Role of hydrogen-bond coordination defects in the structural relaxation of supercooled water

Abstract

In this work, we shall study the role of threefold and fivefold coordination defects in the structure and dynamics of the hydrogen bond network of liquid water, with special emphasis on the glassy regime. A significant defect clusterization propensity will be made evident, with a prevalence of mixed pairs, that is, threefold- and fivefold-coordinated defects being first neighbors of each other. This structural analysis will enable us to determine the existence of defective and nondefective regions compatible with the high local density and low local density molecular states of liquid water, respectively. Hydrogen bond coordination defects will also be shown to promote water´s structural relaxation, with the undercoordinated ones playing a main role in driving glassy relaxation dynamics. Moreover, we shall show that the three-foldcoordinated molecules together with their first neighbors present at the initial configuration act as markers of the dynamical heterogeneities that would emerge at later times commensurate with the structural relaxation of the supercooled system.