English

Structural relaxation, dynamical arrest and aging in soft-sphere liquids

Soft Condensed Matter 2023-01-04 v1

Abstract

We investigate the structural relaxation of a soft-sphere liquid quenched isochorically (ϕ=0.7\phi=0.7) and instantaneously to different temperatures TfT_f above and below the glass transition. For this, we combine extensive Brownian dynamics simulations and theoretical calculations based on the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory. The response of the liquid to a quench generally consists of a sub-linear increase of the α\alpha-relaxation time with system's age. Approaching the ideal glass-transition temperature from above (Tf>TaT_f>T^a) sub-aging appears as a transient process describing a broad equilibration crossover for quenches to nearly arrested states. This allows us to empirically determine an equilibration timescale teq(Tf)t^{eq}(T_f) that becomes increasingly longer as TfT_f approaches TaT^a. For quenches inside the glass (TfTaT_f\leq T^a) the growth rate of the structural relaxation time becomes progressively larger as TfT_f decreases and, unlike the equilibration scenario, τα\tau_{\alpha} remains evolving within the whole observation time-window.These features are consistently found in theory and simulations with remarkable semi-quantitative agreement, and coincide with those revealed in the similar and complementary exercise [Phys. Rev. {\bf 96}, 022608 (2017)] that considered a sequence of quenches with fixed final temperature Tf=0T_f=0 but increasing ϕ\phi towards the hard-sphere dynamical arrest volume fraction ϕHSa=0.582\phi^a_{HS}=0.582. The NE-SCGLE analysis, however, unveils various fundamental aspects of the glass transition, involving the abrupt passage from the ordinary equilibration scenario to the persistent aging effects that are characteristic of glass-forming liquids. The theory also explains that, within the time window of any experimental observation, this can only be observed as a continuous crossover.

Keywords

Cite

@article{arxiv.2208.08436,
  title  = {Structural relaxation, dynamical arrest and aging in soft-sphere liquids},
  author = {Patricia Mendoza-Méndez and Ricardo Peredo-Ortiz and Edilio Lázaro Lázaro and M. Chávez-Paez and F. Pacheco-Vázquez and M. Medina-Noyola and L. F. Elizondo-Aguilera},
  journal= {arXiv preprint arXiv:2208.08436},
  year   = {2023}
}
R2 v1 2026-06-25T01:46:36.897Z