251. Dynamic Evolving Exothermicity Steers Ultrafast Formation of a Correlated Triplet Pair State.
- Author
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Wu Y, Lu L, Yu B, Zhang S, Luo P, Chen M, He J, Li Y, Zhang C, Zhu J, Yao J, and Fu H
- Abstract
Singlet fission (SF) presents an attractive solution to overcome the Shockley-Queisser limit of single-junction solar cells. The conversion from an initial singlet state to final triplet is mediated by the correlated triplet pair state
1 (T1 T1 ). Despite significant advancement on1 (T1 T1 ) properties and its role in SF, a comprehensive understanding of the energetic landscape during SF is still unclear. Here, we study an unconventional SF system with excited-state aromaticity, i.e., cyano-substituted dipyrrolonaphtheridinedione derivative (DPND-CN), using time-resolved spectroscopy as a function of the temperature. We demonstrate that the population transfer from S1 to1 (T1 T1 ) is driven by a time-dependent exothermicity resulting from the coherent coupling between electronic and spin degrees of freedom. This is followed by thermal-activated dissociation of1 (T1 T1 ) to yield free triplets. Our results provide some new insight into the SF mechanism, which may guide the development of new efficient and stable SF materials for practical applications.- Published
- 2023
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