Metabasin dynamics and local structure in supercooled water.
We employ the distance matrix method to investigate metabasin dynamics in supercooled water. We find that the motion of the system consists in the exploration of a finite region of configuration space (enclosing several distinct local minima), named metabasin, followed by a sharp crossing to a different metabasin. The characteristic time between metabasin transitions is comparable to the structural relaxation time, suggesting that these transitions are relevant for the long-time dynamics. The crossing between metabasins is accompanied by very rapid diffusional jumps of several groups of dynamically correlated particles. These particles form relatively compact clusters and act as cooperative relaxing units responsible for the density relaxation. We find that these mobile particles are often characterized by an average coordination larger than four, i.e., they are located in regions where the tetrahedral hydrogen bond network is distorted.
Rodríguez Fris
Jorge Ariel
JA
Fisicoquímica, Departamento de Química, Universidad Nacional del Sur, Avenida Alem 1253, 8000 Bahía Blanca, Argentina.
Appignanesi
Gustavo A
GA
La Nave
Emilia
E
Sciortino
Francesco
F