The singlet fission process involves the conversion of one singlet excited state into two triplet states, which has significant potential for enhancing the energy utilization efficiency of solar cells. Carotenoid, a typical π conjugated chromophore, exhibits specific aggregate morphologies known to display singlet fission behavior. In this study, we investigate the singlet fission process in lycopene H-aggregates using femtosecond stimulated Raman spectroscopy aided by quantum chemical calculation. The experimental results reveal two reaction pathways that effectively relax the S2 (11Bu+) state populations in lycopene H-aggregates: a monomer-like singlet excited state relaxation pathway through S2 (11Bu+) → 11Bu− → S1 (21Ag−) and a dominant sequential singlet fission reaction pathway involving the S2 (11Bu+) state, followed by S* state, a triplet pair state [1(TT)], eventually leading to a long lifetime triplet state T1. Importantly, the presence of both anionic and cationic fingerprint Raman peaks in the S* state is indicative of a substantial charge-transfer character.
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21 May 2024
Research Article|
May 17 2024
Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy Available to Purchase
Special Collection:
Light-matter Interaction at the Nano and Molecular Scale
Bo Peng;
Bo Peng
(Data curation, Formal analysis, Methodology, Writing – original draft)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
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Ziyu Wang;
Ziyu Wang
(Investigation, Methodology, Visualization)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
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Jiaming Jiang;
Jiaming Jiang
(Conceptualization, Investigation, Methodology)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
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Yifan Huang
;
Yifan Huang
a)
(Methodology, Project administration, Software, Supervision, Writing – review & editing)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
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Weimin Liu
Weimin Liu
a)
(Methodology, Project administration, Supervision, Writing – review & editing)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
Search for other works by this author on:
Bo Peng
Data curation, Formal analysis, Methodology, Writing – original draft
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
Ziyu Wang
Investigation, Methodology, Visualization
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
Jiaming Jiang
Conceptualization, Investigation, Methodology
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
Yifan Huang
Methodology, Project administration, Software, Supervision, Writing – review & editing
a)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
Weimin Liu
Methodology, Project administration, Supervision, Writing – review & editing
a)
School of Physical Science and Technology, ShanghaiTech University
, Shanghai 201210, China
J. Chem. Phys. 160, 194304 (2024)
Article history
Received:
January 29 2024
Accepted:
April 22 2024
Citation
Bo Peng, Ziyu Wang, Jiaming Jiang, Yifan Huang, Weimin Liu; Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy. J. Chem. Phys. 21 May 2024; 160 (19): 194304. https://doi.org/10.1063/5.0200802
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