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Radical pair intersystem crossing: Quantum dynamics or incoherent kinetics?

Thomas P Fay1, David E Manolopoulos1

  • 1Department of Chemistry, University of Oxford, Physical and Theoretical Chemistry Laboratory, South Parks Road, Oxford OX1 3QZ, United Kingdom.

The Journal of Chemical Physics
|April 22, 2019
PubMed
Summary
This summary is machine-generated.

This study explains how simple kinetic models accurately describe radical pair reactions, connecting them to quantum mechanics. It shows how finite lifetimes and dephasing cause incoherent intersystem crossing in spin dynamics.

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Area of Science:

  • Chemical Physics
  • Quantum Mechanics
  • Spin Chemistry

Background:

  • Magnetic field effects on radical pair reactions involve complex spin dynamics.
  • Rigorous treatment requires solving the Liouville-von Neumann equation.
  • Incoherent kinetic models often suffice for experimental data.

Purpose of the Study:

  • To provide the theoretical basis for incoherent kinetic models of radical pair reactions.
  • To elucidate the connection between these models and exact quantum mechanics.
  • To derive expressions for spin state interconversion rates.

Main Methods:

  • Theoretical analysis connecting incoherent models to quantum mechanics.
  • Derivation of expressions for radical pair spin state interconversion rates.
  • Testing kinetic master equations against quantum dynamical simulations.

Main Results:

  • Finite radical pair lifetime and spin-state dephasing lead to incoherent intersystem crossing.
  • Simple expressions for interconversion rates were derived.
  • Kinetic master equation validated against simulations for model systems and molecular wires.

Conclusions:

  • Incoherent kinetic models provide a valid and useful description of magnetic field effects in radical pair reactions.
  • The derived expressions offer approximations to existing functional forms.
  • The study bridges the gap between simplified models and fundamental quantum dynamics.