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Complex Fluid Models of Mixed Quantum-Classical Dynamics.

François Gay-Balmaz1, Cesare Tronci2

  • 1Division of Mathematical Sciences, Nanyang Technological University, Singapore, Singapore.

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|July 5, 2024
PubMed
Summary

This study introduces a novel complex fluid system for nonadiabatic molecular dynamics, resolving computational challenges and mathematical inconsistencies in existing models. The new approach ensures a Hamiltonian structure and energy/momentum balance for more robust simulations.

Keywords:
Complex fluidsEuler-Poincaré reductionHamiltonian structureMixed quantum-classical dynamicsQuantum backreaction

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Area of Science:

  • Quantum dynamics
  • Computational chemistry
  • Theoretical physics

Background:

  • Nonadiabatic molecular dynamics often uses hydrodynamic descriptions for nuclei coupled to quantum electronics.
  • Existing models face computational challenges due to quantum potentials and mathematical inconsistencies, particularly in phase-space formulations.
  • Approximations neglecting quantum potentials lead to classical nuclear motion, creating complex fluid systems.

Purpose of the Study:

  • To present a new complex fluid system that overcomes the limitations of previous models in nonadiabatic molecular dynamics.
  • To develop a model that resolves computational challenges and mathematical inconsistencies.
  • To ensure the new system possesses a Hamiltonian structure and conserves energy and momentum.

Main Methods:

  • A novel complex fluid system is derived by applying fluid closure at the action principle level of a phase-space model.
  • The model's structural properties and dynamical invariants are analyzed.
  • The model is illustrated using pure-dephasing dynamics.

Main Results:

  • The new complex fluid system resolves computational and mathematical issues present in prior methods.
  • The system exhibits a Hamiltonian structure, ensuring energy and momentum conservation.
  • Analysis reveals key structural properties and dynamical invariants.

Conclusions:

  • The developed complex fluid system offers a more tractable and consistent approach for nonadiabatic molecular dynamics.
  • This method provides a robust framework for simulating quantum-classical systems, including solvation dynamics.
  • The study concludes by presenting invariant planar models derived from this new system.