Dynamics of probes in model glassy matrices.
The dynamics of diatomic probe molecules in matrices composed of hard spheres are studied using molecular dynamics simulations. The matrix particles are connected to fixed attachment points by strings of length, l, which is varied from l-->infinity (fluid) to 0 ("glass"). The probe diffusion coefficient, D interpolates smoothly between these limits when l is changed. As l is decreased, D displays a transition from a power-law l dependence, which is well fit by the mode-coupling theory expression, to an Arrhenius l dependence. Single particle analysis shows that the hopping motion sets in for l much larger than a critical length, l(c), and Arrhenius behavior occurs when hopping becomes the dominant mode of transport. The system displays dynamic heterogeneity even though there is no growing dynamic correlation length of any kind.
Jagannathan
Kamakshi
K
Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706, USA.
Sung
Bong June
BJ
Yethiraj
Arun
A
D003198:Computer Simulation; D004058:Diffusion; D005898:Glass / Q000737:chemistry*; D008956:Models, Chemical; D013816:Thermodynamics