Structure and relaxations in liquid and amorphous Selenium

We report a molecular dynamics simulation of selenium, described by a three-body interaction. The temperatures T_g and T_c and the structural properties are in agreement with experiment. The mean nearest neighbor coordination number is 2.1. A small pre-peak at about 1 AA^-1 can be explained in terms of void correlations. In the intermediate self-scattering function, i.e. the density fluctuation correlation, classical behavior, alpha- and beta-regimes, is found. We also observe the plateau in the beta-regime below T_g. In a second step, we investigated the heterogeneous and/or homogeneous behavior of the relaxations. At both short and long times the relaxations are homogeneous (or weakly heterogeneous). In the intermediate time scale, lowering the temperature increases the heterogeneity. We connect these different domains to the vibrational (ballistic), beta- and alpha-regimes. We have also shown that the increase in heterogeneity can be understood in terms of relaxations

Properties of the energy landscape of network models for covalent glasses

We investigate the energy landscape of two dimensional network models for covalent glasses by means of the lid algorithm. For three different particle densities and for a range of network sizes, we exhaustively analyse many configuration space regions enclosing deep-lying energy minima. We extract the local densities of states and of minima, and the number of states and minima accessible below a certain energy barrier, the 'lid'. These quantities show on average a close to exponential growth as a function of their respective arguments. We calculate the configurational entropy for these pockets of states and find that the excess specific heat exhibits a peak at a critical temperature associated with the exponential growth in the local density of states, a feature of the specific heat also observed in real glasses at the glass transition.Comment: RevTeX, 19 pages, 7 figure

Simulation of thermal conductivity and heat transport in solids

Using molecular dynamics (MD) with classical interaction potentials we present calculations of thermal conductivity and heat transport in crystals and glasses. Inducing shock waves and heat pulses into the systems we study the spreading of energy and temperature over the configurations. Phonon decay is investigated by exciting single modes in the structures and monitoring the time evolution of the amplitude using MD in a microcanonical ensemble. As examples, crystalline and amorphous modifications of Selenium and $\rm{SiO_2}$ are considered.Comment: Revtex, 8 pages, 11 postscript figures, accepted for publication in PR

Observation of Single Transits in Supercooled Monatomic Liquids

A transit is the motion of a system from one many-particle potential energy valley to another. We report the observation of transits in molecular dynamics (MD) calculations of supercooled liquid argon and sodium. Each transit is a correlated simultaneous shift in the equilibrium positions of a small local group of particles, as revealed in the fluctuating graphs of the particle coordinates versus time. This is the first reported direct observation of transit motion in a monatomic liquid in thermal equilibrium. We found transits involving 2 to 11 particles, having mean shift in equilibrium position on the order of 0.4 R_1 in argon and 0.25 R_1 in sodium, where R_1 is the nearest neighbor distance. The time it takes for a transit to occur is approximately one mean vibrational period, confirming that transits are fast.Comment: 19 pages, 8 figure

Pressure dependence of diffusion in simple glasses and supercooled liquids

Using molecular dynamics simulation, we have calculated the pressure dependence of the diffusion constant in a binary Lennard-Jones Glass. We observe four temperature regimes. The apparent activation volume drops from high values in the hot liquid to a plateau value. Near the critical temperature of the mode coupling theory it rises steeply, but in the glassy state we find again small values, similar to the ones in the liquid. The peak of the activation volume at the critical temperature is in agreement with the prediction of mode coupling theory

Voronoi-Delaunay analysis of normal modes in a simple model glass

We combine a conventional harmonic analysis of vibrations in a one-atomic model glass of soft spheres with a Voronoi-Delaunay geometrical analysis of the structure. ``Structure potentials'' (tetragonality, sphericity or perfectness) are introduced to describe the shape of the local atomic configurations (Delaunay simplices) as function of the atomic coordinates. Apart from the highest and lowest frequencies the amplitude weighted ``structure potential'' varies only little with frequency. The movement of atoms in soft modes causes transitions between different ``perfect'' realizations of local structure. As for the potential energy a dynamic matrix can be defined for the ``structure potential''. Its expectation value with respect to the vibrational modes increases nearly linearly with frequency and shows a clear indication of the boson peak. The structure eigenvectors of this dynamical matrix are strongly correlated to the vibrational ones. Four subgroups of modes can be distinguished

Anharmonicity, vibrational instability and Boson peak in glasses

We show that a {\em vibrational instability} of the spectrum of weakly interacting quasi-local harmonic modes creates the maximum in the inelastic scattering intensity in glasses, the Boson peak. The instability, limited by anharmonicity, causes a complete reconstruction of the vibrational density of states (DOS) below some frequency $\omega_c$, proportional to the strength of interaction. The DOS of the new {\em harmonic modes} is independent of the actual value of the anharmonicity. It is a universal function of frequency depending on a single parameter -- the Boson peak frequency, $\omega_b$ which is a function of interaction strength. The excess of the DOS over the Debye value is $\propto\omega^4$ at low frequencies and linear in $\omega$ in the interval $\omega_b \ll \omega \ll \omega_c$. Our results are in an excellent agreement with recent experimental studies.Comment: LaTeX, 8 pages, 6 figure

Interaction of quasilocal harmonic modes and boson peak in glasses

The direct proportionality relation between the boson peak maximum in glasses, $\omega_b$, and the Ioffe-Regel crossover frequency for phonons, $\omega_d$, is established. For several investigated materials $\omega_b = (1.5\pm 0.1)\omega_d$. At the frequency $\omega_d$ the mean free path of the phonons $l$ becomes equal to their wavelength because of strong resonant scattering on quasilocal harmonic oscillators. Above this frequency phonons cease to exist. We prove that the established correlation between $\omega_b$ and $\omega_d$ holds in the general case and is a direct consequence of bilinear coupling of quasilocal oscillators with the strain field.Comment: RevTex, 4 pages, 1 figur

Diffusion and viscosity in a supercooled polydisperse system

We have carried out extensive molecular dynamics simulations of a supercooled polydisperse Lennard-Jones liquid with large variations in temperature at a fixed pressure. The particles in the system are considered to be polydisperse both in size and mass. The temperature dependence of the dynamical properties such as the viscosity ($\eta$) and the self-diffusion coefficients ($D_i$) of different size particles is studied. Both viscosity and diffusion coefficients show super-Arrhenius temperature dependence and fit well to the well-known Vogel-Fulcher-Tammann (VFT) equation. Within the temperature range investigated, the value of the Angell's fragility parameter (D $\approx 1.4$) classifies the present system into a strongly fragile liquid. The critical temperature for diffusion ($T_o^{D_i}$) increases with the size of the particles. The critical temperature for viscosity ($T_o^{\eta}$) is larger than that for the diffusion and a sizeable deviations appear for the smaller size particles implying a decoupling of translational diffusion from viscosity in deeply supercooled liquid. Indeed, the diffusion shows markedly non-Stokesian behavior at low temperatures where a highly nonlinear dependence on size is observed. An inspection of the trajectories of the particles shows that at low temperatures the motions of both the smallest and largest size particles are discontinuous (jump-type). However, the crossover from continuous Brownian to large length hopping motion takes place at shorter time scales for the smaller size particles.Comment: Revtex4, 7 pages, 8 figure