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Dynamic Landau theory for supramolecular self-assembly.

Nitin S Tiwari1, Koen Merkus2, Paul van der Schoot2,3

  • 1Department of Applied Physics, Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands. n.tiwari@tue.nl.

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We developed a new dynamical Landau theory to model reversible polymerisation kinetics. This approach simplifies complex supramolecular self-assembly by reducing parameters and explaining phenomena like hysteresis.

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Soft Matter: Self-organisation and Supramolecular Assemblies

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Area of Science:

  • Supramolecular Chemistry
  • Polymer Science
  • Theoretical Chemistry

Background:

  • Reversible polymerisation kinetics are crucial for understanding supramolecular self-assembly.
  • Existing pathway-specific kinetic theories often require numerous system-specific parameters.

Purpose of the Study:

  • To develop a simplified dynamical Landau theory for activated linear supramolecular self-assembly kinetics.
  • To reduce the number of parameters needed to describe self-assembly phenomena.
  • To explain generic behaviors such as hysteresis, overshooting, undershooting, and lag times.

Main Methods:

  • Construction of a dynamical Landau theory.
  • Modeling activated linear supramolecular self-assembly.
  • Phenomenological approach based on phase transition analogy.

Main Results:

  • The theory drastically reduces the number of system-specific parameters.
  • Successfully describes hysteresis, overshooting, undershooting, and lag times in polymerisation kinetics.
  • Identifies conditions necessary for observing these phenomena.

Conclusions:

  • The dynamical Landau theory provides a powerful, simplified framework for studying self-assembly kinetics.
  • The phenomenological kinetic parameter acts as a 'pathway controller', influencing molecular pathway contributions.
  • This approach offers insights into the fundamental mechanisms of supramolecular polymerisation.