Turning on Organic Radical Emitters

Radical emitters have attracted considerable interest because of their potential to surpass the limitations of singlet emitters due to spin statistics, thereby revolutionizing organic LEDs. Utilizing the well-known Pariser–Parr–Pople (PPP) model for correlated electrons in π-conjugated systems, we perform extended configuration interaction with single, double, and triple excitations (XCISDT) to explore the photophysics of various phenalenyl radicals differently decorated with nitrogen atoms. By introducing the PPP particle-hole difference operator and connecting it to DFT calculations, we offer a new tool for predicting highly emissive organic radicals using ground-state quantum chemistry methods.