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Coarse-grained single-particle dynamics in two-dimensional solids and liquids.

Jörg R Silbermann1, Martin Schoen, Sabine H L Klapp

  • 1Stranski-Laboratorium für Physikalische und Theoretische Chemie, Sekretariat C7, Technische Universität Berlin, Strasse des 17, Juni 115, Berlin, Germany. joerg.silbermann@fluids.tu-berlin.de

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
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Summary

This study validates the generalized Langevin equation (GLE) for describing single-particle dynamics in a 2D Lennard-Jones system. The GLE accurately models particle motion, even in high-temperature liquid phases where harmonic approximations fail.

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Area of Science:

  • Condensed Matter Physics
  • Statistical Mechanics
  • Computational Physics

Background:

  • The Mori-Zwanzig projection operator formalism enables describing single-particle dynamics via a generalized Langevin equation (GLE).
  • This GLE is exact for low-temperature solids under the harmonic approximation.
  • The validity of the GLE beyond the harmonic approximation is not well-established.

Purpose of the Study:

  • To investigate the accuracy of the generalized Langevin equation (GLE) for describing single-particle dynamics.
  • To evaluate the GLE's performance under thermodynamic conditions where harmonic approximations are invalid.
  • To compare GLE predictions with molecular dynamics simulations in a 2D Lennard-Jones system.

Main Methods:

  • Molecular dynamics (MD) simulations of a 2D system with Lennard-Jones interactions.
  • Computation of characteristic time autocorrelation functions for a tagged particle in MD simulations.
  • Solving the generalized Langevin equation (GLE) and comparing its results with MD data.

Main Results:

  • Excellent agreement between GLE predictions and MD simulations was observed at low temperatures.
  • Deviations between GLE and MD results emerge at higher temperatures.
  • These deviations remain surprisingly small even in the high-temperature liquid phase.

Conclusions:

  • The generalized Langevin equation (GLE) provides a robust description of single-particle dynamics in 2D Lennard-Jones systems.
  • The GLE retains significant accuracy beyond the harmonic approximation, extending its applicability to liquid phases.
  • This work validates the GLE as a powerful tool for studying complex particle dynamics in condensed matter systems.