Correlation-driven sub-3 fs charge migration in ionised adenine

(submitted), (2021)

Correlation-driven sub-3 fs charge migration in ionised adenine

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

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 change. Capturing this few-femtosecond/attosecond charge redistribution represents the real-time observation of the electron correlation in the molecule. So far, there has been no experimental evidence of this process. Here we report on a time-resolved study of the correlation-driven charge migration process occurring in the bio-relevant molecule adenine after ionisation by 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 the many-body excitation. This conclusion is supported by first-principles time-dependent simulations. Our findings opens new important perspectives for the control of the molecular reactivity at the electronic timescale.

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F.Ca. acknowledges support from the European Research Council under the ERC-2014-StG STARLIGHT (Grant Agreement No. 637756). F. Ca and A. R. acknowledge support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – SFB-925 – project 170620586 and the Cluster of Excellence Advanced Imaging of Matter (AIM). F.L. and V.W. acknowledge the Fonds de recherche du Qu´ebec – Nature et technologies (FRQNT) and the National Science and Engineering Research Council (NSERC). V.W. acknowledges support from the Vanier Canada Graduate Scholarship (Vanier CGS) program. S. L. acknowledges support from the Alexander von Humboldt foundation. A. R. acknowl- 17 edge financial support from the European Research Council(ERC-2015-AdG-694097). The Flatiron Institute is a division of the Simons Foundation. G.S. and E.P. acknowledge EC funding through the RISE Co-ExAN (Grant No. GA644076), the European Union project MaX Materials design at the eXascale H2020- EINFRA-2015-1, Grant Agreement No. 676598, Nanoscience Foundries and Fine Analysis-Europe H2020-INFRAIA-2014-2015, Grant Agreement No. 654360 and Tor Vergata University for financial support through the Mission Sustainability Project 2DUTOPI. J. B. G. acknowledge support from the EPSRC (UK) grant number EP/M001644/1.

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