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The efficiency of an organic light-emitting diode (OLED) depends on themicroscopic orientation of transition dipole moments of the molecular emitters.The most effective materials used for light generation have threefold symmetry,which prohibit a priori determination of dipole orientation due to thedegeneracy of the fundamental transition. Single-molecule spectroscopy revealsthat the model triplet emitter tris(2-phenylisoquinoline)iridium(III)(Ir(piq)3) does not behave as a linear dipole, radiating with lowerpolarization anisotropy than expected. Spontaneous symmetry breaking occurs inthe excited state, leading to a random selection of one of the three ligands toform a charge transfer state with the metal. This non-deterministiclocalization is revealed in switching of the degree of linear polarization ofphosphorescence. Polarization scrambling likely raises out-coupling efficiencyand should be taken into account when deriving molecular orientation of theguest emitter within the OLED host from ensemble angular emission profiles.

Spontaneous fluctuations of transition dipole moment orientation in OLED triplet emitters