Heterogeneity and Memory Effect in the Sluggish Dynamics of Vacancy Defects in Colloidal Disordered Crystals and Their Implications to High-Entropy Alloys.

Vacancy dynamics of high-density 2D colloidal crystals with a polydispersity in particle size are studied experimentally. Heterogeneity in vacancy dynamics is observed. Inert vacancies that hardly hop to other lattice sites and active vacancies that hop frequently between different lattice sites are found within the same samples. The vacancies show high probabilities of first hopping from one lattice site to another neighboring lattice site, then staying at the new site for some time, and later hopping back to the original site in the next hop. This back-returning hop probability increases monotonically with the increase in packing fraction, up to 83%. This memory effect makes the active vacancies diffuse sluggishly or even get trapped in local regions. Strain-induced vacancy motion on a distorted lattice is also observed. New glassy properties in the disordered crystals are discovered, including the dynamical heterogeneity, the presence of cooperative rearranging regions, memory effect, etc. Similarities between the colloidal disordered crystals and the high-entropy alloys (HEAs) are also discussed. Molecular dynamics simulations further support the experimental observations. These results help to understand the microscopic origin of the sluggish dynamics in materials with ordered structures but in random energy landscapes, such as high-entropy alloys.

Direct Evidence of Void-Induced Structural Relaxations in Colloidal Glass Formers.

Particle dynamics in supercooled liquids are often dominated by stringlike motions in which lines of particles perform activated hops cooperatively. The structural features triggering these motions, crucial in understanding glassy dynamics, remain highly controversial. We experimentally study microscopic particle dynamics in colloidal glass formers at high packing fractions. With a small polydispersity leading to glass-crystal coexistence, a void in the form of a vacancy in the crystal can diffuse reversibly into the glass and further induces stringlike motions. In the glass, a void takes the form of a quasivoid consisting of a few neighboring free volumes and is transported by the stringlike motions it induces. In fully glassy systems with a large polydispersity, similar quasivoid actions are observed. The mobile particles cluster into stringlike or compact geometries, but the compact ones can be further broken down into connected sequences of strings, establishing their general importance.