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Journal Article

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

MPS-Authors
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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;

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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;

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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;

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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
Fulltext (public)

s42004-021-00510-5.pdf
(Publisher version), 2MB

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: http://hdl.handle.net/21.11116/0000-0008-6EC3-1
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.