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Spatiotemporal mapping of mesoscopic liquid dynamics.

Zhiqiang Shen1, Jihong Ma1, Jan-Michael Y Carrillo1

  • 1Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.

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This study introduces spatiotemporal mapping of intermediate scattering functions for analyzing liquid dynamics. This new method offers a clearer global view of mesoscopic behaviors in liquids, improving upon traditional techniques.

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Area of Science:

  • Condensed Matter Physics
  • Soft Matter Physics
  • Computational Materials Science

Background:

  • Studying liquid dynamics at mesoscopic scales is challenging due to theoretical and experimental limitations.
  • Traditional methods analyze space-time correlation functions at discrete wave numbers, offering limited insight.
  • Advancements in computing power and neutron scattering techniques enable new approaches.

Purpose of the Study:

  • To demonstrate the benefits of spatiotemporally mapping intermediate scattering functions for understanding liquid dynamics.
  • To provide a more intuitive and fruitful approach to analyzing mesoscopic liquid behavior.
  • To investigate four diverse model systems using this novel mapping technique.

Main Methods:

  • Utilized molecular dynamics simulations to generate data for analysis.
  • Employed spatiotemporal mapping of intermediate scattering functions on a dense grid of correlation times and wave numbers.
  • Investigated four model systems: Lennard-Jones liquid, polymer melt, molten sodium chloride, and poly(ethylene oxide) melt.

Main Results:

  • Spatiotemporal mapping effectively elucidates mesoscopic dynamics, revealing molecular relaxations, hydrodynamic modes, and nonhydrodynamic excitations.
  • Direct visualization on 2D color maps allows global appraisal of complex mesoscopic dynamics, surpassing traditional methods.
  • Scaling relations between space and time for molecular motions are identified directly from the maps without model-dependent analysis.

Conclusions:

  • The spatiotemporal mapping method provides a powerful, intuitive approach to studying liquid dynamics at mesoscopic scales.
  • This visualization technique facilitates the understanding of collective mesoscopic dynamics and comparison with theoretical models.
  • The method offers a new perspective valuable for general liquid dynamics research.