It is difficult to relate the properties of liquids and glasses directly to their structure because of complexity in the structure which defies precise definition. The potential energy landscape (PEL) approach is a very insightful way to conceptualiz
e the structure-property relationship in liquids and glasses, particularly on the effect of temperature and history. However, because of the highly multi-dimensional nature of the PEL it is hard to determine, or even visualize, the actual details of the energy landscape. In this article we introduce a modified concept of the local energy landscape (LEL) which is limited in phase space, and demonstrate its usefulness using molecular dynamics simulation on a simple liquid at high temperatures. The local energy landscape is given as a function of the local coordination number, the number of the nearest neighbor atoms. The excitations in the LEL corresponds to the so-called beta-relaxation process. The LEL offers a simple but useful starting point to discuss complex phenomena in liquids and glasses.
The elementary excitations of vibration in solids are phonons. But in liquids phonons are extremely short-lived and marginalized. In this letter through classical and ab-initio molecular dynamics simulations of the liquid state of various metallic sy
stems we show that different excitations, the local configurational excitations in the atomic connectivity network, are the elementary excitations in high temperature metallic liquids. We also demonstrate that the competition between the configurational excitations and phonons determines the so-called crossover phenomenon in liquids. These discoveries open the way to the explanation of various complex phenomena in liquids, such as fragility and the rapid increase in viscosity toward the glass transition, in terms of these excitations.
Atomic correlations in a simple liquid in steady-state flow under shear stress were studied by molecular dynamics simulation. The local atomic level strain was determined through the anisotropic pair-density function (PDF). The atomic level strain ha
s a limited spatial extension whose range is dependent on the strain rate and extrapolates to zero at the critical strain rate. A failure event is identified with altering the local topology of atomic connectivity by exchanging bonds among neighboring atoms.
We report an extension of the smoothed profile method (SPM)[Y. Nakayama, K. Kim, and R. Yamamoto, Eur. Phys. J. E {bf 26}, 361(2008)], a direct numerical simulation method for calculating the complex modulus of the dispersion of particles, in which w
e introduce a temporally oscillatory external force into the system. The validity of the method was examined by evaluating the storage $G(omega)$ and loss $G(omega)$ moduli of a system composed of identical spherical particles dispersed in an incompressible Newtonian host fluid at volume fractions of $Phi=0$, 0.41, and 0.51. The moduli were evaluated at several frequencies of shear flow; the shear flow used here has a zigzag profile, as is consistent with the usual periodic boundary conditions.
The non-Newtonian behavior of a monodisperse concentrated dispersion of spherical particles was investigated using a direct numerical simulation method, that takes into account hydrodynamic interactions and thermal fluctuations accurately. Simulation
s were performed under steady shear flow with periodic boundary conditions in the three directions. The apparent shear viscosity of the dispersions was calculated at volume fractions ranging from 0.31 to 0.56. Shear-thinning behavior was clearly observed at high volume fractions. The low- and high-limiting viscosities were then estimated from the apparent viscosity by fitting these data into a semi-empirical formula. Furthermore, the short-time motions were examined for Brownian particles fluctuating in concentrated dispersions, for which the fluid inertia plays an important role. The mean square displacement was monitored in the vorticity direction at several different Peclet numbers and volume fractions so that the particle diffusion coefficient is determined from the long-time behavior of the mean square displacement. Finally, the relationship between the non-Newtonian viscosity of the dispersions and the structural relaxation of the dispersed Brownian particles is examined.
The short-time motion of Brownian particles in an incompressible Newtonian fluid under shear, in which the fluid inertia becomes important, was investigated by direct numerical simulation of particulate flows. Three-dimensional simulations were perfo
rmed, wherein external forces were introduced to approximately form Couette flows throughout the entire system with periodic boundary conditions. In order to examine the validity of the method, the mean square displacement of a single spherical particle in a simple shear flow was calculated, and these results were compared with a hydrodynamic analytical solution that includes the effects of the fluid inertia. Finally, the dynamical behavior of a monodisperse dispersion composed of repulsive spherical particles was examined on short time scales, and the shear-induced diffusion coefficients were measured for several volume fractions up to 0.50.
Motions of fluctuating Brownian particles in an incompressible viscous fluid have been studied by coupled simulations of Brownian particles and host fluid. We calculated the velocity autocorrelation functions of Brownian particles and compared them w
ith the theoretical results. Extensive discussions have been made on the time scales for which our numerical model is valid.
We present a numerical method that consistently implements thermal fluctuations and hydrodynamic interactions to the motion of Brownian particles dispersed in incompressible host fluids. In this method, the thermal fluctuations are introduced as rand
om forces acting on the Brownian particles. The hydrodynamic interactions are introduced by directly resolving the fluid motions with the particle motion as a boundary condition to be satisfied. The validity of the method has been examined carefully by comparing the present numerical results with the fluctuation-dissipation theorem whose analytical form is known for dispersions of a single spherical particle. Simulations are then performed for more complicated systems, such as a dispersion composed of many spherical particles and a single polymeric chain in a solvent.
