Fluctuations of driven probes reveal nonequilibrium transitions in complex fluids

TL;DR

This paper introduces a method to detect nonequilibrium transitions in complex fluids by analyzing probe fluctuations, linking microstructural changes to stress relaxation dynamics through simulations, and providing an experimental approach to study nonlinear rheology.

Contribution

It presents a novel empirical method based on probe fluctuation variance to identify microstructural transitions in complex fluids, overcoming limitations of continuum models.

Findings

Variance scaling regimes indicate transitions from diffusive to jump dynamics.

Stored elastic stress may explain nonlinear friction and multi-step rheology.

Method applicable in experiments to detect nonequilibrium structural changes.

Abstract

Complex fluids subjected to localized microscopic energy inputs, typical of active microrheology setups, exhibit poorly understood nonequilibrium behaviors because of the intricate self-organization of their mesoscopic constituents. In this work we show how to identify changes in the microstructural conformation of the fluid by monitoring the variance of the probe position, based on a general method grounded in the breakdown of the equipartition theorem. To illustrate our method, we perform large-scale Brownian dynamics simulations of an effective model of micellar solution, and we link the different scaling regimes in the variance of the probe's position to the transitions from diffusive to jump dynamics, where the fluid intermittently relaxes the accumulated stress. This suggests stored elastic stress may be the physical mechanism behind the nonlinear friction curves recently measured in micellar solutions, pointing at a mechanism for the observed multi-step rheology. Our approach overcomes the limitations of continuum macroscopic descriptions and introduces an empirical method, applicable in experiments, to detect nonequilibrium transitions in the structure of complex fluids.