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Michelle C Anderson1, Amro Dodin1,2, Thomas P Fay1

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We introduce a quantum committor to understand quantum reactions and control outcomes. This method generalizes transition states and quantifies coherence effects, achieving near 100% yields in models.

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Area of Science:

  • Quantum mechanics
  • Chemical reaction dynamics
  • Physical chemistry

Background:

  • Coherent effects are crucial in many quantum processes.
  • Classical transition state theory fails to capture quantum phenomena.
  • Understanding quantum reaction mechanisms is challenging.

Purpose of the Study:

  • To introduce a general definition of a quantum committor.
  • To generalize the concept of a transition state to quantum superpositions.
  • To quantify the impact of quantum interference on reaction progress.

Main Methods:

  • Developed a formalism applicable to linear quantum master equations with metastability.
  • Applied absorbing boundary conditions for reactant and product states.
  • Utilized the quantum committor to analyze polaritonic systems and conical intersections.

Main Results:

  • Determined the dependence of the quantum transition state on coherences.
  • Optimized initialization states in a conical intersection model.
  • Achieved reaction yields approaching 100% for desired outcomes.

Conclusions:

  • The quantum committor provides a practical tool for controlling quantum reactions.
  • It offers a conceptual framework for understanding reactions beyond classical intuition.
  • This formalism is essential for processes where coherent effects dominate.