Synergy of Electrostatic and π–π Interactions in the Realization of Nanoscale Artificial Photosynthetic Model Systems

Eduardo Anaya-Plaza, Jan Joseph, Stefan Bauroth, Maximilian Wagner, Christian Dolle, Michael Sekita, Franziska Gröhn, Erdmann Spiecker, Timothy Clark, Andrés de la Escosura*, Dirk M. Guldi, Tomás Torres

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

1 Citation (Scopus)

Abstract

In the scientific race to build up photoactive electron donor-acceptor systems with increasing efficiencies, little is known about the interplay of their building blocks when integrated into supramolecular nanoscale arrays, particularly in aqueous environments. Here, we describe an aqueous donor-acceptor ensemble whose emergence as a nanoscale material renders it remarkably stable and efficient. We have focused on a tetracationic zinc phthalocyanine (ZnPc) featuring pyrenes, which shows an unprecedented mode of aggregation, driven by subtle cooperation between electrostatic and π–π interactions. Our studies demonstrate monocrystalline growth in solution and a symmetry-breaking intermolecular charge transfer between adjacent ZnPcs upon photoexcitation. Immobilizing a negatively charged fullerene (C60) as electron acceptor onto the monocrystalline ZnPc assemblies was found to enhance the overall stability, and to suppress the energy-wasting charge recombination found in the absence of C60. Overall, the resulting artificial photosynthetic model system exhibits a high degree of preorganization, which facilitates efficient charge separation and subsequent charge transport.

Original languageEnglish
Number of pages10
JournalAngewandte Chemie - International Edition
DOIs
Publication statusE-pub ahead of print - 11 Jul 2020
MoE publication typeA1 Journal article-refereed

Keywords

  • artificial photosynthesis
  • fullerenes
  • nanoscale self-assembly
  • phthalocyanines

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