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Controlling the Size, Shape and Stability of Supramolecular Polymers in Water
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Characterizing the Interplay between Polymer Solvation and Conformation.

Debdas Dhabal1, Zhitong Jiang1, Akash Pallath1

  • 1Department of Chemical and Biomolecular Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.

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Summary
This summary is machine-generated.

Understanding polymer collapse is key for flexible molecules. This study reveals that perturbing water molecules around a hydrophobic polymer can trigger collapse, with similar mechanisms observed in both water and octane solvents.

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Area of Science:

  • Physical Chemistry
  • Polymer Science
  • Computational Chemistry

Background:

  • Conformational transitions in flexible molecules, particularly those influenced by hydrophobic effects, are often impeded by desolvation barriers.
  • Characterizing the interplay between solvation and molecular conformation is crucial for understanding these transitions.

Purpose of the Study:

  • To characterize the solvation-conformation interplay for a hydrophobic polymer.
  • To investigate the mechanism of coil-to-globule transitions induced by external perturbations.
  • To compare collapse mechanisms in aqueous and nonpolar solvents.

Main Methods:

  • Utilized specialized molecular simulations to study a hydrophobic polymer in water.
  • Applied an external potential to perturb polymer hydration waters.
  • Investigated polymer collapse in octane, a nonpolar solvent, for comparative analysis.

Main Results:

  • An external potential can induce a coil-to-globule transition in the hydrophobic polymer.
  • The relative stability of collapsed versus extended states is quantifiable by the external potential strength.
  • Polymer collapse is bottlenecked by the formation and collective dewetting of large water clusters.

Conclusions:

  • The study provides mechanistic insights into polymer collapse, identifying cluster formation and dewetting as key factors.
  • The fundamental mechanisms driving hydrophobic polymer collapse are qualitatively similar in both water and nonpolar octane.
  • External perturbation of solvation shells offers a method to control and study conformational transitions.