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Structure and dynamics of responsive colloids with dynamical polydispersity.

Upayan Baul1, Joachim Dzubiella1,2

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Responsive colloids (RCs) exhibit dynamic property fluctuations, like size changes, which are often ignored in simulations. This study reveals that accounting for these dynamic changes in soft hydrogel colloids significantly alters their structure and diffusion dynamics.

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Area of Science:

  • Colloid and Interface Science
  • Soft Matter Physics
  • Computational Chemistry

Background:

  • Responsive colloids (RCs) possess intrinsic dynamical polydispersity in properties like size and shape.
  • This dynamic behavior is crucial but often unaddressed in coarse-grained mesoscale simulations.
  • Conventional simulations typically use frozen distributions or fixed sizes, neglecting dynamic interactions.

Purpose of the Study:

  • To investigate the impact of dynamically fluctuating particle sizes in responsive colloids (RCs) using Brownian dynamics simulations.
  • To analyze how these dynamic size changes affect liquid structure, emergent size distributions, diffusion, and relaxation kinetics.
  • To compare simulation results with conventional polydisperse and monodisperse systems.

Main Methods:

  • Brownian dynamics simulations of soft hydrogel colloids with explicitly resolved, dynamically fluctuating particle sizes.
  • Calculation of liquid structure, emergent size distributions, long-time diffusion, and property relaxation kinetics.
  • Comparison with reference cases: conventional polydisperse (frozen distribution) and monodisperse (fixed size) systems.

Main Results:

  • Dynamical polydispersity in RCs leads to significant differences in structure and dynamics compared to conventional models, especially at high densities.
  • Many-body correlations and the coupling between particle property and translation are key factors in RC systems.
  • Translational diffusion in RC systems closely resembles free diffusion due to a cancellation of crowding and size compression effects.
  • An effective monodisperse pair potential can approximate RC system behavior by incorporating emergent size distributions and a mean diffusion constant.

Conclusions:

  • Accounting for dynamical polydispersity in RCs is essential for accurately simulating their behavior.
  • The dynamic coupling between particle properties and translation significantly influences system-level observables.
  • Effective potentials can be developed to capture the complex behavior of RC systems in simulations.