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Updated: Jun 18, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Tailoring Molecular Architectures for Intramolecular Charge Separation of the Multiexciton State Generated by Singlet
Guiying He1,2, Huaxi Huang3, Bernardo Salcido-Santacruz2,4
1Department of Physics, Graduate Center, City University of New York, New York, New York 10016, United States.
Abstract:
Harvesting multiexcitons generated by singlet fission (SF) holds promise for advancing optoelectronic devices and photochemistry. Conventional approaches have previously focused on interfacial exciton or charge transfer after dephasing the triplet-pair [T1T1] to low-energy free triplets. However, multiexciton-driven processes that directly leverage the unique characteristic multireference wave function of the [T1T1] state and its high chemical potential are underexplored, opening new opportunities for advancing photochemistry. Here, we report a functional multicomponent system with covalently integrated electron-rich moieties to direct multiexciton charge transfer directly from the [T1T1] state to a charge-separated diradical (CS) state, a previously unreported transformation. We elucidate the design rules of second generation [G2] SF chromophores using spectroscopic studies, including the role of the local dielectric environment in modulating the fate of the triplet pair from conventional triplet pair dephasing to multiexciton charge separation. These findings provide fundamental insights into multiexciton dynamics and lay the foundation for unconventional multiexciton-driven energy conversion systems.
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