Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 11, Issue 24, Pages 7265-7275Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200500610
Keywords
donor-acceptor Systems; fullerenes; host-guest systems; nanostructures; porphyrinoids; self-assembly
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Novel gold nanoparticles modified with a mixed self-assembled monolayer of porphyrin alkanethiol and short-chain alkanethiol were prepared (first step) to examine the size and shape effects of surface holes (host) on porphyrin-modified gold nanoparticles. ne porphyrin-modified gold nanoparticles with a size of about 10 nm incorporated C-60 molecules (guest) into the large, bucket-shaped holes, leading to the formation of a supramolecular complex of porphyrin-C-60 composites (second step). Large composite clusters with a size of 200400 nm were grown from the supramolecular complex of porphyrin-C-60 composites in mixed solvents (third step) and deposited electrophoretically onto nanostructured SnO2 electrodes (fourth step). Differences in the porphyrin:C-60, ratio were found to affect the structures and photoelectrochemical properties of the composite clusters in mixed solvents as well as on the SnO2, electrodes. The photoelectrochemical performance of a photoelectrochemical device consisting of SnO2 electrodes modified with the porphyrin-C-60 composites was enhanced relative to a reference system with small, wedged-shaped surface holes on the gold nanoparticle, Time-resolved transient absorption spectroscopy with fluorescence lifetime measurements suggest the occurrence of ultrafast electron transfer from the porphyrin excited singlet states to C-60 or the formation of a partial charge-transfer state in the composite clusters of supramolecular complexes formed between porphyrin and C-60 leading to efficient photocurrent generation in the system. Elucidation of the relationship between host-guest interactions and photoelectrochemical function in the present system will provide valuable information on the design of molecular devices and machines including molecular photo-voltaics.
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