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A High‐Energy Charge‐Separated State of 1.70 eV from a High‐Potential Donor–Acceptor Dyad: A Catalyst for Energy‐Demanding Photochemical Reactions
Author(s) -
Lim Gary N.,
Obondi Christopher O.,
D'Souza Francis
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201606112
Subject(s) - photochemistry , chemistry , porphyrin , intramolecular force , acceptor , ultrafast laser spectroscopy , covalent bond , catalysis , photoinduced charge separation , artificial photosynthesis , photocatalysis , stereochemistry , spectroscopy , organic chemistry , physics , quantum mechanics , condensed matter physics
A high potential donor–acceptor dyad composed of zinc porphyrin bearing three meso ‐pentafluorophenyl substituents covalently linked to C 60 , as a novel dyad capable of generating charge‐separated states of high energy (potential) has been developed. The calculated energy of the charge‐separated state was found to be 1.70 eV, the highest reported for a covalently linked porphyrin–fullerene dyad. Intramolecular photoinduced electron transfer leading to charge‐separated states of appreciable lifetimes in polar and nonpolar solvents has been established from studies involving femto‐ to nanosecond transient absorption techniques. The high energy stored in the form of charge‐separated states along with its persistence of about 50–60 ns makes this dyad a potential electron‐transporting catalyst to carry out energy‐demanding photochemical reactions. This type of high‐energy harvesting dyad is expected to open new research in the areas of artificial photosynthesis especially producing energy (potential) demanding light‐to‐fuel products.