Proceedings of Online International Conference on Hybrid and Organic Photovoltaics (OnlineHOPV20)
DOI: https://doi.org/10.29363/nanoge.onlinehopv.2020.013
Publication date: 22nd May 2020
Multiexciton generation through singlet fission has the potential of exceeding Shockley–Queisser limit in photovoltaic devices. However, only very few materials suitable for singlet fission are available at present and the mechanism of inter- and intra-molecular singlet fission are not fully understood. Detailed knowledge regarding the processes is crucial for developing new materials. In this talk, I will present the significance of electronic spin density distribution in facilitating efficient intramolecular singlet exciton fission (iSEF) in π-bridged pentacene dimers. We synthetically modulate the spin density distribution in a series of pentacene dimers using phenyl-, thienyl- and selenyl- flanked diketopyrrolopyrrole (DPP) derivatives as π-bridges. Using femtosecond transient absorption spectroscopy, we find that efficient iSEF is only observed for the phenyl-derivative in ~2.4 ps while absent in the other two dimers. Electronic structure calculations reveal that phenyl-DPP bridge localizes α- and β-spin densities on distinct terminal pentacenes. Upon photoexcitation, a spin exchange mechanism enables iSEF from a singlet state which has an innate triplet pair character. This emergent mechanism should motivate new time-resolved experiments for spin-state tracking in SEF-active materials, while bringing into focus the use of chromophoric bridges, which can simultaneously act as antennas for sensitizing iSEF and fine-tune the properties that enable fission.
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