- Tytuł:
- Singlet Fission in a New Series of Systematically Designed Through-space Coupled Tetracene Oligomers
- Autorzy:
-
Yang, Shang-Da
Chen, Bo-Han
Hsu, Chao-Hsien
Majdecki, Maciej
Zakrocka, Magdalena
Chou, Pi-Tai
Wang, Chih-Hsing
Shi, Emily Hsue-Chi
Wei, Yu-Chen
Lu, Chih-Hsuan
Gaweł, Przemysław - Wydawca:
- Wiley
- Cytata wydawnicza:
- Angew. Chem. Int. Ed. 2024, e202401103 ; https://doi.org/10.1002/anie.202401103
- Opis:
-
Polish National Science Centre (SONATA 2020/39/D/ST4/00560);
National Agency for Academic Exchange (Polish Returns PPN_PPO_2020_1_00012);
Poland’s high-performance Infrastructure PLGrid (HPC Centers: ACK Cyfronet AGH, PCSS, CI TASK, WCSS) grant no.: PLG/2021/014515, PLG/2022/01539 and PLG/2023/016125;
National Science and Technology Council (grant no. NSTC-112-2639-M-002-007-ASP)
Singlet fission (SF) holds great promise for current photovoltaic technologies, where tetracenes, with their relatively high triplet energies, play a major role for application in silicon-based solar cells. However, the SF efficiencies in tetracene dimers are low due to the unfavorable energetics of their singlet and triplet energy levels. In the solid state, tetracene exhibits high yields of triplet formation through SF, raising great interest about the underlying mechanisms. To address this discrepancy, we designed and prepared a novel molecular system based on a hexaphenylbenzene core decorated with 2 to 6 tetracene chromophores. The spatial arrangement of tetracene units, induced by steric hindrance in the central part, dictates through-space coupling, making it a relevant model for solid-state chromophore organization. We then revealed a remarkable increase in SF quantum yield with the number of tetracenes, reaching quantitative (196 %) triplet pair formation in hexamer. We observed a short-lived correlated triplet pair and limited magnetic effects, indicating ineffective triplet dissociation in these through-space coupled systems. These findings emphasize the crucial role of the number of chromophores involved and the interchromophore arrangement for the SF efficiency. The insights gained from this study will aid designing more efficient and technology-compatible SF systems for applications in photovoltaics. - Dostawca treści:
- Repozytorium Centrum Otwartej Nauki
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