error-based Shepard interpolation as surrogate for highly non- linear material models in high dimensions
Many problems in computational materials science and chemistry require the
evaluation of expensive functions with locally rapid changes, such as the
turn-over frequency of first principles kinetic Monte Carlo models for
heterogeneous catalysis. Because of the high computational cost, it is often
desirable to replace the original with a surrogate model, e.g., for use in
coupled multiscale simulations. The construction of surrogates becomes
particularly challenging in high-dimensions. Here, we present a novel version
of the modified Shepard interpolation method which can overcome the curse of
dimensionality for such functions to give faithful reconstructions even from
very modest numbers of function evaluations. The introduction of local metrics
allows us to take advantage of the fact that, on a local scale, rapid
variation often occurs only across a small number of directions. Furthermore,
we use local error estimates to weigh different local approximations, which
helps avoid artificial oscillations. Finally, we test our approach on a number
of challenging analytic functions as well as a realistic kinetic Monte Carlo
model. Our method not only outperforms existing isotropic metric Shepard
methods but also state-of-the-art Gaussian process regression
Analysis of Granular Packing Structure by Scattering of THz Radiation
Scattering methods are widespread used to characterize the structure and
constituents of matter on small length scales. This motivates this introductory
text on identifying prospective approaches to scattering-based methods for
granular media. A survey to light scattering by particles and particle
ensembles is given. It is elaborated why the established scattering methods
using X-rays and visible light cannot in general be transferred to granular
media. Spectroscopic measurements using Terahertz radiation are highlighted as
they to probe the scattering properties of granular media, which are sensitive
to the packing structure. Experimental details to optimize spectrometer for
measurements on granular media are discussed. We perform transmission
measurements on static and agitated granular media using Fourier-transform
spectroscopy at the THz beamline of the BessyII storage ring. The measurements
demonstrate the potential to evaluate degrees of order in the media and to
track transient structural states in agitated bulk granular media.Comment: 12 Pages, 9 Figures, 56 Reference
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