Comparison of dynamical heterogeneity in hard-sphere and attractive glass formers.
Using molecular dynamics simulations, we have determined that the nature of dynamical heterogeneity in jammed liquids is very sensitive to short-ranged attractions. Weakly attractive systems differ little from dense hard-sphere and Lennard-Jones fluids. Particle motion is punctuated and tends to proceed in steps of roughly a single particle diameter. Both of these basic features change in the presence of appreciable short-ranged attractions. Transient periods of particle mobility and immobility cannot be discerned at intermediate attraction strength, for which structural relaxation is greatly enhanced. Strong attractions, known to dramatically inhibit relaxation, restore bimodality of particle motion. But in this regime, transiently mobile particles move in steps that are significantly more biased toward large displacements than those in the case of weak attractions. This modified feature of dynamical heterogeneity, which cannot be captured by conventional mode coupling theory, verifies recent predictions from a model of spatially correlated facilitating defects.
Reichman
David R
DR
Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027, USA.
Rabani
Eran
E
Geissler
Phillip L
PL