Unveiling Structural Bottlenecks of Dynamic Disorder in a Density-Tunable Glass Former: From Strong to Fragile Regimes

Abstract

Fragility characterizes how rapidly a glass-forming liquid slows down upon supercooling, but whether strong and fragile behaviors arise from the same microscopic relaxation mechanism remains unclear. Here, we address this question using a density-tunable soft-repulsive binary mixture spanning distinct fragility regimes and analyze particle jump dynamics within the framework of dynamic disorder. Across these regimes, we show that increasing fragility leads to progressively broader cage-lifetime distributions and increasingly non-exponential survival probabilities, revealing non-Poisson cage-to-jump statistics governed by fluctuating jump rates and slowly evolving structural variables. To characterize their structural origin, we first identify the neighbor ranks most strongly coupled to jump motion using Kullback-Leibler divergence and Pearson correlation analyses. We then introduce a structural slowness parameter that combines these neighbor-distance fluctuations into a reduced slow coordinate for constructing the slow-fluctuation survival probability. A comparison with the actual survival probability shows that localized neighbor-distance fluctuations control the jump rate in the strong regime, whereas extended neighbor rearrangements become relevant in the intermediate and fragile regimes, increasing the effective dimensionality of the slow-variable space. In the fragile regime, distance-based descriptors alone become insufficient at the lowest temperature, where the Voronoi free volume captures additional cage-volume fluctuations in the rate-controlling slow variable. Point-to-set correlations grow with fragility, but the spatial extent of the slow variables exceeds the point-to-set length. These results show that fragility changes the structural bottleneck for microscopic rate fluctuations, linking dynamic disorder and multidimensional slow variables.