132,618 research outputs found

### Torsional anharmonicity in the conformational thermodynamics of flexible molecules

We present an algorithm for calculating the conformational thermodynamics of large, flexible molecules that combines ab initio electronic structure theory calculations with a torsional path integral Monte Carlo (TPIMC) simulation. The new algorithm overcomes the previous limitations of the TPIMC method by including the thermodynamic contributions of non-torsional vibrational modes and by affordably incorporating the ab initio calculation of conformer electronic energies, and it improves the conventional ab initio treatment of conformational thermodynamics by accounting for the anharmonicity of the torsional modes. Using previously published ab initio results and new TPIMC calculations, we apply the algorithm to the conformers of the adrenaline molecule

### Frequency shift of cesium clock transition due to blackbody radiation

We have performed ab initio calculations of the frequency shift induced by a
static electric field on the cesium clock hyperfine transition. The
calculations are used to find the frequency shifts due to blackbody radiation.
Our result ($\delta \nu/E^2=-2.26(2)\times 10^{-10}$Hz/(V/m)$^2$) is in good
agreement with early measurements and ab initio calculations performed in other
groups. We present arguments against recent claims that the actual value of the
effect might be smaller. The difference ($\sim$ 10%) between ab initio and
semiempirical calculations is due to the contribution of the continuum spectrum
to the sum over intermediate states.Comment: Accepted for publication in Phys. Rev. Let

### Raman spectra of BN-nanotubes: Ab-initio and bond-polarizability model calculations

We present it ab-initio calculations of the non-resonant Raman spectra of
zigzag and armchair BN nanotubes. In comparison, we implement a generalized
bond-polarizability model where the parameters are extracted from
first-principles calculations of the polarizability tensor of a BN sheet. For
light-polarization along the tube-axis, the agreement between model and it
ab-initio spectra is almost perfect. For perpendicular polarization,
depolarization effects have to be included in the model in order to reproduce
the it ab-initio Raman intensities.Comment: 4 pages, submitted to Phys. Rev. B rapid com

### Ab initio Quantum and ab initio Molecular Dynamics of the Dissociative Adsorption of Hydrogen on Pd(100)

The dissociative adsorption of hydrogen on Pd(100) has been studied by ab
initio quantum dynamics and ab initio molecular dynamics calculations. Treating
all hydrogen degrees of freedom as dynamical coordinates implies a high
dimensionality and requires statistical averages over thousands of
trajectories. An efficient and accurate treatment of such extensive statistics
is achieved in two steps: In a first step we evaluate the ab initio potential
energy surface (PES) and determine an analytical representation. Then, in an
independent second step dynamical calculations are performed on the analytical
representation of the PES. Thus the dissociation dynamics is investigated
without any crucial assumption except for the Born-Oppenheimer approximation
which is anyhow employed when density-functional theory calculations are
performed. The ab initio molecular dynamics is compared to detailed quantum
dynamical calculations on exactly the same ab initio PES. The occurence of
quantum oscillations in the sticking probability as a function of kinetic
energy is addressed. They turn out to be very sensitive to the symmetry of the
initial conditions. At low kinetic energies sticking is dominated by the
steering effect which is illustrated using classical trajectories. The steering
effects depends on the kinetic energy, but not on the mass of the molecules.
Zero-point effects lead to strong differences between quantum and classical
calculations of the sticking probability. The dependence of the sticking
probability on the angle of incidence is analysed; it is found to be in good
agreement with experimental data. The results show that the determination of
the potential energy surface combined with high-dimensional dynamical
calculations, in which all relevant degrees of freedon are taken into account,
leads to a detailed understanding of the dissociation dynamics of hydrogen at a
transition metal surface.Comment: 15 pages, 9 figures, subm. to Phys. Rev.

### Short range correlations and the isospin dependence of nuclear correlation functions

Pair densities and associated correlation functions provide a critical tool
for introducing many-body correlations into a wide-range of effective theories.
Ab initio calculations show that two-nucleon pair-densities exhibit strong spin
and isospin dependence. However, such calculations are not available for all
nuclei of current interest. We therefore provide a simple model, which involves
combining the short and long separation distance behavior using a single
blending function, to accurately describe the two-nucleon correlations inherent
in existing ab initio calculations. We show that the salient features of the
correlation function arise from the features of the two-body short-range
nuclear interaction, and that the suppression of the pp and nn pair-densities
caused by the Pauli principle is important. Our procedure for obtaining
pair-density functions and correlation functions can be applied to heavy nuclei
which lack ab initio calculations.Comment: 5 pages, 4 figure

### A comment on "Ab initio calculations of pressure-dependence of high-order elastic constants using finite deformations approach" by I. Mosyagin, A.V. Lugovskoy, O.M. Krasilnikov, Yu.Kh. Vekilov, S.I. Simak and I.A. Abrikosov

Recently, I. Mosyagin, A.V. Lugovskoy, O.M. Krasilnikov, Yu.Kh. Vekilov, S.I.
Simak and I.A. Abrikosov in the paper: "Ab initio calculations of
pressure-dependence of high-order elastic constants using finite deformations
approach"[Computer Physics Communications 220 (2017) 2030] presented a
description of a technique for ab initio calculations of the pressure
dependence of second- and third-order elastic constants. Unfortunately, the
work contains serious and fundamental flaws in the field of finite-deformation
solid mechanics.Comment: 3 pages, 0 figure

### Structural and electronic properties of silver/silicon interfaces and implications for solar cell performance

We present the results of an experimental and atomistic modelling investigation of the Sili- con/Silver (Si/Ag) interfaces found in industrial solar cells. We use small ab initio calculations to parameterize a new interatomic potential for the Si/Ag interaction. This interatomic potential is then validated against larger ab initio calculations as well as the results of previous experimental and theoretical studies of Si/Ag systems. The interatomic potential allows us to perform a large- scale search of the conformational space of Si/Ag interfaces identified from transmission electron microscopy (TEM) studies. The most favourable geometries thus identified are then used as the input for more accurate ab initio calculations. We demonstrate that the two interfaces which we identify experimentally have significantly different geometric and electronic structures. We also demonstrate how these different structures result in significantly different Schottky barriers at the interfaces

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