Quantum Dynamics of Radical-Ion-Pair Reactions

TL;DR

This paper provides a comprehensive quantum mechanical analysis of radical-ion-pair reactions, clarifying misconceptions and extending understanding of their dynamics across different coherence regimes, with implications for spin chemistry.

Contribution

It generalizes previous work by applying quantum measurement theory to radical-ion-pair reactions, using an analogy with the double-slit experiment to cover all coherence scenarios.

Findings

Unified quantum treatment of radical-ion-pair reactions

Clarification of misconceptions in spin chemistry

Extension of theory to partial coherence regimes

Abstract

Radical-ion-pair reactions were recently shown to represent a rich biophysical laboratory for the application of quantum measurement theory methods and concepts, casting doubt on the validity of the theoretical treatment of these reactions and the results thereof that has been at the core of spin chemistry for several decades now. The ensued scientific debate, although exciting, is plagued with several misconceptions. We will here provide a comprehensive treatment of the quantum dynamics of radical-ion-pair reactions, generalizing our recent work and elaborating on the analogy with the double-slit experiment having partial "which-path" information. This analogy directly leads to the general treatment of radical-ion pair reactions covering the whole range between the two extremes, that of perfect singlet-triplet coherence and that of complete incoherence.