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

Physical Chemistry Chemical Physics : PCCP
Jennifer AhrensDirk Schwarzer

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 distri...Continue Reading

References

Apr 22, 2004·Journal of the American Chemical Society·Durwin R StriplinThomas J Meyer
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Citations

Feb 3, 2018·Angewandte Chemie·Witold M BlochGuido H Clever
Jun 25, 2021·Chemical Science·Sonja PullenGuido H Clever
Mar 14, 2019·The Journal of Physical Chemistry. a·Magnus W D Hanson-Heine

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