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Mode-dependent phonon relaxation in time-resolved electron diffraction pattern simulations.

Wojciech Marciniak1, Joanna Marciniak2, José Ángel Castellanos-Reyes3

  • 1Department of Physics and Astronomy, Uppsala University, P.O. Box 516, 75120, Uppsala, Sweden; Institute of Physics, Poznań University of Technology, Piotrowo 3, 60-965, Poznań, Poland.

Ultramicroscopy
|January 24, 2026
PubMed
Summary

We developed a new simulation method to study ultrafast phonon dynamics in materials. This approach reveals how specific phonon modes relax, offering insights for time-resolved transmission electron microscopy (TEM) studies.

Keywords:
Frozen phonon multislice simulationsHigh-throughput atomistic simulationsMolecular dynamicsMulti-phonon scatteringPhonon relaxationTime-resolved electron diffraction

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Ultrafast Dynamics

Background:

  • Time-resolved pump-probe experiments are crucial for studying ultrafast processes.
  • Interpreting phonon dynamics in electron diffraction patterns at sub-picosecond scales requires advanced simulation tools, which are currently limited.

Purpose of the Study:

  • To introduce a novel simulation framework for analyzing ultrafast phonon dynamics.
  • To extend frozen phonon multislice simulations into the time domain for sub-picosecond analysis.
  • To investigate mode-dependent phonon relaxation in materials.

Main Methods:

  • Developed the frozen trajectory excitation (FTE) method to excite phonons beyond thermal equilibrium.
  • Implemented an ensemble sampling approach to extend frozen phonon multislice simulations to the time domain.
  • Applied the framework to face-centered cubic (fcc) Nickel (Ni) with a 10 fs relaxation time resolution.

Main Results:

  • Simulations revealed multi-phonon scattering processes.
  • Demonstrated strong mode dependence in phonon relaxation.
  • Identified measurable signatures of mode-dependent relaxation in diffraction patterns.

Conclusions:

  • Phonon-specific behavior is critical for understanding ultrafast dynamics.
  • The developed method provides predictive guidance for future time-resolved transmission electron microscopy (TEM) studies.
  • Mode-dependent relaxation significantly impacts diffraction patterns.