Increasing the lifetimes of charge separated states in porphyrin–fullerene polyads

Literature Information

Publication Date 2017-07-31
DOI 10.1039/C7CP04193D
Impact Factor 3.676
Authors

Di Gao, Shawkat M. Aly, Paul-Ludovic Karsenti, Gessie Brisard, Pierre D. Harvey


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Abstract

Two linear polyads were designed using zinc(II)porphyrin, [ZnP], and N-methyl-2-phenyl-3,4-fullero-pyrrolidine (C60) where C60 is dangling either at the terminal position of [ZnP]–C6H4––C6H4–[ZnP]–C60 (1) or at the central position of [ZnP]–C6H4––C6H4–[ZnP(C60)]–C6H4––C6H4–[ZnP] (2) in order to test whether the fact of having one or two side electron donors influences the rate of electron transfer, ket. These polyads were studied using cyclic voltammograms, DFT computations, steady state and time-resolved fluorescence spectroscopy, and femtosecond transient absorption spectroscopy (fs-TAS). Photo-induced electron transfer confirmed by the detection of the charge separated state [ZnP˙+]/C60˙− from fs-TAS occurs with rates (ket) of 3–4 × 1010 s−1 whereas the charge recombinations (CRs) are found to produce the [ZnP] ground state via two pathways (central [ZnP˙+]/C60˙− (ps) and terminal central [ZnP˙+]/C60˙− (ns) producing [1ZnP] (ground state) and [3ZnP*]). The formation of the T1 species is more predominant for 2.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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