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

Medientyp: E-Artikel

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

Beteiligte: Månsson, Erik P.; Latini, Simone; Covito, Fabio; Wanie, Vincent; Galli, Mara; Perfetto, Enrico; Stefanucci, Gianluca; Hübener, Hannes; De Giovannini, Umberto; Castrovilli, Mattea C.; Trabattoni, Andrea; Frassetto, Fabio; Poletto, Luca; Greenwood, Jason B.; Légaré, François; Nisoli, Mauro; Rubio, Angel; Calegari, Francesca

Erschienen: Springer Science and Business Media LLC, 2021

Sprache: Englisch

DOI: 10.1038/s42004-021-00510-5

ISSN: 2399-3669

Schlagwörter: Materials Chemistry ; Biochemistry ; Environmental Chemistry ; General Chemistry

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Beschreibung: AbstractSudden 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.

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