Abstract
Harvesting multiexcitons generated by singlet fission (SF) holds promise for advancing optoelectronic devices and photochemistry. Conventional approaches focus on interfacial exciton or charge transfer after dephasing the triplet-pair [T1T1] to low-energy free triplets. However, the high potential [T1T1] state possesses a unique characteristic multi-reference wavefunction, opening new opportunities for advancing underexplored multiexciton-driven photochemical processes. Here, we report a functional multicomponent system with covalently integrated electron-rich moieties to direct multiexciton charge transfer specifically from the [T1T1] state to a charge separated (CS) state. We elucidate the design rules of these second generation [G2] SF chromophores that favor multiexciton-driven charge separation prior to dephasing into free triplets. Our spectroscopic studies reveal how the same SF system can mediate either generation of free triplets or CS formation from [T1T1] by modulating the local dielectric environment. These findings provide fundamental insights into multiexciton dynamics and lay the foundation for unconventional multiexciton-driven energy conversion systems.
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