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Picosecond reactions of excited radical ion super-reductants

Author

Listed:
  • Björn Pfund

    (University of Basel)

  • Deyanira Gejsnæs-Schaad

    (University of Basel)

  • Bruno Lazarevski

    (University of Basel)

  • Oliver S. Wenger

    (University of Basel)

Abstract

Classical photochemistry requires nanosecond excited-state lifetimes for diffusion-controlled reactions. Excited radicals with picosecond lifetimes have been implied by numerous photoredox studies, and controversy has arisen as to whether they can actually be catalytically active. We provide direct evidence for the elusive pre-association between radical ions and substrate molecules, enabling photoinduced electron transfer beyond the diffusion limit. A strategy based on two distinct light absorbers, mimicking the natural photosystems I and II, is used to generate excited radicals, unleashing extreme reduction power and activating C(sp2)―Cl and C(sp2)―F bonds. Our findings provide a long-sought mechanistic understanding for many previous synthetically-oriented works and permit more rational future photoredox reaction development. The newly developed excitation strategy pushes the current limits of reactions based on multi-photon excitation and very short-lived but highly redox active species.

Suggested Citation

  • Björn Pfund & Deyanira Gejsnæs-Schaad & Bruno Lazarevski & Oliver S. Wenger, 2024. "Picosecond reactions of excited radical ion super-reductants," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49006-5
    DOI: 10.1038/s41467-024-49006-5
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    References listed on IDEAS

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    1. Ian A. MacKenzie & Leifeng Wang & Nicholas P. R. Onuska & Olivia F. Williams & Khadiza Begam & Andrew M. Moran & Barry D. Dunietz & David A. Nicewicz, 2020. "Discovery and characterization of an acridine radical photoreductant," Nature, Nature, vol. 580(7801), pages 76-80, April.
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