Suppression of the rate of growth of dynamic heterogeneities and its relation to the local structure in a supercooled polydisperse liquid

Details Suppression of the rate of growth of dynamic heterogeneities and its relation to the local structure in a supercooled polydisperse liquid Suppression of the rate of growth of dynamic heterogeneities and its relation to the local structure in a supercooled polydisperse liquid

2008-09-02

arxiv.org/abs/0809.0368v3

Physics

Condensed Matter

Soft Condensed Matter

Scientific paper

10.1103/PhysRevE.78.051501

The relationship between the microscopic arrangement of molecules in a supercooled liquid and its slow dynamics at low temperature near glass transition is studied by Molecular Dynamics (MD) simulations. A Lennard-Jones liquid with polydispersity in size and mass of constituent particles is chosen as the model system. Our studies reveal that the local structure (that varies with polydispersity) plays a crucial role both in the slowing down of dynamics and in the growth of the dynamic heterogeneities, besides determining the glass forming ability (GFA) of the system. Increasing polydispersity at fixed volume fraction is found to suppress the rate of growth of dynamic correlations, as detected by the growth in the peak of the non-linear density response function. The growth in dynamical correlation is manifested in a stronger than usual breakdown of Stokes-Einstein relation at lower polydispersity at low temperatures and also leads to a decrease in the fragility of the system with polydispersity. We show that the suppression of the rate of growth of the dynamic heterogeneity can be attributed to the loss of structural correlations (as measured by the structure factor and the local bond orientational order) with polydispersity. While a critical polydispersity is required to avoid crystallization, we find that further increase in polydispersity lowers the glass forming ability (GFA).

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