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题名: Toward quantitative prediction of molecular fluorescence quantum efficiency: Role of Duschinsky rotation
作者: Peng, Qian;  Yi, Yuanping;  Shuai, Zhigang;  Shao, Jiushu
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2007-08-01
DOI: 10.1021/ja067946e
卷: 129, 期:30, 页:9333-9339
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: It is a highly desirable but difficult task to predict the molecular fluorescence quantum efficiency from first principles. The molecule in the excited state can undergo spontaneous radiation, conversion of electronic energy to nuclear motion, or chemical reaction. For relatively large molecules, it is impossible to obtain the full potential energy surfaces for the ground state and the excited states to study the excited-state dynamics. We show that, under harmonic approximation by considering the Duschinsky rotation effect, the molecular fluorescence properties can be quantitatively calculated from first principles coupled with our correlation function formalism for the internal conversion. In particular, we have explained the peculiar fluorescence behaviors of two isomeric compounds, cis,cis-1,2,3,4-tetraphenyl-1,3-butadiene and 1,1,4,4-tetraphenyl-butadiene, the former being nonemissive in solution and strongly emissive in aggregation or at low temperature, and the latter being strongly emissive in solution. The roles of low-frequency phenyl ring twist motions and their Duschinsky mode mixings are found to be crucial, especially to reveal the temperature dependence. As an independent check, we take a look at the well-established photophysics of 1,4-diphenylbutadiene for its three different conformers. Both the calculated radiative and nonradiative rates are in excellent agreement with the available experimental measurements.
关键词[WOS]: AB-INITIO CALCULATIONS ;  FRANCK-CONDON FACTORS ;  RESTRICTED INTRAMOLECULAR ROTATION ;  AGGREGATION-INDUCED EMISSION ;  DENSITY-FUNCTIONAL METHODS ;  POTENTIAL-ENERGY SURFACES ;  EXCITED-STATE GEOMETRY ;  LIGHT-EMITTING-DIODES ;  ELECTRON-TRANSFER ;  VIBRONIC SPECTRA
语种: 英语
WOS记录号: WOS:000248281100033
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/140415
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Key Lab Organ Solids, Beijing 100080, Peoples R China
2.Beijing Normal Univ, Dept Chem, Beijing 100875, Peoples R China
3.Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100080, Peoples R China

Recommended Citation:
Peng, Qian,Yi, Yuanping,Shuai, Zhigang,et al. Toward quantitative prediction of molecular fluorescence quantum efficiency: Role of Duschinsky rotation[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2007,129(30):9333-9339.
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