Dynamics and correlation length scales of a glass-forming liquid in quiescent and sheared conditions

We numerically study dynamics and correlation length scales of a colloidal liquid in both quiescent and sheared conditions to further understand the origin of slow dynamics and dynamic heterogeneity in glass-forming systems. The simulation is performed in a weakly frustrated two-dimensional liquid, where locally preferred order is allowed to develop with increasing density. The four-point density correlations and bond-orientation correlations, which have been frequently used to capture dynamic and static length scales ξ in a quiescent condition, can be readily extended to a system under steady shear in this case. In the absence of shear, we confirmed the previous findings that the dynamic slowing down accompanies the development of dynamic heterogeneity. The dynamic and static length scales increase with α-relaxation time τ(α) as a power law [Formula: see text], with μ?>?0. In the presence of shear, both viscosity and τ(α) have power-law dependences on shear rate in the marked shear-thinning regime. However, the dependence of correlation lengths cannot be described by power laws in the same regime. Furthermore, the relation [Formula: see text] between length scales and dynamics holds for not too strong shear where thermal fluctuations and external forces are both important in determining the properties of dense liquids. Thus, our results demonstrate a link between slow dynamics and structure in glass-forming liquids even under nonequilibrium conditions.     

Nonequilibrium Thermodynamics of Polymeric Liquids via Atomistic Simulation

The challenge of calculating nonequilibrium entropy in polymeric liquids undergoing flow was addressed from the perspective of extending equilibrium thermodynamics to include internal variables that quantify the internal microstructure of chain-like macromolecules and then applying these principles to nonequilibrium conditions under the presumption of an evolution of quasie equilibrium states in which the requisite internal variables relax on different time scales. The nonequilibrium entropy can be determined at various levels of coarse-graining of the polymer chains by statistical expressions involving nonequilibrium distribution functions that depend on the type of flow and the flow strength. Using nonequilibrium molecular dynamics simulations of a linear, monodisperse, entangled C₁₀₀₀H₂₀₀₂ polyethylene melt, nonequilibrium entropy was calculated directly from the nonequilibrium distribution functions, as well as from their second moments, and also using the radial distribution function at various levels of coarse-graining of the constituent macromolecular chains. Surprisingly, all these different methods of calculating the nonequilibrium entropy provide consistent values under both planar Couette and planar elongational flows. Combining the nonequilibrium entropy with the internal energy allows determination of the Helmholtz free energy, which is used as a generating function of flow dynamics in nonequilibrium thermodynamic theory.     

Shock waves in high-energy materials: the initial chemical events in nitramine RDX

We extend the reactive force field ReaxFF to describe the high energy nitramine RDX and use it with molecular dynamics (MD) to study its shock-induced chemistry. We studied shock propagation via nonequilibrium MD simulations at various collision velocities. We find that for high impact velocities (>6 km/s) the RDX molecules decompose and react to form a variety of small molecules in very short time scales (<3 ps). These products are consistent with those found experimentally at longer times. For lower velocities only NO2 is formed, also in agreement with experiments.     

Thermomolecular orientation of nonpolar fluids

We investigate the response of molecular fluids to temperature gradients. Using nonequilibrium molecular dynamics computer simulations we show that nonpolar diatomic fluids adopt a preferred orientation as a response to a temperature gradient. We find that the magnitude of this thermomolecular orientation effect is proportional to the strength of the temperature gradient and the degree of molecular anisotropy, as defined by the different size or mass of the molecular atomic sites. We show that the preferred orientation of the molecules follows the same trends observed in the Soret effect of binary mixtures. We argue this is a general effect that should be observed in a wide range of length scales.     

Discrete hydrodynamics: Numerical results for the soft-sphere viscosity

Numerical calculations have been done of the viscosity of the soft-sphere liquid, using a new molecular dynamics technique. It is based on a formulation of hydrodynamics which is discrete in space and time, and exactly renormalizable. The present data turn out to be sufficient to estimate the viscosity, but determination of the full equations of motion (and therefore renormalization) requires further calculations using a smaller discrete time interval; these are presently under way. The present results indicate that this method is more than 100 times more efficient than previous (Green-Kubo or nonequilibrium molecular dynamics) methods. This suggests that the discrete formulation is the most natural way to approach hydrodynamics.     

