Tetrahedron
Tetrahedron
5 years ago

Photoinitiated long-lived charge separation with near-unity quantum yield in donor-acceptor1-acceptor2 systems for artificial photosynthesis

Photoinitiated long-lived charge separation with near-unity quantum yield in donor-acceptor1-acceptor2 systems for artificial photosynthesis
We report the synthesis and photophysical characterization of isomeric donor-acceptor1-acceptor2 (D-A 1 -A 2 ) triads each comprising a perylene donor (D) connected by a xylene bridge to a naphthalene-1,8-dicarboximide primary acceptor (NMI, A 1 ) that is, in turn, covalently linked to a naphthalene-1,4:5,8-bis(dicarboximide) secondary acceptor (NDI, A 2 ) through a benzene ring at its ortho, meta or para positions (Per-Xy-NMI-x-NDI). Selective photoexcitation of Per produces both Per +• and NDI ‒• simultaneously with time constants of ∼50 ps in benzonitrile and ∼80 ps in toluene with a >98% yield. This is much faster than expected for single-step electron transfer from 1* Per to NDI and is consistent with a two-step mechanism, 1* Per-Xy-NMI-x-NDI → Per +• -Xy-NMI ‒• -x-NDI → Per +• -Xy-NMI-x-NDI ‒• , in which the second step is much faster than the first step. In addition, preserving long-lived charge separation in these systems is found to depend on inhibiting charge recombination by a triplet radical ion pair recombination pathway.

Publisher URL: www.sciencedirect.com/science

DOI: S0040402017306403

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