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We show from many-body quantum mechanical calculations that there occurstructurally distinct triplet-pair eigenstates in the intramolecular singletfission (iSF) compound pentacene-tetracene-pentacene. Triplet excitons occupyneigboring pentacene and tetracene monomers in the higher energy doublydegenerate triplet-triplet multiexcitons, and terminal pentacene chromophoresin the lower energy multiexciton. The lowest energy multiexciton is reached byultrafast triplet migration within the triplet-triplet manifold, a result withprofound implication for the design of superior iSF compounds.

Distinct contiguous versus separated triplet-pair multiexcitons in an intramolecular singlet fission chromophore