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题名: Tuning the luminescence lifetimes of ruthenium(II) polypyridine complexes and its application in luminescent oxygen sensing
作者: Ji, Shaomin1;  Wu, Wanhua1;  Wu, Wenting1;  Song, Peng2;  Han, Keli2;  Wang, Zhonggang3;  Liu, Shasha2;  Guo, Huimin4;  Zhao, Jianzhang1
刊名: JOURNAL OF MATERIALS CHEMISTRY
发表日期: 2010
DOI: 10.1039/b916468e
卷: 20, 期:10, 页:1953-1963
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Materials Science
英文摘要: Ru(Phen)(bpy)(2) (1) and its new derivatives (2-5) with pyrenyl or ethynylated pyrene and phenyl units appended to the 3-position of the phenanthroline (Phen) ligand were prepared and these complexes generate long-lived room temperature phosphorescence in the red and near IR range (600-800 nm). The photophysical properties of these complexes were investigated by UV-Vis absorption, luminescence emission, transient absorption spectra and DFT/TDDFT calculations. We found the luminescence lifetime (tau)can be drastically extended by ligand modification (increased up to 140-fold), e. g. tau = 58.4 mu s for complex 3 (with pyrenyl ethynylene appendents) was found, compared to tau = 0.4 mu s for the reference complex 1. Ethynylated phenyl appendents alter the tau also (complex 2, tau = 2.4 mu s). With pyrenyl appendents (4 and 5), lifetimes of 2.5 mu s and 9.2 mu s were observed. We proposed three different mechanisms for the lifetime extension of 2, 3, 4 and 5. For 2, the stabilization of the (3)MLCT state by pi-conjugation is responsible for the extension of the lifetime. For 3, the emissive state was assigned as an intra-ligand (IL) long-lived (3)pi-pi* state ((3)IL/(3)LLCT, intraligand or ligand-to-ligand charge transfer), whereas a C-C single bond linker results in a triplet state equilibrium between 3MLCT state and the pyrene localized (3)pi-pi* triplet state ((3)IL, e.g. 4 and 5). DFT/TDDFT calculations support the assignment of the emissive states. The effects of the lifetime extension on the oxygen sensing properties of these complexes were studied in both solution and polymer films. With tuning the emissive states, and thus extension of the luminescence lifetimes, the luminescent O(2) sensing sensitivity of the complexes can be improved by ca. 77-fold in solution (I(0)/I(100) 1438 for complex 3, vs. I(0)/I(100) = 18.5 for complex 1). In IMPES-C polymer films, the apparent quenching constant K(SV)(app) is improved by 150-fold from 0.0023 Torr(-1) (complex 1) to 0.35 Torr(-1) (complex 3). The K(SV)(app) value of complex 3 is even higher than that of PtOEP under similar conditions (0.15 Torr(-1)).
关键词[WOS]: ROOM-TEMPERATURE PHOSPHORESCENCE ;  TRANSITION-METAL-COMPLEXES ;  ELECTRON-TRANSFER DYNAMICS ;  EXCITED-STATE LIFETIMES ;  RU-II COMPLEXES ;  CHARGE-TRANSFER ;  PHOTOPHYSICAL PROPERTIES ;  ENERGY-TRANSFER ;  SPECTROSCOPIC PROPERTIES ;  TRIPLET-STATE
语种: 英语
WOS记录号: WOS:000274920500017
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141692
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.Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116012, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Dalian Univ Technol, Sch Chem Engn, Dept Polymer Sci & Mat, Dalian 116012, Peoples R China
4.Dalian Univ Technol, Sch Chem Engn, Dept Chem, Dalian 116012, Peoples R China

Recommended Citation:
Ji, Shaomin,Wu, Wanhua,Wu, Wenting,et al. Tuning the luminescence lifetimes of ruthenium(II) polypyridine complexes and its application in luminescent oxygen sensing[J]. JOURNAL OF MATERIALS CHEMISTRY,2010,20(10):1953-1963.
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