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Dynamics of living polymers.

B O'Shaughnessy¹, D Vavylonis

¹Department of Chemical Engineering, Columbia University, 500 West 120th Street, New York, NY 10027, USA. bo8@columbia.edu

The European Physical Journal. E, Soft Matter

|March 10, 2004

Summary

Living polymerization dynamics exhibit ultrasensitivity to perturbations. Small changes trigger non-linear responses in molecular weight distribution, with distinct stages of chain growth, hole filling, and global relaxation.

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Area of Science:

Polymer Chemistry
Chemical Kinetics

Background:

Living polymerization allows monomer addition/subtraction at chain ends, maintaining equilibrium.
Equilibrium involves a balance where average growth rate negates fluctuations, resulting in an exponential molecular weight distribution (MWD).

Purpose of the Study:

To theoretically investigate the dynamics of living polymers after small perturbations.
To analyze the non-linear response and multi-stage relaxation of the MWD.

Main Methods:

Theoretical study of living polymer dynamics.
Analysis of molecular weight distribution (MWD) changes following perturbations.
Comparison with experimental viscosity measurements.

Main Results:

Perturbations disrupt equilibrium, causing boosted chain growth rates.
A three-stage response is observed: coherent growth/shrinkage, hole/peak filling, and global MWD relaxation.
Ultrasensitive, non-linear responses occur even for small perturbations, with distinct behaviors for epsilon > epsilonc and epsilon < epsilonc.

Conclusions:

Living polymerization dynamics display ultrasensitivity, leading to non-linear MWD evolution.
The theoretical predictions align with experimental observations in alpha-methylstyrene polymerization.
Understanding these dynamics is crucial for controlling polymer properties.

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