45 research outputs found
Instantaneous Normal Mode analysis of liquid HF
We present an Instantaneous Normal Modes analysis of liquid HF aimed to
clarify the origin of peculiar dynamical properties which are supposed to stem
from the arrangement of molecules in linear hydrogen-bonded network. The
present study shows that this approach is an unique tool for the understanding
of the spectral features revealed in the analysis of both single molecule and
collective quantities. For the system under investigation we demonstrate the
relevance of hydrogen-bonding ``stretching'' and fast librational motion in the
interpretation of these features.Comment: REVTeX, 7 pages, 5 eps figures included. Minor changes in the text
and in a figure. Accepted for publication in Phys. Rev. Let
New black holes in the brane-world?
It is known that the Einstein field equations in five dimensions admit more
general spherically symmetric black holes on the brane than four-dimensional
general relativity. We propose two families of analytic solutions (with
g_tt\not=-1/g_rr), parameterized by the ADM mass and the PPN parameter beta,
which reduce to Schwarzschild for beta=1. Agreement with observations requires
|\beta-1| |\eta|<<1. The sign of eta plays a key role in the global causal
structure, separating metrics which behave like Schwarzschild (eta<0) from
those similar to Reissner-Nordstroem (eta>0). In the latter case, we find a
family of black hole space-times completely regular.Comment: 4 pages, RevTeX, 3 eps figures, final version to appear in Phys. Rev.
Continuum limit of amorphous elastic bodies: A finite-size study of low frequency harmonic vibrations
The approach of the elastic continuum limit in small amorphous bodies formed
by weakly polydisperse Lennard-Jones beads is investigated in a systematic
finite-size study. We show that classical continuum elasticity breaks down when
the wavelength of the sollicitation is smaller than a characteristic length of
approximately 30 molecular sizes. Due to this surprisingly large effect
ensembles containing up to N=40,000 particles have been required in two
dimensions to yield a convincing match with the classical continuum predictions
for the eigenfrequency spectrum of disk-shaped aggregates and periodic bulk
systems. The existence of an effective length scale \xi is confirmed by the
analysis of the (non-gaussian) noisy part of the low frequency vibrational
eigenmodes. Moreover, we relate it to the {\em non-affine} part of the
displacement fields under imposed elongation and shear. Similar correlations
(vortices) are indeed observed on distances up to \xi~30 particle sizes.Comment: 28 pages, 13 figures, 3 table
Irreversible reorganization in a supercooled liquid originates from localised soft modes
The transition of a fluid to a rigid glass upon cooling is a common route of
transformation from liquid to solid that embodies the most poorly understood
features of both phases1,2,3. From the liquid perspective, the puzzle is to
understand stress relaxation in the disordered state. From the perspective of
solids, the challenge is to extend our description of structure and its
mechanical consequences to materials without long range order. Using computer
simulations, we show that the localized low frequency normal modes of a
configuration in a supercooled liquid are causally correlated to the
irreversible structural reorganization of the particles within that
configuration. We also demonstrate that the spatial distribution of these soft
local modes can persist in spite of significant particle reorganization. The
consequence of these two results is that it is now feasible to construct a
theory of relaxation length scales in glass-forming liquids without recourse to
dynamics and to explicitly relate molecular properties to their collective
relaxation.Comment: Published online: 20 July 2008 | doi:10.1038/nphys1025 Available from
http://www.nature.com/nphys/journal/v4/n9/abs/nphys1025.htm
Relaxation processes in harmonic glasses?
A relaxation process, with the associated phenomenology of sound attenuation
and sound velocity dispersion, is found in a simulated harmonic Lennard-Jones
glass. We propose to identify this process with the so called microscopic (or
instantaneous) relaxation process observed in real glasses and supercooled
liquids. A model based on the memory function approach accounts for the
observation, and allows to relate to each others: 1) the characteristic time
and strength of this process, 2) the low frequency limit of the dynamic
structure factor of the glass, and 3) the high frequency sound attenuation
coefficient, with its observed quadratic dependence on the momentum transfer.Comment: 11 pages, 3 figure
Elastic constant dishomogeneity and dependence of the broadening of the dynamical structure factor in disordered systems
We propose an explanation for the quadratic dependence on the momentum ,
of the broadening of the acoustic excitation peak recently found in the study
of the dynamic structure factor of many real and simulated glasses. We ascribe
the observed law to the spatial fluctuations of the local wavelength of
the collective vibrational modes, in turn produced by the dishomegeneity of the
inter-particle elastic constants. This explanation is analitically shown to
hold for 1-dimensional disordered chains and satisfatorily numerically tested
in both 1 and 3 dimensions.Comment: 4 pages, RevTeX, 5 postscript figure
Vibrational spectrum of topologically disordered systems
The topological nature of the disorder of glasses and supercooled liquids
strongly affects their high-frequency dynamics. In order to understand its main
features, we analytically studied a simple topologically disordered model,
where the particles oscillate around randomly distributed centers, interacting
through a generic pair potential. We present results of a resummation of the
perturbative expansion in the inverse particle density for the dynamic
structure factor and density of states. This gives accurate results for the
range of densities found in real systems.Comment: Completely rewritten version, accepted in Physical Review Letter
The evolution of vibrational excitations in glassy systems
The equations of the mode-coupling theory (MCT) for ideal liquid-glass
transitions are used for a discussion of the evolution of the
density-fluctuation spectra of glass-forming systems for frequencies within the
dynamical window between the band of high-frequency motion and the band of
low-frequency-structural-relaxation processes. It is shown that the strong
interaction between density fluctuations with microscopic wave length and the
arrested glass structure causes an anomalous-oscillation peak, which exhibits
the properties of the so-called boson peak. It produces an elastic modulus
which governs the hybridization of density fluctuations of mesoscopic wave
length with the boson-peak oscillations. This leads to the existence of
high-frequency sound with properties as found by X-ray-scattering spectroscopy
of glasses and glassy liquids. The results of the theory are demonstrated for a
model of the hard-sphere system. It is also derived that certain schematic MCT
models, whose spectra for the stiff-glass states can be expressed by elementary
formulas, provide reasonable approximations for the solutions of the general
MCT equations.Comment: 50 pages, 17 postscript files including 18 figures, to be published
in Phys. Rev.
Water Dynamics at Protein Interfaces: Ultrafast Optical Kerr Effect Study
The behavior of water molecules surrounding a protein can have an important bearing on its structure and function. Consequently, a great deal of attention has been focused on changes in the relaxation dynamics of water when it is located at the protein surface. Here we use the ultrafast optical Kerr effect to study the H-bond structure and dynamics of aqueous solutions of proteins. Measurements are made for three proteins as a function of concentration. We find that the water dynamics in the first solvation layer of the proteins are slowed by up to a factor of 8 in comparison to those in bulk water. The most marked slowdown was observed for the most hydrophilic protein studied, bovine serum albumin, whereas the most hydrophobic protein, trypsin, had a slightly smaller effect. The terahertz Raman spectra of these protein solutions resemble those of pure water up to 5 wt % of protein, above which a new feature appears at 80 cm–1, which is assigned to a bending of the protein amide chain