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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
Communications chemistry, 05/2021, Letnik: 4, Številka: 1Journal Article
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.
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