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Register a new userOn the low magnetic field effect in radical pair reactions
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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 strong magnetic field increases the singlet yield. The high field effect arises from energy conservation: when the magnetic field is stronger than the sum of the hyperfine fields in the two radicals, ${rm S}to {rm T}_{pm}$ transitions become energetically forbidden, thereby reducing the number of pathways for singlet to triplet interconversion. The low field effect arises from symmetry breaking: the application of a weak magnetic field lifts degeneracies among the zero field eigenstates and increases the number of pathways for singlet to triplet interconversion. However, the details of this effect are more subtle, and have not previously been properly explained. Here we present a complete analysis of the low field effect in a radical pair containing a single proton, and in a radical pair in which one of the radicals contains a large number of hyperfine-coupled nuclear spins. We find that the new transitions that occur when the field is switched on are between ${rm S}$ and ${rm T}_0$ in both cases, and not between ${rm S}$ and ${rm T}_{pm}$ as has previously been claimed. We then illustrate this result by using it in conjunction with semiclassical spin dynamics simulations to account for the observation of a biphasic--triphasic--biphasic transition with increasing magnetic field strength in the magnetic field effect on the time-dependent survival probability of a photoexcited carotenoid-porphyrin-fullerene radical pair.
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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.
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 one of the four possible types of solution are analysed. It is demonstrated that in the absence of spin relaxation, besides the zero field invariant an invariant at large amplitudes of the resonant microwave field can be found. The two invariants open the possibility for simple calculation of microwave pulses to control quantum state of the radical pair. The effect of relaxation on the invariants is analysed and it is shown that changes in the high field invariant are induced by phase relaxation.
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 solution of the Liouville-von Neumann equation for a long-lived radical pair containing many hyperfine-coupled nuclear spins. Using a modified formulation of Floquet theory, treating the time-dependent magnetic field as a perturbation, and exploiting the slow radical pair recombination, we show that one can obtain a good approximation to the product yield by considering only nearly-degenerate sub-spaces of the Floquet space. Within a significant parameter range, the resulting method is found to give product yields in good agreement with exact quantum mechanical results for a variety of simple model radical pairs. Moreover it is considerably more efficient than the exact calculation, and it can be applied to radical pairs containing significantly more nuclear spins. This promises to open the door to realistic theoretical investigations of the effect of radiofrequency electromagnetic radiation on the photochemically induced radical pair recombination reactions in the avian retina which are believed to be responsible for the magnetic compass sense of migratory birds.
In this work we explore the effects of a weak magnetic field and a thermal bath on the decay process of a neutral scalar boson into two charged scalar bosons. Our findings indicate that magnetic field inhibits while temperature enhances the pair production. The employed formalism allows us to isolate the contribution of magnetic fields in vacuum, leading to a separate analysis of the effects of different ingredients. This is essential since the analytical computation of the decay width necessarily needs of some approximation and the results that can be found in the literature are not always coincident. We perform the calculation in vacuum by two different weak field approximations. The particle pair production in vacuum was found to coincide with finite temperature behavior, which is opposite to results obtained by other authors in scenarios that involve neutral particles decaying into a pair of charged fermions. Among other differences between these scenarios, we traced that the analytical structure of the self-energy imposed by the spin of particles involved in the process is determinant in the behavior of the decay rate with the magnetic field.
The ionization efficiency of helicon plasma discharge is explored by changing the low axial magnetic field gradients near the helicon antenna. The highest plasma density is found for a most possible diverging field near the antenna by keeping the other operating condition constant. Measurement of axial wave number together with estimated radial wavenumber suggests the oblique mode propagation of helicon wave along the resonance cone boundary. Propagation of helicon wave near the resonance cone angle boundary can excite electrostatic fluctuations which subsequently can deposit energy in the plasma. This process has been shown to be responsible for peaking in density in low field helicon discharges, where the helicon wave propagates at an angle with respect to the applied uniform magnetic field. The increased efficiency can be explained on the basis of multiple resonances for multimode excitation by the helicon antenna due to the availability of a broad range of magnetic field values in the near field of the antenna when a diverging magnetic field is applied in the source.
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