Change in relaxation scenario at the order-disorder transition of a colloidal fluid of hard spheres seen from the Gaussian limit of the self-intermediate scattering function

Self-intermediate scattering functions (ISFs) are measured by dynamic light scattering for the colloidal fluid of hard spheres for both equilibrium and nonequilibrium (undercooled) conditions, i.e., for volume fractions below and above the known freezing transition of the hard-sphere system. The delay time tau(m) where the mean-squared displacement, or the low wave-vector limit of the ISF, exhibits its maximum stretching is identified as a characteristic of the non-Markovian process(es) and is used to separate the ISF into fast (tau tau(m)) contributions. Each of these contributions exposes qualitative differences in the dynamics of the particles between the equilibrium and nonequilibrium colloidal fluids. These changes in the relaxation scenario signal the colloidal fluid's awareness of its traversal of the freezing volume fraction.