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Singlet fission (SF), a spin-allowed multiexciton generation process, experienced renewed interest in the last decade due to its potential to increase the efficiency of photovoltaic devices. The hurdles now lie in the limited range of SF-capable materials and demanding morphology requirement for an efficient fission process. Although primary fission to yield triplet pair (1TT) can occur independently of film morphology in intramolecular singlet fission (iSF) materials, the separation of the 1TT state has been shown to be highly dependent on the packing motif and morphologies. In this work, we have demonstrated that both iSF and triplet pair separation processes took place irrelevant of molecular order and/or film morphology in a series of pentalene compounds. With the >180% fission efficiency, the suitable triplet energy levels, and the long lifetime of the triplet excitons, these iSF systems can be integrated into practical photovoltaic application. [ABSTRACT FROM AUTHOR]