| Téléchargement | - Voir la version finale : Towards simultaneous imaging of ultrafast nuclear and electronic dynamics in small molecules (PDF, 5.0 Mio)
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| DOI | Trouver le DOI : https://doi.org/10.1038/s41598-025-93707-w |
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| Auteur | Rechercher : Mhatre, Saurabh; Rechercher : Dube, Zack1; Rechercher : Staudte, André2Identifiant ORCID : https://orcid.org/0000-0002-8284-3831; Rechercher : Gräfe, Stefanie; Rechercher : Kübel, MatthiasIdentifiant ORCID : https://orcid.org/0000-0001-6065-6122 |
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| Affiliation | - Conseil national de recherches Canada. Technologies de sécurité et de rupture
- Conseil national de recherches Canada. Quantique et nanotechnologies
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| Format | Texte, Article |
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| Résumé | When a chemical bond is broken, the molecular structure undergoes a transformation. An ideal experiment should probe the change in the electronic and nuclear structure simultaneously. Here, we present a method for the simultaneous time-resolved imaging of nuclear and electron dynamics by combining Coulomb explosion imaging with strong-field photoelectron momentum imaging. We study the dissociative photoionization of H₂ and N₂O using time-resolved photoion-photoelectron coincidence spectroscopy. The measured delay-dependent kinetic energy release clearly reveals the ultrafast nuclear dynamics. The transient changes in the electronic structure of the dissociating H⁺₂ molecular ion are studied by solving the three-dimensional Schrödinger equation in the fixed-nuclei approximation. A detailed comparison of the numerical results to those from a simple imaging model is conducted. The numerical results reflect the evolution in the electron density in the molecular ion as its bond is first stretched and then breaks apart. While these details remain unresolved in the H₂ experiment, we demonstrate the sensitivity of the photoelectron signal to the site of electron localization following bond cleavage for the case of N₂O. Our work shows opportunities and challenges on the track towards capturing simple gas-phase chemical dynamics in complete molecular movies. |
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| Date de publication | 2025-03-18 |
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| Maison d’édition | Nature |
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| Licence | |
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| Dans | |
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| Langue | anglais |
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| Publications évaluées par des pairs | Oui |
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| Exporter la notice | Exporter en format RIS |
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| Signaler une correction | Signaler une correction (s'ouvre dans un nouvel onglet) |
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| Identificateur de l’enregistrement | 956d1bc2-f652-438a-8fcf-17b8e15d4718 |
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| Enregistrement créé | 2025-05-08 |
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| Enregistrement modifié | 2025-05-08 |
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