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Absolute Quantum Yield Measurement of Powder Samples
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Studying rare nonadiabatic dynamics with transition path sampling quantum jump trajectories.

Addison J Schile1, David T Limmer1

  • 1Department of Chemistry, University of California, Berkeley, California 94618, USA.

The Journal of Chemical Physics
|December 12, 2018
PubMed
Summary

We developed a new method using transition path sampling and quantum jump trajectories to study rare nonadiabatic dynamics in quantum systems. This approach provides mechanistic insights and accurate rates for ultrafast relaxation processes.

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Area of Science:

  • Quantum dynamics
  • Chemical physics
  • Statistical mechanics

Background:

  • Studying rare nonadiabatic dynamics in open quantum systems is challenging.
  • Existing methods often require prior knowledge of transition states.
  • Understanding ultrafast relaxation processes is crucial in chemistry and physics.

Purpose of the Study:

  • To present a novel computational method for studying rare nonadiabatic dynamics.
  • To provide mechanistic insight into ultrafast relaxation processes.
  • To enable unbiased computation of rates, branching ratios, and yields.

Main Methods:

  • Utilizing transition path sampling (TPS) and quantum jump trajectories.
  • Formulating a quantum path ensemble from an unravelled quantum master equation.
  • Conditioning trajectories on specific initial and final quantum states.

Main Results:

  • The method provides mechanistic insight into ultrafast relaxation processes.
  • Accurate rates for these processes can be computed.
  • Demonstrated utility in donor-bridge-acceptor energy transfer and electron transfer models.

Conclusions:

  • The developed method is effective for studying complex reactive quantum dynamics.
  • Path ensemble methods offer a powerful tool for quantum dynamics research.
  • This approach paves the way for future investigations of quantum phenomena.