Toward quantitative prediction of molecular fluorescence quantum efficiency: Role of Duschinsky rotation
文献类型：期刊论文
| 作者 | Peng, Qian; Yi, Yuanping; Shuai, Zhigang; Shao, Jiushu |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2007-08-01 |
| 卷号 | 129期号:30页码:9333-9339 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/ja067946e |
| 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. |
| 语种 | 英语 |
| WOS记录号 | WOS:000248281100033 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/60495]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Shuai, Zhigang |
| 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 |
| 推荐引用方式 GB/T 7714 | 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. |
| APA | Peng, Qian,Yi, Yuanping,Shuai, Zhigang,&Shao, Jiushu.(2007).Toward quantitative prediction of molecular fluorescence quantum efficiency: Role of Duschinsky rotation.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,129(30),9333-9339. |
| MLA | Peng, Qian,et al."Toward quantitative prediction of molecular fluorescence quantum efficiency: Role of Duschinsky rotation".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 129.30(2007):9333-9339. |
入库方式： OAI收割
来源：化学研究所
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