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Quantifying the spin-spin interactions which influence electronic transitionsin organic semiconductors is crucial for understanding theirmagneto-optoelectronic properties. By combining a theoretical model for threespin interactions in the coherent regime with pulsed electrically detectedmagnetic resonance experiments on MEH-PPV diodes, we quantify the spin-couplingwithin complexes comprising three spin-half particles. We determine that theseparticles form triplet-exciton:polaron pairs, where the polaron:excitonexchange is over 5 orders of magnitude weaker (less than 170 MHz) than thatwithin the exciton. This approach providing a direct spectroscopic approach fordistinguishing between coupling regimens, such as strongly bound trions, whichhave been proposed to occur in organic devices.

Using coherent dynamics to quantify spin-coupling within triplet-exciton/polaron complexes in organic diodes