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Spin dynamics in triplet radical pairs are theoretically studied under the spin-locking condition, where singlet–triplet mixing is blocked by the resonant microwave field. A key assumption in the theory is simultaneous excitations of T+–T0 and T−–T0 transitions in triplet radical pairs. This assumption allows for the application of a three-state model [Yago, J. Chem. Phys. 151, 214501 (2019)] to describe the spin dynamics of triplet radical pairs. The analysis based on the three-state model shows that the triplet states are quantized along the direction of a microwave-induced magnetic field (B1) in the rotating frame under the spin-locking condition. This gives rise to a new spin-locking phenomenon where T+–T0 and T−–T0 mixing are most enhanced at magnetic fields that deviate from the resonance by ±B1. It is also shown that the quantum beats observed under the spin-locking condition originate from the spin dynamics in triplet radical pairs. [ABSTRACT FROM AUTHOR]

Using the density operator formalism, a simple analytical model is developed to study low magnetic field effects on triplet pair annihilations in organic solids. Analysis is restricted to canonical orientations where two identical triplet molecules have the same orientation and the direction of the external magnetic field is parallel to one of the principle axes of the dipolar coupling tensor for a triplet. The analytical solution reveals that the low magnetic field effect in the triplet pair arises from the anisotropic dipole-dipole coupling in a triplet. In the presence of the dipole-dipole coupling, the spin quantization axis for each triplet gradually changes with the increase of the external magnetic field from zero field to high field. The low magnetic field effect reaches a maximum when the Zeeman splitting between the spin states matches a dipole-dipole coupling component orthogonal to the external magnetic field direction. The result is also discussed with the low magnetic field effect in the radical pair with one isotropic hyperfine coupling. [ABSTRACT FROM AUTHOR]

Pulsed electron nuclear double resonance (ENDOR) using a modified Davies-type [Phys. Lett. 47A, 1 (1974)] sequence is employed to study the hyperfine (HF) structure of the photoexcited triplet state of pentacene dispersed in protonated and deuterated p-terphenyl single crystals. The strong electron spin polarization and long phase memory time of triplet pentacene enable us to perform the ENDOR measurements on the S=1 spin system at room temperature. Proton HF tensor elements and spin density values of triplet pentacene are extracted from a detailed angular-dependent study in which the orientation of the magnetic field is varied systematically in two different pentacene planes. Analysis reveals that the pentacene molecule is no longer planar in the p-terphenyl host lattice. The distortion is more pronounced in the deuterated crystal where the unit cell dimensions are slightly smaller than those of the protonated crystal.