Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 19, Issue 16, Pages 5088-5096Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201203913
Keywords
electrochemistry; electron transfer; gold; molecular wires; self-assembly
Categories
Funding
- MEXT of Japan [24750054, 21108002]
- JSPS Research Fellowship for Young Scientists
- Global COE Program for Chemistry Innovation
- The Japan Prize Foundation
- Iketani Science and Technology Foundation
- The Murata Science Foundation
- Grants-in-Aid for Scientific Research [21108002, 21108001, 12J08850, 24750054, 23245029] Funding Source: KAKEN
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This article completes our comprehensive understanding of the electron transport properties of our original -conjugated redox-active molecular wires comprising Fe bridged by p-phenylene linkers (tpy=2,2:6,2-terpyridine). The Fe(tpy)2 oligomer wires comprise three types of tpy ligands: the anchor tpy ligand (A series) makes a junction between the wire and electrode, the bridging bis-tpy ligand (L series) connects the Fe(tpy)2 units, and the terminal tpy ligand (T series) possesses a redox site as a probe for the long-range electron transport ability. Taking advantage of the precise tunability of the composition of the Fe(tpy)2 oligomer wires, thus far we investigated how A and L impacted on the electron-transport ability. The excellent long-range electron transport ability with ultrasmall attenuation constants (d, 0.002 angstrom 1 as the minimum) depends on L significantly [Chem. Asian J. 2009, 4, 1361], whereas A is unrelated to the d value, but influences the zero-distance electron-transfer rate constant, ket0 [J. Am. Chem. Soc. 2010, 132, 4524]. Herein we study the influence of terminal ligand Tx (x=13). d is independent of T, however, T3, with a cyclometallated Ru complex as the redox site, gives rise to a ket0 value greater than T1 and T2 with ferrocene. This series of simple but definitive conclusions indicates that we have reached the stage of being able to precisely design molecular wires to attain desirable single-molecule electron conduction.
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