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学科主题: 物理化学
题名: Photophysical Properties of Self-Assembled Multinuclear Platinum Metallacycles with Different Conformational Geometries
作者: Chen, Jun-Sheng1, 2;  Zhao, Guang-Jiu1;  Cook, Timothy R.3;  Han, Ke-Li1;  Stang, Peter J.3
通讯作者: 韩克利 ;  Peter J. Stang
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2013-05-01
DOI: 10.1021/ja402421w
卷: 135, 期:17, 页:6694-6702
收录类别: SCI
合作性质: 
文章类型: Article
部门归属: 11
项目归属: 1101
产权排名: 待补充
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
资助者: 1,1
研究领域[WOS]: Chemistry
英文摘要: In this work, spectroscopic techniques and quantum chemistry calculations were used to investigate the photophysical properties of various multinuclear platinum complexes with different conformational geometries. This suite of complexes includes a Pt-pyridyl square, a Pt-carboxylate triangle, and a mixed Pt-pyridyl-carboxylate rectangle, as well as two mononuclear Pt model complexes. Studying the individual molecular precursors in the context of larger assemblies is important to provide a complete understanding of the factors governing the observed photophysical properties of a given system. The absorption and emission bands of the parent linear dipyridyl donor (ligand 1) are largely preserved in the [4 + 4] square and the multicomponent [4 + 2 + 2] rectangle (3 and 4, respectively), with significant red shifts. The [3 + 3] Pt-carboxylate triangle containing p-phthalic acid is nonemissive. Phosphorescence and nanosecond transient spectroscopy on 3 and 4 reveal that the introduction of platinum atoms enhances spin-orbital coupling, thereby increasing the rate of intersystem crossing. This phenomenon is consistent with the low fluorescence quantum yields and short fluorescence lifetimes of 3 and 4. Moreover, the electronic structures for the ground state and low-lying excited states of these compounds were studied using quantum chemistry calculations. The fluorescent states of the platinum complexes are local excited states of ligand-centered pi-pi* transition features, whereas the nonfluorescent states are intramolecular charge-transfer states. These low-lying intramolecular charge-transfer states are responsible for the nonemissive nature of small molecules 1 and 2 and triangle S. As the interactions between these components determine the properties of their corresponding assemblies, we establish novel excited-state decay mechanisms which dictate the observed spectra.
关键词[WOS]: DENSITY-FUNCTIONAL CALCULATIONS ;  TRIPLET EXCITED-STATES ;  GAUSSIAN-BASIS SETS ;  CHARGE-TRANSFER ;  MOLECULAR DESIGN ;  ATOMS LI ;  COMPLEXES ;  COORDINATION ;  FLUORESCENCE ;  SYMMETRY
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000318469100046
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/119411
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, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Univ Utah, Dept Chem, Salt Lake City, UT 84112 USA

Recommended Citation:
Chen, Jun-Sheng,Zhao, Guang-Jiu,Cook, Timothy R.,et al. Photophysical Properties of Self-Assembled Multinuclear Platinum Metallacycles with Different Conformational Geometries[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2013,135(17):6694-6702.
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