Non-Gaussian rotational diffusion and swing motion of dumbbell probes in two-dimensional colloids

Abstract

Two-dimensional (2D) colloids exhibit intriguing phase behaviors distinct from those in three dimensions, as well as dynamic heterogeneity reminiscent of glass-forming liquids. Here, using discontinuous molecular dynamics simulations, we investigate the reporting dynamics of dicolloidal dumbbell probes in 2D colloids across the liquid–hexatic phase transition, where hexagonal bond-orientational order (HBOO) extends to a quasi-long-ranged one. The rotational dynamics of dumbbell probes faithfully captures the structural and dynamical features of the host: Brownian in the isotropic liquid and non-Gaussian in the hexatic and solid phases, reflecting both HBOO and dynamic heterogeneity of the medium. In the 2D hexatic and solid phases, probe rotation reflects heterogeneity as the dumbbells sample multiple dynamical domains of the host system: in mobile domains, they undergo rotational jumps of π/3 in accordance with HBOO, whereas in immobile domains, they librate within cages formed by surrounding disks. Such non-Gaussianity disappears upon re-entrant melting of the host medium driven by size polydispersity, highlighting a close connection between HBOO and probe dynamics. Furthermore, the probe dynamics exhibits translation–rotation decoupling through the breakdown of the Debye–Stokes–Einstein relation, regardless of how the rotational diffusion coefficient is defined. We identify swing motion as the dominant microscopic diffusion mechanism of the dumbbell probes, consistent with the observed decoupling.