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

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