Sub-100-fs energy transfer in coenzyme NADH is a coherent process assisted by a charge-transfer state

Vishal Kumar Jaiswal, Daniel Aranda Ruiz, Vasilis Petropoulos, Piotr Kabaciński, Francesco Montorsi, Lorenzo Uboldi, Simone Ugolini, Shaul Mukamel, Giulio Cerullo (), Marco Garavelli (), Fabrizio Santoro and Artur Nenov ()
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Vishal Kumar Jaiswal: Università di Bologna
Daniel Aranda Ruiz: Universidad de Valencia
Vasilis Petropoulos: Politecnico di Milano
Piotr Kabaciński: Politecnico di Milano
Francesco Montorsi: Università di Bologna
Lorenzo Uboldi: Politecnico di Milano
Simone Ugolini: Università di Bologna
Shaul Mukamel: University of California
Giulio Cerullo: Politecnico di Milano
Marco Garavelli: Università di Bologna
Fabrizio Santoro: Area della Ricerca del CNR
Artur Nenov: Università di Bologna

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Excitation energy transfer (EET) is a key photoinduced process in biological chromophoric assemblies. Here we investigate the factors which can drive EET into efficient ultrafast sub-ps regimes. We demonstrate how a coherent transport of electronic population could facilitate this in water solvated NADH coenzyme and uncover the role of an intermediate dark charge-transfer state. High temporal resolution ultrafast optical spectroscopy gives a 54±11 fs time constant for the EET process. Nonadiabatic quantum dynamical simulations computed through the time-evolution of multidimensional wavepackets suggest that the population transfer is mediated by photoexcited molecular vibrations due to strong coupling between the electronic states. The polar aqueous solvent environment leads to the active participation of a dark charge transfer state, accelerating the vibronically coherent EET process in favorably stacked conformers and solvent cavities. Our work demonstrates how the interplay of structural and environmental factors leads to diverse pathways for the EET process in flexible heterodimers and provides general insights relevant for coherent EET processes in stacked multichromophoric aggregates like DNA strands.

Date: 2024
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DOI: 10.1038/s41467-024-48871-4

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