4.6 Article

Adiabatic limit collapse and local interaction effects in non-linear active microrheology molecular simulations of two-dimensional fluids

Journal

SOFT MATTER
Volume 19, Issue 28, Pages 5288-5299

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d3sm00358b

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Nonlinear active microrheology molecular dynamics simulations reveal that strong confining forces and an external pulling force generate a correlation between velocity and position dynamics of tracer particles. This correlation is characterized by an effective temperature and an effective mobility, which disrupt the equilibrium fluctuation-dissipation theorem. By measuring the temperature and mobility of the tracer particles and formulating a diffusion theory, the effective thermal and transport properties are decoupled from the velocity dynamics. The flexibility of attractive and repulsive forces allows for the analysis of temperature and mobility behaviors in relation to interactions and the surrounding fluid structure under different pulling forces.
Nonlinear active microrheology molecular dynamics simulations of high-density two-dimensional fluids show that the presence of strong confining forces and an external pulling force induces a correlation between the velocity and position dynamics of the tracer particle. This correlation manifests in the form of an effective temperature and an effective mobility of the tracer particle, which is responsible for the breaking of the equilibrium fluctuation-dissipation theorem. This fact is shown by measuring the tracer particle's temperature and mobility directly from the first two moments of the velocity distribution of a tracer particle and by formulating a diffusion theory in which effective thermal and transport properties are decoupled from the velocity dynamics. Furthermore, the flexibility of the attractive and repulsive forces in the tested interaction potentials allowed us to relate the temperature and mobility behaviors to the nature of the interactions and the structure of the surrounding fluid as a function of the pulling force. These results provide a refreshing physical interpretation of the phenomena observed in non-linear active microrheology.

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