A Combined Experimental and Computational Study of Linear Ruthenium(II) Coordination Oligomers with End-Capping Organic Redox Sites: Insight into the Light Absorption and Charge Delocalization

doi:10.1002/chem.201301319

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	A Combined Experimental and Computational Study of Linear Ruthenium(II) Coordination Oligomers with End-Capping Organic Redox Sites: Insight into the Light Absorption and Charge Delocalization
	Yao, Chang-Jiang 1,2; Zheng, Ren-Hui 3; Nie, Hai-Jing 1; Cui, Bin-Bin 1,2; Shi, Qiang 3; Yao, Jiannian 1; Zhong, Yu-Wu 1
刊名	CHEMISTRY-A EUROPEAN JOURNAL
	2013-09-09
卷号	19 期号:37 页码:12376-12387
关键词	Coordination Oligomers Density Functional Calculations Ruthenium Triarylamines
ISSN号	0947-6539
DOI	10.1002/chem.201301319
英文摘要	Two series of linear ruthenium coordination oligomers, [(Ntpy)Ru-n(tppz)(n-1)(tpy)](2n+) (mono-Ntpy series, n=1-3) and [(Ntpy)(2)Ru-n(tppz)(n-1)](2n+) (bis-Ntpy series, n=1-3) have been prepared, where Ntpy is the capping ligand 4-di-p-anisylamino-2,2:6,2-terpyridine, tppz is tetra-2-pyridylpyrazine, and tpy is 2,2:6,2-terpyridine. The electrochemical measurements evidence oxidation events from both the amine segments and the metal centers and reduction waves from tppz and the capping ligands. Both series complexes display much enhanced light absorption with respect to model complexes without terminal amine units. Density functional theory (DFT) calculations have been performed on both series and time-dependent DFT (TD-DFT) calculations have been performed on the bis-Ntpy-series compounds (n=1-4) to characterize their electronic structures and excited states and predict the electronic properties of long-chain polymers. Upon one-electron oxidation, the mono-Ntpy-series monoruthenium and diruthenium complexes display N+-localized transitions and metal-to-nitrogen charge-transfer (MNCT) transitions in the near-infrared (NIR) region. DFT and TD-DFT computations on the one-electron-oxidized forms of the mono-Ntpy-series compounds (n=1-4) provide insight into the nature of the MNCT transitions and the degree of charge delocalization.
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000323731200029
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/54445]
专题	中国科学院化学研究所
通讯作者	Zhong, Yu-Wu
作者单位	1.Chinese Acad Sci, Inst Chem, CAS Key Lab Photochem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Yao, Chang-Jiang,Zheng, Ren-Hui,Nie, Hai-Jing,et al. A Combined Experimental and Computational Study of Linear Ruthenium(II) Coordination Oligomers with End-Capping Organic Redox Sites: Insight into the Light Absorption and Charge Delocalization[J]. CHEMISTRY-A EUROPEAN JOURNAL,2013,19(37):12376-12387.
APA	Yao, Chang-Jiang.,Zheng, Ren-Hui.,Nie, Hai-Jing.,Cui, Bin-Bin.,Shi, Qiang.,...&Zhong, Yu-Wu.(2013).A Combined Experimental and Computational Study of Linear Ruthenium(II) Coordination Oligomers with End-Capping Organic Redox Sites: Insight into the Light Absorption and Charge Delocalization.CHEMISTRY-A EUROPEAN JOURNAL,19(37),12376-12387.
MLA	Yao, Chang-Jiang,et al."A Combined Experimental and Computational Study of Linear Ruthenium(II) Coordination Oligomers with End-Capping Organic Redox Sites: Insight into the Light Absorption and Charge Delocalization".CHEMISTRY-A EUROPEAN JOURNAL 19.37(2013):12376-12387.