Collective Hard Core Interactions Leave Multiscale Signatures in Number Fluctuation Spectra

Abstract: A full understanding of transport in dense, interacting suspensions requires analysis frameworks sensitive to self and collective dynamics across all relevant spatial and temporal scales. Here we introduce a trajectory-free approach to address this problem based on the power spectral density of particle number fluctuations (N-PSD). By combining colloidal experiments and theory we show that the N-PSD naturally probes behaviour across multiple important dynamic regimes and we fully uncover the mechanistic origins of characteristic spectral scalings and timescales. In particular, we demonstrate that while high-frequency scalings link to self-diffusion, low-frequency scalings sensitively capture long-lived correlations and collective dynamics. In this regime, interactions lead to non-trivial spectral signatures, governed by pairwise particle exchange at small length scales and collective rearrangements over large scales. Our findings thus provide important insight into the effect of interactions on microscopic dynamics and fluctuation phenomena and establish a powerful new tool with which to probe dynamics in complex systems.