Turning on Organic\nRadical Emitters

Radical emitters have attracted considerable interest\nbecause of\ntheir potential to surpass the limitations of singlet emitters due\nto spin statistics, thereby revolutionizing organic LEDs. Utilizing\nthe well-known Pariser–Parr–Pople (PPP) model for correlated\nelectrons in π-conjugated systems, we perform extended configuration\ninteraction with single, double, and triple excitations (XCISDT) to\nexplore the photophysics of various phenalenyl radicals differently\ndecorated with nitrogen atoms. By introducing the PPP particle-hole\ndifference operator and connecting it to DFT calculations, we offer\na new tool for predicting highly emissive organic radicals using ground-state\nquantum chemistry methods.