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Intermediate-range order governs dynamics in dense colloidal liquids.

Navneet Singh1, Zhen Zhang2, A K Sood3,4

  • 1Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore 560064, India.

Proceedings of the National Academy of Sciences of the United States of America
|May 1, 2023
PubMed
Summary

Liquids possess surprising intermediate-range order, not just nearest-neighbor structure. This order correlates with dynamical heterogeneities, impacting liquid relaxation dynamics.

Keywords:
colloidsreal-space imagingstructure-dynamicssupercooled liquids and glassesthree-dimensional structure

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Area of Science:

  • Soft Matter Physics
  • Colloidal Science
  • Materials Science

Background:

  • Conventional view: liquids lack structure beyond nearest neighbors.
  • Emerging evidence: liquid microstructure is rich and functionally important.
  • Existing methods: often system-specific or lack physical intuition.

Purpose of the Study:

  • To uncover and characterize the intermediate-range order in bidisperse colloidal liquids.
  • To link this structure to the system's dynamics and relaxation properties.
  • To provide a physically intuitive framework for understanding liquid structure-dynamics relationships.

Main Methods:

  • Single-particle resolved three-dimensional confocal microscopy.
  • Application of a novel four-point correlation function.
  • Quantification of particle-level dynamics.

Main Results:

  • Bidisperse colloidal liquids exhibit nontrivial structure with alternating icosahedral and dodecahedral layers.
  • This order extends beyond nearest-neighbor distances and increases with supercooling.
  • Intermediate-range order, not short-range order, directly correlates with dynamical heterogeneities.

Conclusions:

  • Established a direct link between intermediate-range liquid structure and dynamics.
  • Demonstrated the critical role of order beyond nearest neighbors in liquid behavior.
  • Opened new avenues for investigating structure-property relationships in diverse liquid systems.