Persistent Local Structural Defectiveness as an Early Time Predictor of Intermittent Glassy Relaxation Events in Supercooled Water

J Phys Chem B. 2023 Apr 20;127(15):3516-3523. doi: 10.1021/acs.jpcb.2c08583. Epub 2023 Apr 6.

Abstract

To become a glass from the metastable supercooled state, a liquid experiences a dramatic dynamical slowing down within a narrow temperature window. However, the attainment of solid rigidity is not the result of breaking translational symmetry as in a crystal: the structure of the resulting amorphous solid strikingly resembles that of the liquid state. Moreover, the supercooled liquid is dynamically heterogeneous; that is, the dynamics varies by orders of magnitude from one region of the sample to another, but the establishment of the existence of strong structural differences between such regions has demanded hard efforts along the years. In this work, we focus precisely on such a structure-dynamics link for supercooled water showing that local regions with structural defectiveness are persistent during the structural relaxation of the system, hence acting as early time predictors of later intermittent glassy relaxation events.