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The carbonyl-lock mechanism underlying non-aromatic fluorescence in biological matter

Author

Listed:
  • Gonzalo Díaz Mirón

    (Universidad de Buenos Aires)

  • Jonathan A. Semelak

    (Universidad de Buenos Aires)

  • Luca Grisanti

    (Ruder Bošković Institute)

  • Alex Rodriguez

    (The Abdus Salam International Centre for Theoretical Physics)

  • Irene Conti

    (Università di Bologna)

  • Martina Stella

    (The Abdus Salam International Centre for Theoretical Physics)

  • Jayaramakrishnan Velusamy

    (University of Cambridge)

  • Nicola Seriani

    (The Abdus Salam International Centre for Theoretical Physics)

  • Nadja Došlić

    (Ruder Bošković Institute)

  • Ivan Rivalta

    (Università di Bologna
    CNRS)

  • Marco Garavelli

    (Università di Bologna)

  • Dario A. Estrin

    (Universidad de Buenos Aires)

  • Gabriele S. Kaminski Schierle

    (University of Cambridge)

  • Mariano C. González Lebrero

    (Universidad de Buenos Aires)

  • Ali Hassanali

    (The Abdus Salam International Centre for Theoretical Physics)

  • Uriel N. Morzan

    (The Abdus Salam International Centre for Theoretical Physics)

Abstract

Challenging the basis of our chemical intuition, recent experimental evidence reveals the presence of a new type of intrinsic fluorescence in biomolecules that exists even in the absence of aromatic or electronically conjugated chemical compounds. The origin of this phenomenon has remained elusive so far. In the present study, we identify a mechanism underlying this new type of fluorescence in different biological aggregates. By employing non-adiabatic ab initio molecular dynamics simulations combined with a data-driven approach, we characterize the typical ultrafast non-radiative relaxation pathways active in non-fluorescent peptides. We show that the key vibrational mode for the non-radiative decay towards the ground state is the carbonyl elongation. Non-aromatic fluorescence appears to emerge from blocking this mode with strong local interactions such as hydrogen bonds. While we cannot rule out the existence of alternative non-aromatic fluorescence mechanisms in other systems, we demonstrate that this carbonyl-lock mechanism for trapping the excited state leads to the fluorescence yield increase observed experimentally, and set the stage for design principles to realize novel non-invasive biocompatible probes with applications in bioimaging, sensing, and biophotonics.

Suggested Citation

  • Gonzalo Díaz Mirón & Jonathan A. Semelak & Luca Grisanti & Alex Rodriguez & Irene Conti & Martina Stella & Jayaramakrishnan Velusamy & Nicola Seriani & Nadja Došlić & Ivan Rivalta & Marco Garavelli & , 2023. "The carbonyl-lock mechanism underlying non-aromatic fluorescence in biological matter," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42874-3
    DOI: 10.1038/s41467-023-42874-3
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    References listed on IDEAS

    as
    1. Xin Ji & Weiguo Tian & Kunfeng Jin & Huailing Diao & Xin Huang & Guangjie Song & Jun Zhang, 2022. "Anionic polymerization of nonaromatic maleimide to achieve full-color nonconventional luminescence," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
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