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Molecular Hydrodynamics from Memory Kernels.

Dominika Lesnicki1, Rodolphe Vuilleumier1, Antoine Carof2

  • 1École Normale Supérieure, PSL Research University, Département de Chimie, Sorbonne Universités-UPMC Université Paris 06, CNRS UMR 8640 PASTEUR, 24 rue Lhomond, 75005 Paris, France.

Physical Review Letters
|April 23, 2016
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Summary
This summary is machine-generated.

The memory kernel for a tagged particle in a fluid exhibits a long-time tail, leading to the emergence of the hydrodynamic Basset-Boussinesq force. This study reveals a negative added mass for molecular solutes, challenging conventional hydrodynamics.

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Area of Science:

  • Fluid dynamics
  • Statistical mechanics
  • Computational physics

Background:

  • Understanding particle dynamics in fluids is crucial for various scientific fields.
  • Molecular dynamics simulations provide insights into microscopic fluid behavior.
  • The Basset-Boussinesq force describes added mass and drag on accelerating bodies in viscous fluids.

Purpose of the Study:

  • To investigate the long-time behavior of the memory kernel for a tagged particle in a fluid.
  • To demonstrate the emergence of the hydrodynamic Basset-Boussinesq force from molecular dynamics data.
  • To generalize the concept of hydrodynamic added mass and explore its implications for molecular solutes.

Main Methods:

  • Analysis of memory kernel decay from molecular dynamics simulations.
  • Derivation and generalization of the Basset-Boussinesq force.
  • Investigation of hydrodynamic added mass for molecular solutes.

Main Results:

  • The memory kernel decays algebraically as t^{-3/2}.
  • The hydrodynamic Basset-Boussinesq force naturally emerges from this long-time tail.
  • A negative hydrodynamic added mass was observed for molecular solutes, contradicting incompressible hydrodynamics.
  • Contributions to friction and associated time scales were analyzed.

Conclusions:

  • The study provides a molecular dynamics basis for the Basset-Boussinesq force.
  • The findings highlight deviations from classical hydrodynamics for molecular systems.
  • Understanding the crossover between molecular and hydrodynamic regimes is essential for predicting solute behavior.