Fluctuations of driven probes reveal nonequilibrium transitions in complex fluids

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 that 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.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2025-08-04
DOI
https://doi.org/10.1063/5.0284891
Primary Topic
Micro and Nano Robotics
Type
article
Field-Weighted Citation Impact
0.00

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article

Fluctuations of driven probes reveal nonequilibrium transitions in complex fluids

Gianmaria Falasco, Marco Baiesi, Danilo Forastiere, Emanuele Locatelli et al.
The Journal of Chemical Physics
Micro and Nano Robotics
article

Fluctuations of driven probes reveal nonequilibrium transitions in complex fluids

Gianmaria Falasco, Marco Baiesi, Danilo Forastiere, Emanuele Locatelli, Enzo Orlandini
article en

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 that 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.

The Journal of Chemical PhysicsVol. 163(5)
University of Padua (IT), Istituto Nazionale di Fisica Nucleare, Sezione di Padova (IT), Osservatorio Astronomico di Padova (IT)
Ministero dell’Istruzione, dell’Università e della Ricerca, Università degli Studi di Padova
Affordable and clean energy
Openalex Percentile: Top 88%
Micro and Nano Robotics
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