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

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Authors

  • Erik P. Månsson
  • Simone Latini
  • Fabio Covito
  • Vincent Wanie
  • Andrea Trabattoni

External Research Organisations

  • Deutsches Elektronen-Synchrotron (DESY)
  • National Research Council Italy (CNR)
  • Max-Planck-Gesellschaft zur Förderung der Wissenschaften e.V. (MPG)
  • INRS Universite d'avant-garde
  • Politecnico di Milano
  • Tor Vergata University of Rome
  • Istituto Nazionale di Fisica Nucleare (INFN)
  • University of Palermo
  • Center for Free-Electron Laser Science (CFEL)
  • Queen's University Belfast
  • Flatiron Institute
  • Universität Hamburg
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Details

Original languageEnglish
Article number73
JournalCommunications Chemistry
Volume4
Issue number1
Early online date20 May 2021
Publication statusPublished - Dec 2021
Externally publishedYes

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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Cite this

Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine. / Månsson, Erik P.; Latini, Simone; Covito, Fabio et al.
In: Communications Chemistry, Vol. 4, No. 1, 73, 12.2021.

Research output: Contribution to journalArticleResearchpeer review

Månsson, EP, Latini, S, Covito, F, Wanie, V, Galli, M, Perfetto, E, Stefanucci, G, Hübener, H, De Giovannini, U, Castrovilli, MC, Trabattoni, A, Frassetto, F, Poletto, L, Greenwood, JB, Légaré, F, Nisoli, M, Rubio, A & Calegari, F 2021, 'Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine', Communications Chemistry, vol. 4, no. 1, 73. https://doi.org/10.1038/s42004-021-00510-5
Månsson, E. P., Latini, S., Covito, F., Wanie, V., Galli, M., Perfetto, E., Stefanucci, G., Hübener, H., De Giovannini, U., Castrovilli, M. C., Trabattoni, A., Frassetto, F., Poletto, L., Greenwood, J. B., Légaré, F., Nisoli, M., Rubio, A., & Calegari, F. (2021). Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine. Communications Chemistry, 4(1), Article 73. https://doi.org/10.1038/s42004-021-00510-5
Månsson EP, Latini S, Covito F, Wanie V, Galli M, Perfetto E et al. Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine. Communications Chemistry. 2021 Dec;4(1):73. Epub 2021 May 20. doi: 10.1038/s42004-021-00510-5
Månsson, Erik P. ; Latini, Simone ; Covito, Fabio et al. / Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine. In: Communications Chemistry. 2021 ; Vol. 4, No. 1.
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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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AU - Månsson, Erik P.

AU - Latini, Simone

AU - Covito, Fabio

AU - Wanie, Vincent

AU - Galli, Mara

AU - Perfetto, Enrico

AU - Stefanucci, Gianluca

AU - Hübener, Hannes

AU - De Giovannini, Umberto

AU - Castrovilli, Mattea C.

AU - Trabattoni, Andrea

AU - Frassetto, Fabio

AU - Poletto, Luca

AU - Greenwood, Jason B.

AU - Légaré, François

AU - Nisoli, Mauro

AU - Rubio, Angel

AU - Calegari, Francesca

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