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Transition State Theory01:25

Transition State Theory

Transition-state theory, also known as activated-complex theory, provides a molecular-level explanation of reaction rates in both gas-phase and solution-phase reactions. It extends earlier kinetic models by considering the formation of a short-lived, high-energy configuration during a reaction.The progress of a chemical reaction can be represented using a reaction profile, which plots potential energy against the reaction coordinate. As two reactant molecules approach one another, their...
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Coil-to-globule transition by dissipative particle dynamics simulation.

Jiayi Guo1, Haojun Liang, Zhen-Gang Wang

  • 1CAS Key Laboratory of Soft Matter Chemistry and Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, Anhui, China.

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This study reveals a four-stage polymer collapse pathway in dilute solutions using dissipative particle dynamics. Polymers avoid "sausage" shapes, collapsing into a compact globule efficiently.

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Area of Science:

  • Polymer Physics
  • Soft Matter Physics
  • Computational Chemistry

Background:

  • Understanding polymer collapse dynamics is crucial for materials science and biophysics.
  • Previous studies suggested polymers could get trapped in metastable configurations during collapse.
  • Explicit solvent modeling is essential for capturing hydrodynamic and many-body interactions.

Purpose of the Study:

  • To investigate the polymer collapse dynamics under temperature quench in dilute solution.
  • To identify the distinct stages of polymer collapse.
  • To determine the scaling laws for collapse time with quench depth and chain length.

Main Methods:

  • Dissipative Particle Dynamics (DPD) simulations were employed.
  • Explicit solvent particles were incorporated to preserve hydrodynamic and many-body interactions.
  • Simulations were performed for various quench depths (ξ) and chain lengths (N).

Main Results:

  • A four-stage collapse pathway was identified: localized cluster formation, in situ cluster coarsening, global backbone rearrangement into a crumpled globule, and final globule compaction.
  • The polymer collapse avoided the previously reported metastable "sausage" configuration.
  • Time scales for the initial three stages were determined and their scaling with quench depth and chain length was established.

Conclusions:

  • The polymer collapse dynamics follow a predictable four-stage pathway without getting trapped in undesirable configurations.
  • The total collapse time exhibits specific scaling relationships with temperature quench depth and polymer chain length.
  • Dissipative Particle Dynamics is a suitable method for simulating complex polymer dynamics in solution.