Organic Light‐Emitting Diodes Using a Neutral π Radical as Emitter: The Emission from a Doublet

Triplet harvesting is a main challenge in organic light-emitting devices (OLEDs), because the radiative decay of the triplet is spin-forbidden. Here, we propose a new kind of OLED, in which an organic open-shell molecule, (4-N-carbazolyl-2,6-dichlorophenyl)bis(2,4,6-trichlorophenyl)methyl (TTM-1Cz) radical, is used as an emitter, to circumvent the transition problem of triplet. For TTM-1Cz, there is only one unpaired electron in the highest singly occupied molecular orbital (SOMO). When this electron is excited to the lowest singly unoccupied molecular orbital (SUMO), the SOMO is empty. Thus, transition back of the excited electron to the SOMO is totally spin-allowed. Spectral analysis showed that electroluminescence of the OLED originated from the electron transition between SUMO and SOMO. The magneto-electroluminescence measurements revealed that the spin configuration of the excited state of TTM-1Cz is a doublet. Our results pave a new way to obtain 100% internal quantum efficiency of OLEDs.