Study of spatial correlations in a supercooled molecular system.
Spatial heterogeneities have been investigated in a supercooled system composed of diatomic molecules with an associated dipole moment by using the molecular dynamics simulation technique. Pair distribution functions of molecules with different mobilities have been evaluated, and it has been found that molecules belonging to the same dynamic domain are spatially correlated. Molecules with extremely large mobilities form larger clusters than those resulting from random statistics. These clusters are stringlike shaped. The mean cluster size displays a maximum at times between the ballistic and the diffusive regime, approximately at the end of the beta-relaxation zone. The value of this maximum increases upon cooling the system. An analogous profile has been observed for the characteristic cluster length when plotted against time. Agreement with Adam-Gibbs predictions has been encountered when considering these clusters as the basic dynamic units of the theory. For the extremely slow molecules, a cluster distribution has also been encountered. These clusters are smaller than the ones composed by fast molecules; they do not have a quasilinear geometry and no maximum is observed for their mean cluster size.
Palomar
Ricardo
R
Departament de Física i Enginyeria Nuclear, Universitat Politècnica de Catalunya, Campus Nord-Mòdul B4, c/Jordi Girona 1-3, 08034 Barcelona, Spain.
Sesé
Gemma
G