Evolution of spin coherence of radical pairs due to spin-selective recombination: Comparison of three models

Victor A Bagryansky; Artem O Chetverikov; Vsevolod I Borovkov; Yuri N Molin

doi:10.1063/5.0184479

Evolution of spin coherence of radical pairs due to spin-selective recombination: Comparison of three models

J Chem Phys. 2023 Dec 28;159(24):244112. doi: 10.1063/5.0184479.

Authors

Victor A Bagryansky¹, Artem O Chetverikov^{1

2}, Vsevolod I Borovkov^{1

2}, Yuri N Molin¹

Affiliations

¹ V.V. Voevodsky Institute of Chemical Kinetics and Combustion, 3 Institutskaya Str., Novosibirsk 630090, Russia.
² Novosibirsk State University, 2 Pirogova Str., Novosibirsk 630090, Russia.

PMID: 38149738
DOI: 10.1063/5.0184479

Abstract

This study looked for a way to evaluate the validity of previously suggested models for describing the spin-selective recombination of radical pairs. As an example, for analysis, we used the conventional model, the model by Jones and Hore [Chem. Phys. Lett. 488, 90 (2010)], and the model by Salikhov [Am. J. Phys. Chem. 11, 67 (2022)]. To do this, analytical solutions to the evolution of the radical pair density matrix due to a radical pair's spin-selective recombination and singlet-triplet transitions in a strong magnetic field were obtained for the conventional model and the Jones and Hore model. Spin interactions included in the Hamiltonian were time-independent exchange interactions as well as Zeeman and hyperfine interactions. The most striking difference between the models' predictions appeared when considering the fraction of singlet pairs among all currently existing ones. In the Jones and Hore model, this ratio has the form of damped oscillations for any values of the spin-hamiltonian parameters. The conventional model and the Salikhov model both predicted that this ratio had the form of undamped oscillations in the absence of exchange interaction and at a sufficiently low recombination rate. Besides, the conventional model predicts the possibility of a resonance-like behavior of this ratio when singlet-triplet transitions in a part of the radical pair ensemble are completely suppressed by tuning the magnetic field strength. Possible experimental conditions in which distinguishing between the models seems to be most straightforward were suggested.