Influence of the Environment Fluctuations on Incoherent Neutron Scattering Functions

In extending the conventional dynamic models, we consider a simple model to account for the environment fluctuations of particle atoms in a protein system and derive the elastic incoherent structure factor (EISF) and the incoherent scattering correlation function C(Q,t) for both the jump dynamics between sites with fluctuating site interspacing and for the diffusion inside a fluctuating sphere. We find that the EISF of the system (or the normalized elastic intensity) is equal to that in the absence of fluctuations averaged over the distribution of site interspacing or sphere radius a. The scattering correlation function is $C(Q,t)=\sum_{n} \psi(t)$, where the average is taken over the Q-dependent effective distribution of relaxation rates \lambda_n(a) and \psi(t) is the correlation function of the length a. When \psi(t)=1, the relaxation of C(Q,t) is exponential for the jump dynamics between sites (since \lambda_n(a) is independent of a) while it is nonexponential for diffusion inside a sphere.Comment: 7 pages, 7 eps figure

Crystal-like high frequency phonons in the amorphous phases of solid water

The high frequency dynamics of low- (LDA) and high-density amorphous-ice (HDA) and of cubic ice (I_c) has been measured by inelastic X-ray Scattering (IXS) in the 1-15 nm^{-1} momentum transfer (Q) range. Sharp phonon-like excitations are observed, and the longitudinal acoustic branch is identified up to Q = 8nm^{-1} in LDA and I_c and up to 5nm^{-1} in HDA. The narrow width of these excitations is in sharp contrast with the broad features observed in all amorphous systems studied so far. The "crystal-like" behavior of amorphous ices, therefore, implies a considerable reduction in the number of decay channels available to sound-like excitations which is assimilated to low local disorder.Comment: 4 pages, 3 figure

Formation, Manipulation, and Elasticity Measurement of a Nanometric Column of Water Molecules

Nanometer-sized columns of condensed water molecules are created by an atomic-resolution force microscope operated in ambient conditions. Unusual stepwise decrease of the force gradient associated with the thin water bridge in the tip-substrate gap is observed during its stretch, exhibiting regularity in step heights (~0.5 N/m) and plateau lengths (~1 nm). Such "quantized" elasticity is indicative of the atomic-scale stick-slip at the tip-water interface. A thermodynamic-instability-induced rupture of the water meniscus (5-nm long and 2.6-nm wide) is also found. This work opens a high-resolution study of the structure and the interface dynamics of a nanometric aqueous column.Comment: 4 pages, 3 figure

Sound modes broadening for Fibonacci one dimensional quasicrystals

We investigate vibrational excitation broadening in one dimensional Fibonacci model of quasicrystals (QCs). The chain is constructed from particles with two masses following the Fibonacci inflation rule. The eigenmode spectrum depends crucially on the mass ratio. We calculate the eigenstates and eigenfunctions. All calculations performed self-consistently within the regular expansion over the three wave coupling constant. The approach can be extended to three dimensional systems. We find that in the intermediate range of mode coupling constants, three-wave broadening for the both types of systems (1D Fibonacci and 3D QCs) depends universally on frequency. Our general qualitative conclusion is that for a system with a non-simple elementary cell phonon spectrum broadening is always larger than for a system with a primitive cell (provided all other characteristics are the same).Comment: 2o pages, 15 figure

Liquid-Liquid Phase Transition for an Attractive Isotropic Potential with Wide Repulsive Range

Recent experimental and theoretical results have shown the existence of a liquid-liquid phase transition in isotropic systems, such as biological solutions and colloids, whose interaction can be represented via an effective potential with a repulsive soft-core and an attractive part. We investigate how the phase diagram of a schematic general isotropic system, interacting via a soft-core squared attractive potential, changes by varying the parameters of the potential. It has been shown that this potential has a phase diagram with a liquid-liquid phase transition in addition to the standard gas-liquid phase transition and that, for a short-range soft-core, the phase diagram resulting from molecular dynamics simulations can be interpreted through a modified van der Waals equation. Here we consider the case of soft-core ranges comparable with or larger than the hard-core diameter. Because an analysis using molecular dynamics simulations of such systems or potentials is too time-demanding, we adopt an integral equation approach in the hypernetted-chain approximation. Thus we can estimate how the temperature and density of both critical points depend on the potential's parameters for large soft-core ranges. The present results confirm and extend our previous analysis, showing that this potential has two fluid-fluid critical points that are well separated in temperature and in density only if there is a balance between the attractive and repulsive part of the potential. We find that for large soft-core ranges our results satisfy a simple relation between the potential's parameters