On the effective viscosity of nanosuspensions

The effective viscosity of nanosuspensions is simulated using the molecular dynamics method. It is found that viscosity is controlled not only by the volume concentration of nanoparticles, by also by their mass and diameter. The viscosity of even strongly rarefied nanosuspensions (with a low concentration of nanoparticles) cannot be described by the Einstein relation. This means that the mechanism responsible for the increase in the viscosity of the medium is not of hydrodynamic origin. It is shown that the formation of viscosity of nanosuspensions is associated to a considerable extent with nonequilibrium microfluctuations of density and velocity of the carrier medium, which are induced by the motion of nanoparticles.     

Lorentz gas shear viscosity via nonequilibrium molecular dynamics and Boltzmann's equation

When nonequilibrium molecular dynamics is used to impose isothermal shear on a two-body periodic system of hard disks or spheres, the equations of motion reduce to those describing a Lorentz gas under shear. In this shearing Lorentz gas a single particle moves, isothermally, through a spatially periodic shearing crystal of infinitely massive scatterers. The curvilinear trajectories are calculated analytically and used to measure the dilute Lorentz gas viscosity at several strain rates. Simulations and solutions of Boltzmann's equation exhibit shear thinning resembling that found inN-body nonequilibrium simulations. For the three-dimensional Lorentz gas we obtained an exact expression for the viscosity which is valid at all strain rates. In two dimensions this is not possible due to the anisotropy of the scattering.     

Shear viscosity and shear thinning in two-dimensional Yukawa liquids

A two-dimensional Yukawa liquid is studied using two different nonequilibrium molecular dynamics simulation methods. Shear viscosity values in the limit of small shear rates are reported for a wide range of Coulomb coupling parameter and screening lengths. At high shear rates it is demonstrated that this liquid exhibits shear thinning; i.e., the viscosity eta diminishes with increasing shear rate. It is expected that two-dimensional dusty plasmas will exhibit this effect.     

Nonequilibrium molecular dynamics simulation of shear viscosity by a uniform momentum source-and-sink scheme

A uniform momentum source-and-sink scheme of nonequilibrium molecular dynamics (NEMD) is developed to calculate the shear viscosity of fluids in this paper. The uniform momentum source and sink are realized by momentum exchanges of individual atoms in the left and right half systems, like the reverse nonequilibrium molecular dynamics (RNEMD) method [20] [Müller-Plathe, Phys. Rev. E, 49 (359), 1999]. This method has all features of RNEMD. In addition, the present momentum swap strategy maximizes the perturbation relaxation and eliminates the boundary jumps, which often harm other NEMD methods greatly. With periodic boundary conditions quadratic velocity profiles can be constructed and from the mean velocities of the right and left half systems the shear viscosity can be easily extracted. The scheme is tested on Lennard-Jones fluids over a wide range of state points (temperature and density), momentum exchange intervals and system sizes. It is demonstrated that the present approach can give reliable results with fast convergence by properly selecting the simulation parameters, i.e. particle number and exchange interval.     

SiO_2气凝胶导热机理的分子动力学模拟研究

本文采用分子动力学方法,选用Lennard-Jones势函数,对氩分子在SiO2气凝胶骨架结构间空隙中的运动进行了平衡分子动力学模拟(EMD)和非平衡分子动力学模拟(NEMD),分析其能量输运特性.结果表明:在骨架空隙尺寸为15nm条件下,气凝胶内部氩分子的扩散系数仅为同等条件下自由空间内氩分子扩散系数的50.35%,...     

A method for tractable dynamical studies of single and double shock compression

A new multiscale simulation method is formulated for the study of shocked materials. The method combines molecular dynamics and the Euler equations for compressible flow. Treatment of the difficult problem of the spontaneous formation of multiple shock waves due to material instabilities is enabled with this approach. The method allows the molecular dynamics simulation of the system under dynamical shock conditions for orders of magnitude longer time periods than is possible using the popular nonequilibrium molecular dynamics approach. An example calculation is given for a model potential for silicon in which a computational speedup of 10(5) is demonstrated. Results of these simulations are consistent with the recent experimental observation of an anomalously large elastic precursor on the nanosecond time scale.     

