Cyclic Tetramers of Zinc Chlorophylls as a Coupled Light-Harvesting Antenna-Charge-Separation System

Yoshinao Shinozaki, Kei Ohkubo, Shunichi Fukuzumi, Kosuke Sugawa, Joe Otsuki

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

A coupled light-harvesting antenna-charge-separation system, consisting of self-assembled zinc chlorophyll derivatives that incorporate an electron-accepting unit, is reported. The cyclic tetramers that incorporated an electron acceptor were constructed by the co-assembly of a pyridine-appended zinc chlorophyll derivative, ZnPy, and a zinc chlorophyll derivative further decorated with a fullerene unit, ZnPyC60. Comprehensive steady-state and time-resolved spectroscopic studies were conducted for the individual tetramers of ZnPy and ZnPyC60 as well as their co-tetramers. Intra-assembly singlet energy transfer was confirmed by singlet-singlet annihilation in the ZnPy tetramer. Electron transfer from the singlet chlorin unit to the fullerene unit was clearly demonstrated by the transient absorption of the fullerene radical anion in the ZnPyC60 tetramer. Finally, with the co-tetramer, a coupled light-harvesting and charge-separation system with practically 100 % quantum efficiency was demonstrated.

Original languageEnglish
Pages (from-to)1165-1176
Number of pages12
JournalChemistry - A European Journal
Volume22
Issue number3
DOIs
StatePublished - 18 Jan 2016

Bibliographical note

Publisher Copyright:
© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords

  • chlorophylls
  • electron transfer
  • energy transfer
  • fullerenes
  • self-assembly

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