3,800 research outputs found
Computational spectroscopy of helium-solvated molecules: effective inertia, from small He clusters toward the nano-droplet regime
Accurate computer simulations of the rotational dynamics of linear molecules
solvated in He clusters indicate that the large-size (nano-droplet) regime is
attained quickly for light rotors (HCN, CO) and slowly for heavy ones (OCS,
NO, CO), thus challenging previously reported results. Those results
spurred the view that the different behavior of light rotors with respect to
heavy ones - including a smaller reduction of inertia upon solvation of the
former - would result from the lack of adiabatic following of the He density
upon molecular rotation. We have performed computer experiments in which the
rotational dynamics of OCS and HCN molecules was simulated using a fictitious
inertia appropriate to the other molecule. These experiments indicate that the
approach to the nano-droplet regime, as well as the reduction of the molecular
inertia upon solvation, is determined by the anistropy of the potential, more
than by the molecular weight. Our findings are in agreement with recent
infrared and/or microwave experimental data which, however, are not yet totally
conclusive by themselves.Comment: 11 pages, 13 figure
Accurate quadratic-response approximation for the self-consistent pseudopotential of semiconductor nanostructures
Quadratic-response theory is shown to provide a conceptually simple but
accurate approximation for the self-consistent one-electron potential of
semiconductor nanostructures. Numerical examples are presented for GaAs/AlAs
and InGaAs/InP (001) superlattices using the local-density approximation to
density-functional theory and norm-conserving pseudopotentials without
spin-orbit coupling. When the reference crystal is chosen to be the
virtual-crystal average of the two bulk constituents, the absolute error in the
quadratic-response potential for Gamma(15) valence electrons is about 2 meV for
GaAs/AlAs and 5 meV for InGaAs/InP. Low-order multipole expansions of the
electron density and potential response are shown to be accurate throughout a
small neighborhood of each reciprocal lattice vector, thus providing a further
simplification that is confirmed to be valid for slowly varying envelope
functions. Although the linear response is about an order of magnitude larger
than the quadratic response, the quadratic terms are important both
quantitatively (if an accuracy of better than a few tens of meV is desired) and
qualitatively (due to their different symmetry and long-range dipole effects).Comment: 16 pages, 20 figures; v2: new section on limitations of theor
On-surface and Subsurface Adsorption of Oxygen on Stepped Ag(210) and Ag(410) Surfaces
The adsorption of atomic oxygen and its inclusion into subsurface sites on
Ag(210) and Ag(410) surfaces have been investigated using density functional
theory. We find that--in the absence of adatoms on the first metal
layer--subsurface adsorption results in strong lattice distortion which makes
it energetically unfavoured. However subsurface sites are significantly
stabilised when a sufficient amount of O adatoms is present on the surface. At
high enough O coverage on the Ag(210) surface the mixed on-surface + subsurface
O adsorption is energetically favoured with respect to the on-surface only
adsorption. Instead, on the Ag(410) surface, at the coverage we have considered
(3/8 ML), the existence of stable terrace sites makes the subsurface O
incorporation less favourable. These findings are compatible with the results
of recent HREEL experiments which have actually motivated this work.Comment: 8 pages, 4 figures and 1 tabl
Electron-vibration coupling constants in positively charged fullerene
Recent experiments have shown that C60 can be positively field-doped. In that
state, fullerene exhibits a higher resistivity and a higher superconducting
temperature than the corresponding negatively doped state. A strong
intramolecular hole-phonon coupling, connected with the Jahn-Teller effect of
the isolated positive ion, is expected to be important for both properties, but
the actual coupling strengths are so far unknown. Based on density functional
calculations, we determine the linear couplings of the two a_g, six g_g, and
eight h_g vibrational modes to the H_u HOMO level of the C60 molecule. The
couplings predict a D_5 distortion, and an H_u vibronic ground state for C60^+.
They are also used to generate the dimensionless coupling constant
which controls the superconductivity and the phonon contribution to the
electrical resistivity in the crystalline phase. We find that is 1.4
times larger in positively-charged C60 than in the negatively-doped case. These
results are discussed in the context of the available transport data and
superconducting temperatures. The role of higher orbital degeneracy in
superconductivity is also addressed.Comment: 22 pages - 3 figures. This revision includes few punctuation
corrections from proofreadin
Elimination of unoccupied state summations in it ab initio self-energy calculations for large supercells
We present a new method for the computation of self-energy corrections in large supercells. It eliminates the explicit summation over unoccupied states, and uses an iterative scheme based on an expansion of the Green's function around a set of reference energies. This improves the scaling of the computational time from the fourth to the third power of the number of atoms for both the inverse dielectric matrix and the self-energy, yielding improved efficiency for 8 or more silicon atoms per unit cell
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