Polydispersity-driven dynamical differences between two- and three-dimensional supercooled liquids

Abstract: Previous studies have suggested a conundrum in the relaxation dynamics of polydisperse supercooled liquids. It has been shown that in two dimensions, the relative relaxation times of particles of different sizes become more similar as the material is cooled, whereas the opposite happens in three dimensions: they decouple. Here we resolve this conundrum. First, we show that the coupling observed in two dimensions is an artifact of cage correction introduced to account for Mermin-Wagner fluctuations. Instead, the relative relaxation time of small and large particles in two dimensions remains constant or slightly decouples with temperature, as opposed to the substantial decoupling observed in three dimensions. Investigating these dimensional differences further, we find through mobile cluster analysis that small particles initiate relaxation in both dimensions. As the clusters grow larger, they remain dominated by small particles in three dimensions whereas in two cluster growth becomes particle-size agnostic. We explain these findings with a minimal model by studying the distributions of single-particle barrier heights in the system, showing there is a clear difference in the environments of small and large particles, depending on the dimensionality. These findings highlight the critical role of dimensionality in glass formation, providing new insights into the mechanisms underlying the glass transition in polydisperse supercooled liquids.