Assessing the role of static length scales behind glassy dynamics in polydisperse hard disks

The glass transition is the freezing of a liquid into a solid state without evident structural order. Although glassy materials are well characterized experimentally, the existence of a phase transition into the glass state remains controversial. Here, we present numerical evidence for the existence of a novel first-order dynamical phase transition in atomistic models of structural glass formers. In contrast to equilibrium phase transitions, which occur in configuration space, this transition occurs in trajectory space, and it is controlled by variables that drive the system out of equilibrium. Coexistence is established between an ergodic phase with finite relaxation time and a nonergodic phase of immobile molecular configurations. Thus, we connect the glass transition to a true phase transition, offering the possibility of a unified picture of glassy phenomena.

Recently it has been revealed that when approaching the glass-transition temperature, T(g), the dynamics of a liquid not only drastically slows down, but also becomes progressively more heterogeneous. From our simulations and experiments of six different glass-forming liquids, we find that the heterogeneous dynamics is a result of critical-like fluctuations of static structural order, contrary to a common belief that it is purely of dynamic origin. The static correlation length and susceptibility of a structural order parameter show Ising-like power-law divergence towards the ideal glass-transition point. However, this structural ordering accompanies little density change, which explains why it has not been detected by the static structure factor so far. Our results suggest a far more direct link than thought before between glass transition and critical phenomena. Indeed, the glass transition may be a new type of critical phenomenon where a structural order parameter is directly linked to slowness.