New developments in the Nonequilibrium Dynamics of spin glasses

We present an overview of recent developments in the nonequilibrium dynamics of spin glasses. The prevailing theoretical pictures are described and discussed in light of numerical results and experimental observations. We focus on aging phenomena like waiting-time-dependent length scales, scaling of two-time quantities, more complex temperature protocols during aging, and the violation of the fluctuation–dissipation theorem. Finally, aging in quantum spin glass models coupled to a dissipative bath is discussed.     

Length Dependence of Thermal Conductivity of Single-Walled Carbon Nanotubes

Dependence of the thermal conductivity on the length of two armchair single-walled carbon nanotubes （SWNTs） is studied by the nonequilibrium molecular dynamics （MD） method with Brenner Ⅱ potential. The thermal conductivities are calculated for （5, 5） and （7, 7） SWNTs with lengths ranging from 22 to 155nm. The results show that the thermal conductivity of SWNTs is sensitive to the length and it does not converge to a finite value when the tube length increases up to 155nm, however it obeys a power law relation.     

Nonequilibrium relaxation of an elastic string in a random potential

We study the nonequilibrium motion of an elastic string in a two dimensional pinning landscape using Langevin dynamics simulations. The relaxation of a line, initially flat, is characterized by a growing length L(t) separating the equilibrated short length scales from the flat long distance geometry that keeps a memory of the initial condition. We show that, in the long time limit, L(t) has a nonalgebraic growth with a universal distribution function. The distribution function of waiting times is also calculated, and related to the previous distribution. The barrier distribution is narrow enough to justify arguments based on scaling of the typical barrier.     

Rheology of ring polymer melts: from linear contaminants to ring-linear blends

Ring polymers remain a challenge to our understanding of polymer dynamics. Experiments are difficult to interpret because of the uncertainty in the purity and dispersity of the sample. Using both equilibrium and nonequilibrium molecular dynamics simulations we have investigated the structure, dynamics, and rheology of perfectly controlled ring-linear polymer blends of chains of up to about 14 entanglements per chain, comparable to experimental systems. Linear contaminants increase the zero-shear viscosity of a ring polymer melt by about 10% around one-fifth of their overlap concentration. For equal concentrations of linear and ring polymers, the blend viscosity is about twice that of the pure linear melt. The diffusion coefficient of the rings decreases dramatically, while the linear polymers are mostly unaffected. Our results are supported by a primitive path analysis.     

Nonequilibrium noise and instabilities in membranes with active pumps

We study the statistical properties and dynamics of flexible fluid membranes containing active transmembrane proteins and find that such active membranes can be either stable or unstable to small disturbances, depending on the signs of certain crucial parameters characterising the protein-membrane interaction. A major finding is that the shape-fluctuation spectrum in the stable case for a zero-tension active membrane has the same form over a large range of length scales as at equilibrium, but with a nonequilibrium “noise temperature” determined by the activity.     

Crystal bridge formation marks the transition to rigidity in a thin lubrication film

We report that the rheological transition in a thin lubrication film of dodecane from bulk to high viscosity states as the thickness is decreased is the result of a novel structural transition. Using nonequilibrium molecular dynamics simulations we find that the initial increase in viscosity as the film thins is due to the formation of isolated crystalline bridges between the surfaces. As the thickness decreases further, these bridges increase in number and organize themselves into a tetratic order in the plane of the surface. We show that this ordered state melts at a temperature of 350 K.     

Nonmonotonous relaxation processes in nonequilibrium nanoforming alloys of Al with transition and rare-earth metals

The temporal dependences of viscosity in Al₈₇Ni₈Y₅, Al₈₆Ni₈Ce₆, and Al₈₆Ni₈La₆ melts were measured at various temperatures after the solid-liquid phase transition. A nonmonotonous change in viscosity with the passage of time was found, due to the destruction of the nonequilibrium microheterogeneous state of melts inherited from the initial multiphase melts. We propose a mechanism of nonmonotonous relaxation of nonequilibrium microheterogeneous melts within the dynamical theory of a molecular field, assuming the emergence of a hierarchy of different relaxation times in the system. A theoretical temporal dependence of viscosity of melts is proposed that is qualitatively consistent with the experimental data.