Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.096
Publication date: 18th July 2019
Singlet fission refers to the conversion of a singlet state (S1) to two triplet states (2xT1). There have been lingering confusions and debates on the nature of the all-important triplet pair intermediate states. Here we attempt to clarify the confusions from both theoretical and experimental perspectives. We distinguish the triplet pair state which maintains electronic coherence between the two constituent triplets from one which does not. The former is characterized by distinct experimental signatures and its formation may occur via incoherent and/or vibronic coherent mechanisms. We present our recent attempts at tuning the energetics of the triplet pair states and, thus, the energetics of singlet fission; this approach may be used to greatly expand the molecular toolbox for singlet fission. Finally, we discuss the challenges in treating singlet fission beyond the dimer approximation, in understanding the often neglected roles of delocalization on singlet fission rates, and in realizing the much lauded goal of increasing solar energy conversion efficiencies with singlet fission chromophores.
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