4,522 research outputs found
Wetting and contact-line effects for spherical and cylindrical droplets on graphene layers: A comparative molecular-dynamics investigation
In Molecular Dynamics (MD) simulations, interactions between water molecules
and graphitic surfaces are often modeled as a simple Lennard-Jones potential
between oxygen and carbon atoms. A possible method for tuning this parameter
consists of simulating a water nanodroplet on a flat graphitic surface,
measuring the equilibrium contact angle, extrapolating it to the limit of a
macroscopic droplet and finally matching this quantity to experimental results.
Considering recent evidence demonstrating that the contact angle of water on a
graphitic plane is much higher than what was previously reported, we estimate
the oxygen-carbon interaction for the recent SPC/Fwwater model. Results
indicate a value of about 0.2 kJ/mol, much lower than previous estimations. We
then perform simulations of cylindrical water filaments on graphitic surfaces,
in order to compare and correlate contact angles resulting from these two
different systems. Results suggest that modified Young's equation does not
describe the relation between contact angle and drop size in the case of
extremely small systems and that contributions different from the one deriving
from contact line tension should be taken into account.Comment: To be published on Physical Review E (http://pre.aps.org/
Polarization forces in water deduced from single molecule data
Intermolecular polarization interactions in water are determined using a
minimal atomic multipole model constructed with distributed polarizabilities.
Hydrogen bonding and other properties of water-water interactions are
reproduced to fine detail by only three multipoles , , and
and two polarizabilities and , which
characterize a single water molecule and are deduced from single molecule data.Comment: 4 revtex pages, 3 embedded color PS figure
Perspective: How good is DFT for water?
Kohn-Sham density functional theory (DFT) has become established as an
indispensable tool for investigating aqueous systems of all kinds, including
those important in chemistry, surface science, biology and the earth sciences.
Nevertheless, many widely used approximations for the exchange-correlation (XC)
functional describe the properties of pure water systems with an accuracy that
is not fully satisfactory. The explicit inclusion of dispersion interactions
generally improves the description, but there remain large disagreements
between the predictions of different dispersion-inclusive methods. We present
here a review of DFT work on water clusters, ice structures and liquid water,
with the aim of elucidating how the strengths and weaknesses of different XC
approximations manifest themselves across this variety of water systems. Our
review highlights the crucial role of dispersion in describing the delicate
balance between compact and extended structures of many different water
systems, including the liquid. By referring to a wide range of published work,
we argue that the correct description of exchange-overlap interactions is also
extremely important, so that the choice of semi-local or hybrid functional
employed in dispersion-inclusive methods is crucial. The origins and
consequences of beyond-2-body errors of approximate XC functionals are noted,
and we also discuss the substantial differences between different
representations of dispersion. We propose a simple numerical scoring system
that rates the performance of different XC functionals in describing water
systems, and we suggest possible future developments
Cooling rate, heating rate and aging effects in glassy water
We report a molecular dynamics simulation study of the properties of the
potential energy landscape sampled by a system of water molecules during the
process of generating a glass by cooling, and during the process of
regenerating the equilibrium liquid by heating the glass. We study the
dependence of these processes on the cooling/heating rates as well as on the
role of aging (the time elapsed in the glass state). We compare the properties
of the potential energy landscape sampled during these processes with the
corresponding properties sampled in the liquid equilibrium state to elucidate
under which conditions glass configurations can be associated with equilibrium
liquid configurations.Comment: to be published in Phys. Rev. E (rapid comunication
Formation energy and interaction of point defects in two-dimensional colloidal crystals
The manipulation of individual colloidal particles using optical tweezers has
allowed vacancies to be created in two-dimensional (2d) colloidal crystals,
with unprecedented possibility of real-time monitoring the dynamics of such
defects (Nature {\bf 413}, 147 (2001)). In this Letter, we employ molecular
dynamics (MD) simulations to calculate the formation energy of single defects
and the binding energy between pairs of defects in a 2d colloidal crystal. In
the light of our results, experimental observations of vacancies could be
explained and then compared to simulation results for the interstitial defects.
We see a remarkable similarity between our results for a 2d colloidal crystal
and the 2d Wigner crystal (Phys. Rev. Lett. {\bf 86}, 492 (2001)). The results
show that the formation energy to create a single interstitial is
lower than that of the vacancy. Because the pair binding energies of the
defects are strongly attractive for short distances, the ground state should
correspond to bound pairs with the interstitial bound pairs being the most
probable.Comment: 5 pages, 2 figure
Magnetic friction due to vortex fluctuation
We use Monte Carlo and molecular dynamics simulation to study a magnetic
tip-sample interaction. Our interest is to understand the mechanism of heat
dissipation when the forces involved in the system are magnetic in essence. We
consider a magnetic crystalline substrate composed of several layers
interacting magnetically with a tip. The set is put thermally in equilibrium at
temperature T by using a numerical Monte Carlo technique. By using that
configuration we study its dynamical evolution by integrating numerically the
equations of motion. Our results suggests that the heat dissipation in this
system is closed related to the appearing of vortices in the sample.Comment: 6 pages, 41 figure
Physics of the liquid-liquid critical point
Within the inherent structure (IS) thermodynamic formalism introduced by
Stillinger and Weber [F. H. Stillinger and T. A. Weber, Phys. Rev. A {\bf 25},
978 (1982)] we address the basic question of the physics of the liquid-liquid
transition and of density maxima observed in some complex liquids such as water
by identifying, for the first time, the statistical properties of the potential
energy landscape (PEL) responsible for these anomalies.
We also provide evidence of the connection between density anomalies and the
liquid-liquid critical point. Within the simple (and physically transparent)
model discussed, density anomalies do imply the existence of a liquid-liquid
transition.Comment: Physical Review Letters, in publicatio
High frequency longitudinal and transverse dynamics in water
High-resolution, inelastic x-ray scattering measurements of the dynamic
structure factor S(Q,\omega) of liquid water have been performed for wave
vectors Q between 4 and 30 nm^-1 in distinctly different thermodynamic
conditions (T= 263 - 420 K ; at, or close to, ambient pressure and at P = 2
kbar). In agreement with previous inelastic x-ray and neutron studies, the
presence of two inelastic contributions (one dispersing with Q and the other
almost non-dispersive) is confirmed. The study of their temperature- and
Q-dependence provides strong support for a dynamics of liquid water controlled
by the structural relaxation process. A viscoelastic analysis of the
Q-dispersing mode, associated with the longitudinal dynamics, reveals that the
sound velocity undergoes the complete transition from the adiabatic sound
velocity (c_0) (viscous limit) to the infinite frequency sound velocity
(c_\infinity) (elastic limit). On decreasing Q, as the transition regime is
approached from the elastic side, we observe a decrease of the intensity of the
second, weakly dispersing feature, which completely disappears when the viscous
regime is reached. These findings unambiguously identify the second excitation
to be a signature of the transverse dynamics with a longitudinal symmetry
component, which becomes visible in the S(Q,\omega) as soon as the purely
viscous regime is left.Comment: 28 pages, 12 figure
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