Abstract
We report a systematic molecular dynamics study of the isochoric equilibration of hard-sphere fluids in their metastable regime close to the glass transition. The thermalization process starts with the system prepared in a nonequilibrium state with the desired final volume fraction for which we can obtain a well-defined nonequilibrium static structure factor . The evolution of the -relaxation time and long-time self-diffusion coefficient as a function of the evolution time is then monitored for an array of volume fractions. For a given waiting time the plot of as a function of exhibits two regimes corresponding to samples that have fully equilibrated within this waiting time [] and to samples for which equilibration is not yet complete []. The crossover volume fraction increases with but seems to saturate to a value . We also find that the waiting time required to equilibrate a system grows faster than the corresponding equilibrium relaxation time, , and that both characteristic times increase strongly as approaches , thus suggesting that the measurement of equilibrium properties at and above is experimentally impossible.
- Received 2 November 2010
DOI:https://doi.org/10.1103/PhysRevE.83.060501
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