Theory of exciton-polaron complexes in pulsed electrically detected magnetic resonance

Several microscopic pathways have been proposed to explain the large magnetic effects observed in organic semiconductors; however, it is difficult to identify and characterize the microscopic process which actually influences the overall magnetic field response in a particular instance. Pulsed electrically detected magnetic resonance provides an ideal platform for this task as it intrinsically monitors the charge carriers of interest and provides dynamical information which is inaccessible through conventional magnetoconductance measurements. Here we develop a general time-domain theory to describe the spin-dependent recombination of exciton-polaron complexes following the coherent manipulation of paramagnetic centers through electron paramagnetic resonance. A general Hamiltonian is treated, and it is shown that the transition frequencies and resonance positions of the exciton-polaron complex can be used to estimate interspecies coupling. This work also provides a general formalism for analyzing multipulse experiments which can be used to extract relaxation and transport rates.