Abstract
AbstractSinglet fission (SF), in which one singlet exciton (S1) splits into two triplets (T1) on adjacent molecules through a correlated triplet‐pair 1(TT) state, requires precise but difficult tuning of exciton energetics and intermolecular electronic couplings in the solid state. Antiaromatic 4nπ dibenzopentalenes (DPs) are demonstrated as a new class of single‐chromophore‐based intramolecular SF materials that exhibit an optically allowed S2 state with E(S2)>2×E(T1) and an optically forbidden S1 state. Ultrafast population transfer from a high‐lying S2 state to a 1(TT) state was observed in monomeric solution of styryl‐substituted DP (SDP) on a sub‐picosecond timescale. There is evidence of exciton diffusion (ED) of the 1(TT) state to yield two individual long‐lived triplets in SDP thin film. The overall triplet yield via intramolecular SF and subsequent triplet‐pair diffusion can be as high as 142±10 % in thin film.
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