Intermediate-range order governs dynamics in dense colloidal liquids

TL;DR

This study reveals that dense colloidal liquids possess complex intermediate-range structures with icosahedral and dodecahedral order, which are strongly linked to their dynamic heterogeneities and relaxation behaviors.

Contribution

It demonstrates, using advanced imaging and correlation functions, that intermediate-range order governs dynamics in dense colloidal liquids, challenging the traditional view of liquids as completely disordered.

Findings

Intermediate-range order extends beyond nearest neighbors.

Order correlates with dynamical heterogeneities.

Order grows with supercooling.

Abstract

The conventional wisdom is that liquids are completely disordered and lack non-trivial structure beyond nearest-neighbor distances. Recent observations have upended this view and demonstrated that the microstructure in liquids is surprisingly rich and plays a critical role in numerous physical, biological, and industrial processes. However, approaches to uncover this structure are either system-specific or yield results that are not physically intuitive. Here, through single-particle resolved three-dimensional confocal microscope imaging and the use of a recently introduced four-point correlation function, we show that bidisperse colloidal liquids have a highly non-trivial structure comprising alternating layers with icosahedral and dodecahedral order, which extends well-beyond nearest-neighbor distances and grows with supercooling. By quantifying the dynamics of the system on the particle level, we establish that it is this intermediate-range order, and not the short-range order, which has a one-to-one correlation with dynamical heterogeneities, a property directly related to the relaxation dynamics of glassy liquids. Our experimental findings provide a direct and much sought-after link between the structure and dynamics of liquids and pave the way for probing the consequences of this intermediate-range order in other liquid state processes.