Details
| Originalsprache | Englisch |
|---|---|
| Aufsatznummer | 73 |
| Fachzeitschrift | Communications Chemistry |
| Jahrgang | 4 |
| Ausgabenummer | 1 |
| Frühes Online-Datum | 20 Mai 2021 |
| Publikationsstatus | Veröffentlicht - Dez. 2021 |
| Extern publiziert | Ja |
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.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Allgemeine Chemie
- Umweltwissenschaften (insg.)
- Umweltchemie
- Biochemie, Genetik und Molekularbiologie (insg.)
- Biochemie
- Werkstoffwissenschaften (insg.)
- Werkstoffchemie
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in: Communications Chemistry, Jahrgang 4, Nr. 1, 73, 12.2021.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine
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
PY - 2021/12
Y1 - 2021/12
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85106238432&partnerID=8YFLogxK
U2 - 10.1038/s42004-021-00510-5
DO - 10.1038/s42004-021-00510-5
M3 - Article
AN - SCOPUS:85106238432
VL - 4
JO - Communications Chemistry
JF - Communications Chemistry
IS - 1
M1 - 73
ER -