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We measure electrically detected magnetic resonance (EDMR) on organiclight-emitting diodes (OLEDs) made of the polymerpoly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) at roomtemperature and high magnetic fields, where spectral broadening of theresonance due to spin-orbit coupling (SOC) exceeds that due to the localhyperfine fields. Density-functional-theory calculations on an open-shell modelof the material reveal g-tensors of charge-carrier spins in the lowestunoccupied (electron) and highest occupied (hole) molecular orbitals. Thesetensors are used for simulations of magnetic resonance line-shapes. Besidesproviding the first quantification and direct observation of SOC effects oncharge-carrier states in these weakly SO-coupled hydrocarbons, this proceduredemonstrates that spin-related phenomena in these materials are fundamentallymonomolecular in nature.

Revealing weak spin-orbit coupling effects on charge carriers in a $\pi$-conjugated polymer