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

Gonzalo Díaz Mirón, Jonathan A. Semelak, Luca Grisanti, Alex Rodriguez, Irene Conti, Martina Stella, Jayaramakrishnan Velusamy, Nicola Seriani, Nadja Došlić, Ivan Rivalta, Marco Garavelli, Dario A. Estrin, Gabriele S. Kaminski Schierle, Mariano C. González Lebrero, Ali Hassanali () and Uriel N. Morzan ()
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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
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

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-42874-3

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