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  Ultrafast IR spectroscopy of photo-induced electron transfer in self-assembled donor-acceptor coordination cages.

Ahrens, J., Frank, M., Clever, G. H., & Schwarzer, D. (2017). Ultrafast IR spectroscopy of photo-induced electron transfer in self-assembled donor-acceptor coordination cages. Physical Chemistry Chemical Physics, 19(21), 13596-13603. doi:10.1039/c7cp02253k.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-5EE0-D Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-5EE4-5
Genre: Journal Article

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 Creators:
Ahrens, J.1, Author              
Frank, M., Author
Clever, G. H., Author
Schwarzer, D.1, Author              
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1Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_578600              

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 Abstract: Photo-induced processes in self-assembled coordination cages were studied by femtosecond infrared pump-probe spectroscopy. Densely packed, interpenetrated double cages were constructed from eight bis-monodentate redoxactive ligands bound to four Pd(ii) nodes. Two types of ligands consisting of electron rich phenothiazine (PTZ) or electron deficient anthraquinone (ANQ) chromophores were used to assemble either homo-octameric or mixed-ligand cages. Upon photoexcitation the homo-octameric acceptor cage undergoes intersystem crossing to a long-lived triplet state, similar to the free acceptor ligand. Excitation of the free donor ligand leads to a fluorescent state with intramolecular charge transfer character. This fluorescence is completely quenched in the homo-octameric donor double cage due to a ligand-to-metal charge transfer followed by back electron transfer on a ps timescale. Only for the mixed-ligand cage irradiation produces a charge separated state with an oxidized PTZ radical cation and a reduced ANQ radical anion as proven by their vibrational fingerprints in the transient IR spectra. In dichloromethane the lifetime of this charge separated state extends from tens of ps to >1.5 ns which is attributed to the broad distribution of mixed-ligand cages with different stoichiometry and/or stereo configurations.

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Language(s): eng - English
 Dates: 2017-05-122017-05-31
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1039/c7cp02253k
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Title: Physical Chemistry Chemical Physics
Source Genre: Journal
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Pages: - Volume / Issue: 19 (21) Sequence Number: - Start / End Page: 13596 - 13603 Identifier: -