Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy

doi:10.1063/5.0200802

	Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy
	Peng, Bo; Wang, Ziyu; Jiang, Jiaming; Huang, Yifan; Liu, Weimin
	2024-05-21
发表期刊	JOURNAL OF CHEMICAL PHYSICS
ISSN	0021-9606
EISSN	1089-7690
卷号	160 期号:19
发表状态	已发表
DOI	10.1063/5.0200802
摘要	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 pi 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 S-2 (1(1)B(u)(+)) state populations in lycopene H-aggregates: a monomer-like singlet excited state relaxation pathway through S-2 (1(1)B(u)(+)) -> 1(1)B(u)(-) -> S-1 (2(1)A(g)(-)) and a dominant sequential singlet fission reaction pathway involving the S-2 (1(1)B(u)(+)) state, followed by S* state, a triplet pair state [(1)(TT)], eventually leading to a long lifetime triplet state T-1. Importantly, the presence of both anionic and cationic fingerprint Raman peaks in the S* state is indicative of a substantial charge-transfer character.
关键词	Aggregates Charge transfer Chromophores Energy utilization Excited states Femtosecond stimulated raman spectroscopies Fission process H-aggregates Lycopenes Reaction pathways S state Singlet excited state Singlet fissions Triplet state Ultra-fast
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收录类别	SCI ; EI
语种	英语
资助项目	National Natural Science Foundation of Chinahttps://doi.org/10.13039/501100001809[22373068] ; National Natural Science Foundation of China[F-0201-16-006]
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:001227733100002
出版者	AIP Publishing
EI入藏号	20242116125145
EI主题词	Quantum chemistry
EI分类号	406 Highway Engineering ; 412.2 Concrete Reinforcements ; 525.3 Energy Utilization ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 804.1 Organic Compounds ; 931.3 Atomic and Molecular Physics ; 931.4 Quantum Theory ; Quantum Mechanics
原始文献类型	Journal article (JA)
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/381239
专题	物质科学与技术学院物质科学与技术学院_PI研究组_刘伟民组物质科学与技术学院_PI研究组_黄逸凡组物质科学与技术学院_博士生大科学中心_公共科研平台_大科学装置建设部
通讯作者	Huang, Yifan; Liu, Weimin
作者单位	ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
第一作者的第一单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Peng, Bo,Wang, Ziyu,Jiang, Jiaming,et al. Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy[J]. JOURNAL OF CHEMICAL PHYSICS,2024,160(19).
APA	Peng, Bo,Wang, Ziyu,Jiang, Jiaming,Huang, Yifan,&Liu, Weimin.(2024).Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy.JOURNAL OF CHEMICAL PHYSICS,160(19).
MLA	Peng, Bo,et al."Investigation of ultrafast intermediate states during singlet fission in lycopene H-aggregate using femtosecond stimulated Raman spectroscopy".JOURNAL OF CHEMICAL PHYSICS 160.19(2024).