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Dynamics and Time Scales of Higher-Order Correlations in Supercooled Colloidal Systems.


ABSTRACT: The dynamics and time scales of higher-order correlations are studied in supercooled colloidal systems. A combination of X-ray photon correlation spectroscopy (XPCS) and X-ray cross-correlation analysis (XCCA) shows the typical slowing of the dynamics of a hard sphere system when approaching the glass transition. The time scales of higher-order correlations are probed using a novel time correlation function gC, tracking the time evolution of cross-correlation function C. With an increasing volume fraction, the ratio of relaxation times of gC to the standard individual particle relaxation time obtained by XPCS increases from ∼0.4 to ∼0.9. While a value of ∼0.5 is expected for free diffusion, the increasing values suggest that the local orders within the sample are becoming more long-lived for larger volume fractions. Furthermore, the dynamics of local order is more heterogeneous than the individual particle dynamics. These results indicate that not only the presence but also the lifetime of locally favored structures increases close to the glass transition.

SUBMITTER: Striker NN 

PROVIDER: S-EPMC10226114 | biostudies-literature | 2023 May

REPOSITORIES: biostudies-literature

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Dynamics and Time Scales of Higher-Order Correlations in Supercooled Colloidal Systems.

Striker Nele N NN   Lokteva Irina I   Dartsch Michael M   Dallari Francesco F   Goy Claudia C   Westermeier Fabian F   Markmann Verena V   Hövelmann Svenja C SC   Grübel Gerhard G   Lehmkühler Felix F  

The journal of physical chemistry letters 20230512 20


The dynamics and time scales of higher-order correlations are studied in supercooled colloidal systems. A combination of X-ray photon correlation spectroscopy (XPCS) and X-ray cross-correlation analysis (XCCA) shows the typical slowing of the dynamics of a hard sphere system when approaching the glass transition. The time scales of higher-order correlations are probed using a novel time correlation function <i>g</i><sub><i>C</i></sub>, tracking the time evolution of cross-correlation function <i  ...[more]

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