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Nonequilibrium design strategies for functional colloidal assemblies.

Avishek Das1, David T Limmer1,2,3,4

  • 1Department of Chemistry, University of California, Berkeley, CA 94720.

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|September 25, 2023
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Summary
This summary is machine-generated.

This study uses a nonequilibrium variational principle to optimize DNA-nanocluster materials. Far-from-equilibrium shear flow enhances material properties by amplifying colloidal state transitions and probability currents.

Keywords:
molecular machinesnonequilibriumself-assembly

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Area of Science:

  • Soft matter physics
  • Materials science
  • Nanotechnology

Background:

  • Self-assembled nanoclusters of DNA-coated colloids are crucial for functional materials.
  • Controlling their dynamic interconversion is challenging, especially under equilibrium conditions.

Purpose of the Study:

  • To develop design strategies for self-assembled nanocluster materials using nonequilibrium principles.
  • To investigate how shear flow influences colloidal state transitions and material properties far from equilibrium.

Main Methods:

  • Application of a nonequilibrium variational principle to optimize steady-state shear-induced interconversion.
  • Utilizing a stochastic optimization algorithm to identify design strategies.
  • Analyzing the effects of shear flow on isolated nanoclusters and microphases.

Main Results:

  • Far-from-equilibrium shear flow significantly enhances flux between colloidal states by decoupling stability and reactivity.
  • Nonequilibrium strategies amplify transition rates by coupling reaction coordinates to shear flow.
  • Shear flow selectively breaks detailed balance and maximizes probability currents by coupling orientational and conformational degrees of freedom.
  • Shear flow amplifies colloid flux in microphases without compromising structure.

Conclusions:

  • Nonequilibrium shear flow offers a powerful route to design and optimize functional nanocluster materials.
  • This approach provides general principles for creating nanoscale, autonomous materials driven far from equilibrium.