Dynamically Slow Processes in Supercooled Water Confined Between Hydrophobic Plates

We study the dynamics of water confined between hydrophobic flat surfaces at low temperature. At different pressures, we observe different behaviors that we understand in terms of the hydrogen bonds dynamics. At high pressure, the formation of the open structure of the hydrogen bond network is inhibited and the surfaces can be rapidly dehydrated by decreasing the temperature. At lower pressure the rapid ordering of the hydrogen bonds generates heterogeneities that are responsible for strong non-exponential behavior of the correlation function, but with no strong increase of the correlation time. At very low pressures, the gradual formation of the hydrogen bond network is responsible for the large increase of the correlation time and, eventually, the dynamical arrest of the system and of the dehydration process.Comment: 14 pages, 3 figure

Liquid-Liquid Phase Transitions for Soft-Core Attractive Potentials

Using event driven molecular dynamics simulations, we study a three dimensional one-component system of spherical particles interacting via a discontinuous potential combining a repulsive square soft core and an attractive square well. In the case of a narrow attractive well, it has been shown that this potential has two metastable gas-liquid critical points. Here we systematically investigate how the changes of the parameters of this potential affect the phase diagram of the system. We find a broad range of potential parameters for which the system has both a gas-liquid critical point and a liquid-liquid critical point. For the liquid-gas critical point we find that the derivatives of the critical temperature and pressure, with respect to the parameters of the potential, have the same signs: they are positive for increasing width of the attractive well and negative for increasing width and repulsive energy of the soft core. This result resembles the behavior of the liquid-gas critical point for standard liquids. In contrast, for the liquid-liquid critical point the critical pressure decreases as the critical temperature increases. As a consequence, the liquid-liquid critical point exists at positive pressures only in a finite range of parameters. We present a modified van der Waals equation which qualitatively reproduces the behavior of both critical points within some range of parameters, and give us insight on the mechanisms ruling the dependence of the two critical points on the potential's parameters. The soft core potential studied here resembles model potentials used for colloids, proteins, and potentials that have been related to liquid metals, raising an interesting possibility that a liquid-liquid phase transition may be present in some systems where it has not yet been observed.Comment: 29 pages, 15 figure

Double dynamical regime of confined water

The Van Hove self correlation function of water confined in a silica pore is calculated from Molecular Dynamics trajectories upon supercooling. At long time in the $\alpha$ relaxation region we found that the behaviour of the real space time dependent correlators can be decomposed in a very slow, almost frozen, dynamics due to the bound water close to the substrate and a faster dynamics of the free water which resides far from the confining surface. For free water we confirm the evidences of an approach to a crossover mode coupling transition, previously found in Q space. In the short time region we found that the two dynamical regimes are overimposed and cannot be distinguished. This shows that the interplay between the slower and the faster dynamics emerges in going from early times to the $\alpha$ relaxation region, where a layer analysis of the dynamical properties can be performed.Comment: 6 pages with 9 figures. RevTeX. Accepted for pulbication in J. Phys. Cond. Mat

Ice XII in its second regime of metastability

We present neutron powder diffraction results which give unambiguous evidence for the formation of the recently identified new crystalline ice phase[Lobban et al.,Nature, 391, 268, (1998)], labeled ice XII, at completely different conditions. Ice XII is produced here by compressing hexagonal ice I_h at T = 77, 100, 140 and 160 K up to 1.8 GPa. It can be maintained at ambient pressure in the temperature range 1.5 < T < 135 K. High resolution diffraction is carried out at T = 1.5 K and ambient pressure on ice XII and accurate structural properties are obtained from Rietveld refinement. At T = 140 and 160 K additionally ice III/IX is formed. The increasing amount of ice III/IX with increasing temperature gives an upper limit of T ~ 150 K for the successful formation of ice XII with the presented procedure.Comment: 3 Pages of RevTeX, 3 tables, 3 figures (submitted to Physical Review Letters