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arXiv · 1101.3746

Computer Simulation Study of the Phase Behavior and Structural Relaxation in a Gel-Former Modeled by Three Body Interactions

Shibu Saw·Niels L. Ellegaard·Walter Kob·Srikanth Sastry
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Abstract

We report a computer simulation study of a model gel-former obtained by modifying the three-body interactions of the Stillinger-Weber potential for silicon. This modification reduces the average coordination number and consequently shifts the liquid-gas phase coexistence curve to low densities, thus facilitating the formation of gels without phase separation. At low temperatures and densities, the structure of the system is characterized by the presence of long linear chains interconnected by a small number of three coordinated junctions at random locations. At small wave-vectors the static structure factor shows a non-monotonic dependence on temperature, a behavior which is due to the competition between the percolation transition of the particles and the stiffening of the formed chains. We compare in detail the relaxation dynamics of the system as obtained from molecular dynamics with the one obtained from Monte Carlo dynamics. We find that the bond correlation function displays stretched exponential behavior at moderately low temperatures and densities, but exponential relaxation at low temperatures. The bond lifetime shows an Arrhenius behavior, independent of the microscopic dynamics. For the molecular dynamics at low temperatures, the mean squared displacement and the (coherent and incoherent) intermediate scattering function display at intermediate times a dynamics with ballistic character and we show that this leads to compressed exponential relaxation. For the Monte Carlo dynamics we find always an exponential or stretched exponential relaxation. Thus we conclude that the compressed exponential relaxation observed in experiments is due to the out-of-equilibrium dynamics.

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Shibu Saw, Niels L. Ellegaard, Walter Kob, Srikanth Sastry. 2011-01-19. Computer Simulation Study of the Phase Behavior and Structural Relaxation in a Gel-Former Modeled by Three Body Interactions. https://doi.org/10.1063/1.3578176

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