Real-time observation of a correlation-driven sub 3 fs charge migration in 
ionised adenine

Mansson, E. P.; Latini, S.; Covito, F.; Wanie, V.; Galli, M.; Perfetto, E.; Stefanucci, G.; Hübener, H.; de Giovannini, U.; Castrovilli, M. C.; Trabattoni, A.; Frassetto, F.; Poletto, L.; Greenwood, J. B.; Legare, F.; Nisoli, M.; Rubio, A.; Calegari, F.

doi:10.1038/s42004-021-00510-5

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Journal Article

Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine

MPS-Authors

Latini, S.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science, Hamburg;

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Covito, F.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science, Hamburg;
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

Hübener, H.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science, Hamburg;

de Giovannini, U.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science, Hamburg;
Dipartimento di Fisica e Chimica, Università degli Studi di Palermo;

Rubio, A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free Electron Laser Science, Hamburg;
Center for Computational Quantum Physics (CCQ), The Flatiron Institute;

External Resource

https://arxiv.org/abs/2101.05753
(Preprint)

https://dx.doi.org/10.1038/s42004-021-00510-5
(Publisher version)

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s42004-021-00510-5.pdf
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Supplementary Material (public)

suppl.zip
(Supplementary material), 11MB

Citation

Mansson, E. P., Latini, S., Covito, F., Wanie, V., Galli, M., Perfetto, E., et al. (2021). Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine. Communications Chemistry, 4: 73. doi:10.1038/s42004-021-00510-5.

Cite as: https://hdl.handle.net/21.11116/0000-0008-968D-0

Abstract

Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly move along the molecular backbone. Capturing this few-femtosecond or attosecond charge redistribution would represent the real-time observation of electron correlation in a molecule with the enticing prospect of following the energy flow from a single excited electron to the other coupled electrons in the system. Here, we report a time-resolved study of the correlation-driven charge migration process occurring in the nucleic-acid base adenine after ionisation with a 15–35 eV attosecond pulse. We find that the production of intact doubly charged adenine – via a shortly-delayed laser-induced second ionisation event – represents the signature of a charge inflation mechanism resulting from many-body excitation. This conclusion is supported by first-principles time-dependent simulations. These findings may contribute to the control of molecular reactivity at the electronic, few-femtosecond time scale.