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We describe how the semiclassical theory of radical pair recombination reactions recently introduced by two of us [D. E. Manolopoulos and P. J. Hore, J. Chem. Phys. 139, 124106 (2013)] can be generalised to allow for different singlet and triplet recombination rates. This is a non-trivial generalisation because when the recombination rates are different the recombination process is dynamically coupled to the coherent electron spin dynamics of the radical pair. Furthermore, because the recombination operator is a two-electron operator, it is no longer sufficient simply to consider the two electrons as classical vectors: one has to consider the complete set of 16 two-electron spin operators as independent classical variables. The resulting semiclassical theory is first validated by comparison with exact quantum mechanical results for a model radical pair containing 12 nuclear spins. It is then used to shed light on the spin dynamics of a carotenoid-porphyrin-fullerene (CPF) triad containing considerably more nuclear spins which has recently been used to establish a proof of principle for the operation of a chemical compass [K. Maeda et al., Nature 453, 387 (2008)]. We find in particular that the intriguing biphasic behaviour that has been observed in the effect of an Earth-strength magnetic field on the time-dependent survival probability of the photo-excited C+PF- radical pair arises from a delicate balance between its asymmetric recombination and the relaxation of the electron spin in the carotenoid radical.
Radical pair recombination reactions are known to be sensitive to the application of both low and high magnetic fields. The application of a weak magnetic field reduces the singlet yield of a singlet-born radical pair, whereas the application of a st
The paper reports an exact solution for the problem of spin evolution of radical ion pair in static magnetic and resonant microwave field taking into account Zeeman and hyperfine interactions and spin relaxation. The values of parameters that provide
We show that the stochastic Schrodinger equation (SSE) provides an ideal way to simulate the quantum mechanical spin dynamics of radical pairs. Electron spin relaxation effects arising from fluctuations in the spin Hamiltonian are straightforward to
We present a new method for calculating the product yield of a radical pair recombination reaction in the presence of a weak time-dependent magnetic field. This method successfully circumvents the computational difficulties presented by a direct solu
Radical pairs and the dynamics they undergo are prevalent in many chemical and biological systems. Specifically, it has been proposed that the radical pair mechanism results from a relatively strong hyperfine interaction with its intrinsic nuclear sp