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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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Open Access. - This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.
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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 (Verlagsversion)
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 Urheber:
Mansson, E. P.1, 2, Autor
Latini, S.3, 4, Autor           
Covito, F.3, 4, Autor           
Wanie, V.1, 2, 5, Autor
Galli, M.1, 6, Autor
Perfetto, E.7, 8, Autor
Stefanucci, G.8, 9, Autor
Hübener, H.3, 4, Autor           
de Giovannini, U.3, 4, 10, Autor           
Castrovilli, M. C.2, 11, Autor
Trabattoni, A.1, Autor
Frassetto, F.12, Autor
Poletto, L.12, Autor
Greenwood, J. B.13, Autor
Legare, F.5, Autor
Nisoli, M.2, 6, Autor
Rubio, A.3, 4, 14, Autor           
Calegari, F.1, 2, 15, Autor
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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 Zusammenfassung: 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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Sprache(n): eng - English
 Datum: 2021-02-232021-04-192021-05-20
 Publikationsstatus: Online veröffentlicht
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: arXiv: 2101.05753
DOI: 10.1038/s42004-021-00510-5
 Art des Abschluß: -

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Projektname : -
Grant ID : 676598
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)
Projektname : -
Grant ID : 654360
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)
Projektname : F. Calegari acknowledges support from the European Research Council under the ERC-2014-StG STARLIGHT (Grant Agreement No. 637756). F. Calegari and A.R. acknowledge support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)—SFB-925—project 170620586 and the CUI: Advanced Imaging of Matter' of the Deutsche Forschungsgemeinschaft (DFG) - EXC 2056 - project ID 390715994. F.L. and V.W. acknowledge the Fonds de recherche du Québec—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) programme. S.L. acknowledges support from the Alexander von Humboldt foundation. A.R. acknowledge 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. The authors would like to acknowledge A. Stolow for the fruitful discussion.
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Quelle 1

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Titel: Communications Chemistry
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: London : Springer Nature
Seiten: - Band / Heft: 4 Artikelnummer: 73 Start- / Endseite: - Identifikator: ISSN: 2399-3669
CoNE: https://pure.mpg.de/cone/journals/resource/2399-3669