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Trajectory Ensemble Methods Provide Single-Molecule Statistics for Quantum Dynamical Systems.

Amro Dodin1, Justin Provazza2,3, David F Coker3

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New theoretical tools enable the simulation of single quantum systems, revealing heterogeneous quantum coherence dynamics and longer coherence times compared to ensemble averages. This advances understanding of quantum dynamics beyond averaged descriptions.

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Area of Science:

  • Quantum dynamics
  • Theoretical chemistry
  • Statistical mechanics

Background:

  • Probing single-molecule quantum dynamics requires advanced theoretical methods beyond ensemble averaging.
  • Understanding individual quantum system behavior is crucial for interpreting complex experimental data.

Purpose of the Study:

  • To develop and apply an efficient method for simulating individual quantum system dynamics.
  • To analyze the nonequilibrium dynamics of the spin-boson model at the single-system level.

Main Methods:

  • Developed an efficient method for sampling and simulating individual quantum system trajectories.
  • Applied classical statistical mechanics tools to analyze the ensemble of single-system trajectories.
  • Studied the nonequilibrium dynamics of the spin-boson model.

Main Results:

  • Quantum coherence dynamics are highly heterogeneous at the single-system level due to initial bath configurations.
  • Single quantum systems exhibit longer coherence retention times than ensemble averages.
  • Introduced a novel thermodynamic entanglement entropy to quantify system-bath entanglement driving forces.

Conclusions:

  • Single-system simulations provide crucial insights into quantum dynamics heterogeneity.
  • Variations in initial bath configurations significantly impact quantum coherence exchange.
  • The developed methods and metrics advance the theoretical understanding of quantum system-bath interactions.