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Area of Science:

  • Soft matter physics
  • Statistical mechanics
  • Colloid science

Background:

  • Macromolecular crowding influences biomolecular and polymer systems.
  • Many systems exhibit two-state transitions (e.g., proteins, DNA).
  • Responsive colloids (RCs) offer a tunable model for studying crowding effects.

Purpose of the Study:

  • Investigate self-crowding effects on soft, bistable RCs.
  • Analyze liquid bulk structure and thermodynamics near coil-to-globule transitions.
  • Explore the impact of energy barriers and particle softness.

Main Methods:

  • Mean-field density functional theory (DFT) for RCs.
  • Explicitly resolving macromolecule size as a degree of freedom.
  • Utilizing a bimodal 'Landau' energy landscape.

Main Results:

  • Substantial crowding effects on internal distributions and complex polydispersity.
  • Quasi-universal compression curves observed with increasing packing fractions.
  • Distinct compression signatures differentiating bimodal from unimodal behavior.
  • Microstructure reveals inhomogeneity due to tuneable local depletion effects.

Conclusions:

  • RC-DFT effectively models crowding effects in soft matter.
  • Bistable RCs show unique responses to self-crowding.
  • Particle softness and energy landscape critically influence liquid microstructure and thermodynamics.