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

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.

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https://arxiv.org/abs/2101.05753 (Preprint)
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https://dx.doi.org/10.1038/s42004-021-00510-5 (Publisher version)
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 Creators:
Mansson, E. P.1, 2, Author
Latini, S.3, 4, Author              
Covito, F.3, 4, Author              
Wanie, V.1, 2, 5, Author
Galli, M.1, 6, Author
Perfetto, E.7, 8, Author
Stefanucci, G.8, 9, Author
Hübener, H.3, 4, Author              
de Giovannini, U.3, 4, 10, Author              
Castrovilli, M. C.2, 11, Author
Trabattoni, A.1, Author
Frassetto, F.12, Author
Poletto, L.12, Author
Greenwood, J. B.13, Author
Legare, F.5, Author
Nisoli, M.2, 6, Author
Rubio, A.3, 4, 14, Author              
Calegari, F.1, 2, 15, Author
Affiliations:
1Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, ou_persistent22              
2Institute for Photonics and Nanotechnologies CNR-IFN, Milano, ou_persistent22              
3Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
4Center for Free Electron Laser Science, Hamburg, ou_persistent22              
5INRS-EMT, Varennes, QC, Canada, ou_persistent22              
6Department of Physics, Politecnico di Milano, ou_persistent22              
7CNR-ISM, Division of Ultrafast Processes in Materials (FLASHit), ou_persistent22              
8Dipartimento di Fisica, Università di Roma Tor Vergata, ou_persistent22              
9INFN, Sezione di Roma Tor Vergata, ou_persistent22              
10Dipartimento di Fisica e Chimica, Università degli Studi di Palermo, ou_persistent22              
11Institute for the Structure of Matter CNR-ISM, Monterotondo Scalo, ou_persistent22              
12Institute for Photonics and Nanotechnologies CNR-IFN, Padova, ou_persistent22              
13Centre for Plasma Physics, School of Maths and Physics, Queen’s University Belfast, ou_persistent22              
14Center for Computational Quantum Physics (CCQ), The Flatiron Institute, ou_persistent22              
15Institut fur Experimentalphysik, Universität Hamburg, ou_persistent22              

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 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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Language(s): eng - English
 Dates: 2021-02-232021-04-192021-05-20
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2101.05753
DOI: 10.1038/s42004-021-00510-5
 Degree: -

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Project name : -
Grant ID : 676598
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : -
Grant ID : 654360
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Communications Chemistry
Source Genre: Journal
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Publ. Info: London : Springer Nature
Pages: - Volume / Issue: 4 Sequence Number: 73 Start / End Page: - Identifier: ISSN: 2399-3669
CoNE: https://pure.mpg.de/cone/journals/resource/2399-3669