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Variational design principles for nonequilibrium colloidal assembly.

Avishek Das1, David T Limmer1

  • 1Department of Chemistry, University of California, Berkeley, California 94609, USA.

The Journal of Chemical Physics
|January 8, 2021
PubMed
Summary
This summary is machine-generated.

We developed a method to design forces for targeted self-assembly of molecular structures. This approach optimizes interactions to enhance the stability of desired configurations, even under external forces like shear flow.

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Area of Science:

  • Physics
  • Chemistry
  • Materials Science

Background:

  • Molecular dynamics simulations are crucial for understanding self-assembly processes.
  • Controlling self-assembly to achieve specific target structures remains a significant challenge.
  • Nonequilibrium steady-states offer unique opportunities for manipulating molecular systems.

Purpose of the Study:

  • To develop a theoretical framework for inverse design of self-assembly.
  • To determine optimal external forces for enhancing the stability of target structures.
  • To investigate the role of shear flow in colloidal cluster assembly.

Main Methods:

  • Application of large deviation theory and stochastic optimal control.
  • Formulation of a variational principle for self-assembly.
  • Development of an optimization algorithm for determining external forces.
  • Modeling colloidal cluster assembly in linear shear flow.

Main Results:

  • Rare molecular trajectories conditioned on target structures encode stabilizing interactions and forces.
  • Optimal forces were determined for targeted self-assembly in nonequilibrium steady-states.
  • Colloidal clusters were assembled with high yield using tunable short-range interactions.
  • Shear flow affects cluster yields: decreasing rigid clusters, increasing nonrigid ones.
  • Generalized linear response theory explains shear-induced yield changes.

Conclusions:

  • The developed inverse design approach enables precise control over self-assembly.
  • Understanding interactions and forces is key to achieving desired structures out of equilibrium.
  • Basic design principles for targeted assembly in nonequilibrium systems were uncovered.