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

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

doi:10.1038/s42004-021-00510-5

Journal Article

PUBDB-2021-01737

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

Månsson, E. P.DESY* ; Latini, S.CFEL*MPG* ; Covito, F.MPG* ; Wanie, V.CFEL*DESY* ; Galli, M.CFEL*Extern* ; Perfetto, E. ; Stefanucci, G. ; Huebener, H.CFEL*MPG* ; De Giovannini, U.CFEL*MPG* ; Castrovilli, M. C.Extern*XFEL.EU* ; Trabattoni, A.CFEL*DESY* ; Frassetto, F.Extern* ; Poletto, L.Extern* ; Greenwood, J. B. ; Légaré, F. ; Nisoli, M. ; Rubio, A.CFEL*MPG* ; Calegari, F. (Corresponding author)DESY*

2021
Macmillan Publishers Limited, part of Springer Nature [London]

Communications chemistry 4(1), 73 (2021) [10.1038/s42004-021-00510-5]

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Please use a persistent id in citations: doi:10.1038/s42004-021-00510-5 doi:10.3204/PUBDB-2021-01737

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.

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