"Watching" the Dark State in Ultrafast Nonadiabatic Photoisomerization Process of a Light-Driven Molecular Rotary Motor
文献类型：期刊论文
| 作者 | Pang, Xiaojuan1,2; Cui, Xueyan1,2; Hu, Deping3; Jiang, Chenwei1,2; Zhao, Di1,2; Lan, Zhenggang3; Li, Fuli1,2
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| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY A
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| 出版日期 | 2017-02-16 |
| 卷号 | 121期号:6页码:1240-1249 |
| 英文摘要 | Photoisomerization dynamics of a light-driven molecular rotary motor, 9-(2-methyl-2,3-dihydro-1H-cyclopenta[a]naphthalen-1-ylidene)-9H-fluorene, is investigated with trajectory surface-hopping dynamics at the semiempirical OM2/MRCI level. The rapid population decay of the S-1 excited state for the M isomer is observed, with two different decay time scales (500 fs and 1.0 ps). By weighting the contributions of fast and slow decay trajectories, the averaged lifetime of the S-1 excited state is about 710 fs. The calculated quantum yield of the M-to-P photoisomerization of this molecular rotary motor is about 59.9%. After the S-0 -> S-1, excitation, the dynamical process of electronic decay is followed by twisting about the central C=C double bond and the motion of pyramidalization at the carbon atom of the stator-axle linkage. Although two S-0/S-1 minimum-energy conical intersections are obtained at the OM2/MRCI level, only one conical intersection is found to be responsible for the nonadiabatic dynamics. The existence of "dark state" in the molecular rotary motor is confirmed through the simulated time-resolved fluorescence emission spectrum. Both quenching and red shift of fluorescence emission spectrum observed by Conyard et al. [Conyard, J.; Addison, K.; Heisler, I. A.; Cnossen, A.; Browne, W.R.; Feringa, B. L.; Meech, S.R. Nat. Chem. 2012, 4, 547-551; Conyard, J.; Conssen, A.; Browne, W. R.; Feringa, B. L.; Meech, S. R. J. Am. Chem. Soc. 2014, 136, 9692-9700] are well understood. We find that this "dark state" in the molecular rotary motor is not a new electronic state, but the "dark region" with low oscillator strength on the initial S-1 state. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 类目[WOS] | Chemistry, Physical ; Physics, Atomic, Molecular & Chemical |
| 研究领域[WOS] | Chemistry ; Physics |
| 关键词[WOS] | CONICAL INTERSECTIONS ; SEMIEMPIRICAL METHODS ; AB-INITIO ; UNIDIRECTIONAL ROTATION ; COMPUTATIONAL DESIGN ; WORKING MECHANISM ; RATE ACCELERATION ; PROTON-TRANSFER ; DYNAMIC CONTROL ; DECAY DYNAMICS |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000394482500009 |
| 源URL | [http://ir.qibebt.ac.cn/handle/337004/9305]  |
| 专题 | 青岛生物能源与过程研究所_先进材料理论与模拟团队 |
| 作者单位 | 1.Xi An Jiao Tong Univ, Key Lab Quantum Informat & Quantum Optoelect Devi, Xian 710049, Shaanxi, Peoples R China 2.Xi An Jiao Tong Univ, Dept Appl Phys, Xian 710049, Shaanxi, Peoples R China 3.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, 189 Songling Rd, Qingdao 266101, Shandong, Peoples R China |
| 推荐引用方式 GB/T 7714 | Pang, Xiaojuan,Cui, Xueyan,Hu, Deping,et al. "Watching" the Dark State in Ultrafast Nonadiabatic Photoisomerization Process of a Light-Driven Molecular Rotary Motor[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2017,121(6):1240-1249. |
| APA | Pang, Xiaojuan.,Cui, Xueyan.,Hu, Deping.,Jiang, Chenwei.,Zhao, Di.,...&Li, Fuli.(2017)."Watching" the Dark State in Ultrafast Nonadiabatic Photoisomerization Process of a Light-Driven Molecular Rotary Motor.JOURNAL OF PHYSICAL CHEMISTRY A,121(6),1240-1249. |
| MLA | Pang, Xiaojuan,et al.""Watching" the Dark State in Ultrafast Nonadiabatic Photoisomerization Process of a Light-Driven Molecular Rotary Motor".JOURNAL OF PHYSICAL CHEMISTRY A 121.6(2017):1240-1249. |
入库方式： OAI收割
来源：青岛生物能源与过程研究所
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