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Title: Ultrafast, Light-Induced Electron Transfer in a Perylene Diimide Chromophore-Donor Assembly on TiO 2

Journal Article · · Journal of Physical Chemistry Letters
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  1. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States
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Surface-bound, perylenediimide (PDI)-based molecular assemblies have been synthesized on nanocrystalline TiO2 by reaction of a dianhydride with a surface-bound aniline and succinimide bonding. In a second step, the Fe(II) polypyridyl complex [FeII(tpy-PhNH2)2]2+ was added to the outside of the film, also by succinimide bonding. Ultrafast transient absorption measurements in 0.1 M HClO4 reveal that electron injection into TiO2 by 1PDI* does not occur, but rather leads to the ultrafast formation of the redox-separated pair PDI•+,PDI•–, which decays with complex kinetics (τ1 = 0.8 ps, τ2 = 15 ps, and τ3 = 1500 ps). With the added Fe(II) polypyridyl complex, rapid (<25 ps) oxidation of Fe(II) by the PDI•+,PDI•– redox pair occurs to give Fe(III),PDI•– persisting for >400 μs in the film environment.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001011; AC05-06OR23100
OSTI ID:
1226090
Alternate ID(s):
OSTI ID: 1387241
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Vol. 6 Journal Issue: 23; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

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Figures / Tables (4)

Chart 1(p. 2)figure Chart 1
Figure 1(p. 2)figure Figure 1
Scheme 1(p. 2)figure Scheme 1
Figure 2(p. 3)figure Figure 2

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
perylene bisimide
surface-bound
interfacial reaction
hole transfer
organic semiconductor