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Transiently amplified fluctuations assemble dissipative materials.

Tae Hyun Ueon1, Joseph P Patterson2,3, Jason R Green1,4

  • 1Department of Chemistry, University of Massachusetts Boston, Boston, MA 02125.

Proceedings of the National Academy of Sciences of the United States of America
|March 18, 2026
PubMed
Summary
This summary is machine-generated.

Chemically active supramolecular materials can transiently amplify fluctuations. This leads to a spontaneous increase in assembled material yield, offering new design possibilities for responsive materials.

Keywords:
dissipative self-assemblynonnormalitysupramolecular materialstransient growth

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Area of Science:

  • Supramolecular chemistry
  • Chemical kinetics
  • Materials science

Background:

  • Chemical reactions enable the creation of dynamic supramolecular materials with self-healing and responsive properties.
  • These behaviors stem from reaction cycles that interconvert molecular states through reagent-driven pathways.

Purpose of the Study:

  • To investigate the potential for transient amplification of fluctuations in supramolecular assembly using a specific network architecture.
  • To explore how chemical kinetics can drive the formation of thermodynamically unstable products.

Main Methods:

  • Analysis of a model supramolecular system with a two-pathway reaction cycle.
  • Mathematical modeling of chemical kinetics and steady-state conditions.
  • Investigation of conditions leading to transient growth and maximum amplification.

Main Results:

  • Demonstrated that the network architecture can transiently amplify small concentration fluctuations, significantly increasing assembled material yield.
  • Observed that kinetics initially evolve away from equilibrium after perturbation, promoting assembly of unstable products.
  • Found that systems farther from detailed balance exhibit stronger amplification and higher transient yields.

Conclusions:

  • The identified dynamics can lead to a pronounced, spontaneous increase in assembled material yield, exceeding steady-state levels.
  • Conditions for transient growth and maximum amplification were mathematically defined.
  • These findings suggest opportunities for designing responsive materials by controlling fluctuation amplification.