Electron and energy transfer in a porphyrin–oxoporphyrinogen–fullerene triad, ZnP–OxP–C60
| Autor: | Francis D'Souza, Jonathan P. Hill, Whitney A. Webre, Katsuhiko Ariga, Paul A. Karr, Mandeep K. Chahal, Daniel T. Payne, Habtom B. Gobeze |
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| Rok vydání: | 2020 |
| Předmět: |
Fullerene
010405 organic chemistry Chemistry General Physics and Astronomy Triad (anatomy) Electron donor Electron 010402 general chemistry Photochemistry 7. Clean energy 01 natural sciences Porphyrin 0104 chemical sciences Electron transfer chemistry.chemical_compound medicine.anatomical_structure Intramolecular force Ultrafast laser spectroscopy medicine Physical and Theoretical Chemistry |
| Zdroj: | Physical Chemistry Chemical Physics. 22:14356-14363 |
| ISSN: | 1463-9084 1463-9076 |
| DOI: | 10.1039/d0cp02696d |
| Popis: | A multichromophoric triad, ZnP–OxP–C60 containing porphyrin (ZnTPP hereafter ZnP), oxoporphyrinogen (OxP) and fullerene (C60) has been synthesized to probe the intramolecular dynamics of its electron and energy transfer in relation to the presence of the closely linked electron deficient OxP–C60 ‘special pair’, constructed as a mimic of the naturally occurring photosynthetic antenna-reaction center. The DFT optimized structure of the triad reveals the relative spatial remoteness of the ZnP entity with proximal OxP/C60 entities. Free-energetics of different energy and electron transfer events were estimated using spectral, computational and electrochemical studies, according to the Rehm–Weller approach. Femtosecond transient absorption spectral studies revealed energy transfer from 1ZnP* to OxP to yield ZnP–1OxP*–C60, and electron transfer to yield ZnP˙+–OxP–C60˙− and/or ZnP–OxP˙+–C60˙− charge seperated states. That is, the ZnP entity in the triad operates as both antenna and electron donor to generate relatively long-lived charge separated states thus mimicking the early photoevents of natural photosynthesis. |
| Databáze: | OpenAIRE |
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