Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion
Abstract Coulomb explosion is an established momentum imaging technique, where the molecules are ionized multiple times on a femtosecond time scale before breaking up into ionized fragments. By measuring the momentum of all the ions, information about the initial molecular structure is theoretically...
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| Format: | Article |
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Nature Portfolio
2024-12-01
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| Series: | Communications Physics |
| Online Access: | https://doi.org/10.1038/s42005-024-01863-8 |
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| author | Aydin Ashrafi-Belgabad Reza Karimi Mohammad Monfared Kaili Tian Parviz Parvin Benji Wales Éric Bisson Samuel Beaulieu Mathieu Giguère Jean-Claude Kieffer Philippe Lassonde François Légaré Heide Ibrahim Joseph H. Sanderson |
| author_facet | Aydin Ashrafi-Belgabad Reza Karimi Mohammad Monfared Kaili Tian Parviz Parvin Benji Wales Éric Bisson Samuel Beaulieu Mathieu Giguère Jean-Claude Kieffer Philippe Lassonde François Légaré Heide Ibrahim Joseph H. Sanderson |
| author_sort | Aydin Ashrafi-Belgabad |
| collection | DOAJ |
| description | Abstract Coulomb explosion is an established momentum imaging technique, where the molecules are ionized multiple times on a femtosecond time scale before breaking up into ionized fragments. By measuring the momentum of all the ions, information about the initial molecular structure is theoretically available. However, significant geometric changes due to multiple ionizations occur before the explosion, posing a challenge in retrieving the ground-state structure of molecules from the measured momentum values of the fragments. In this work, we investigate theoretically and experimentally such a connection between the ground-state geometry of a polyatomic molecule (OCS) and the detected momenta of ionic fragments from the Coulomb explosion. By relying on time-dependent density functional theory (TDDFT), we can rigorously model the ionization dynamics of the molecule in the tunneling regime. We reproduce the energy release and the Newton plot momentum patterns of an experiment in which OCS is ionized to the 6+ charge state. Our results provide insight into the behavior of molecules during strong field multiple ionization, opening a way toward precision imaging of real-space molecular geometries using tabletop lasers. |
| format | Article |
| id | doaj-art-540145da84da4e3c8440459882b788f8 |
| institution | OA Journals |
| issn | 2399-3650 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Physics |
| spelling | doaj-art-540145da84da4e3c8440459882b788f82025-08-20T02:32:26ZengNature PortfolioCommunications Physics2399-36502024-12-01711910.1038/s42005-024-01863-8Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosionAydin Ashrafi-Belgabad0Reza Karimi1Mohammad Monfared2Kaili Tian3Parviz Parvin4Benji Wales5Éric Bisson6Samuel Beaulieu7Mathieu Giguère8Jean-Claude Kieffer9Philippe Lassonde10François Légaré11Heide Ibrahim12Joseph H. Sanderson13Department of Energy Engineering and Physics, Amirkabir University of Technology (Tehran Polytechnic)Department of Energy Engineering and Physics, Amirkabir University of Technology (Tehran Polytechnic)Institute of Condensed Matter Theory and Optics, Friedrich-Schiller-University JenaDepartment of Physics and Astronomy, University of WaterlooDepartment of Energy Engineering and Physics, Amirkabir University of Technology (Tehran Polytechnic)Department of Physics and Astronomy, University of WaterlooAdvanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Université de Bordeaux—CNRS—CEA, CELIA, UMR5107Advanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Advanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Advanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Advanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Advanced Laser Light Source (ALLS), The Institut National de la Recherche Scientifique (INRS-EMT)Department of Physics and Astronomy, University of WaterlooAbstract Coulomb explosion is an established momentum imaging technique, where the molecules are ionized multiple times on a femtosecond time scale before breaking up into ionized fragments. By measuring the momentum of all the ions, information about the initial molecular structure is theoretically available. However, significant geometric changes due to multiple ionizations occur before the explosion, posing a challenge in retrieving the ground-state structure of molecules from the measured momentum values of the fragments. In this work, we investigate theoretically and experimentally such a connection between the ground-state geometry of a polyatomic molecule (OCS) and the detected momenta of ionic fragments from the Coulomb explosion. By relying on time-dependent density functional theory (TDDFT), we can rigorously model the ionization dynamics of the molecule in the tunneling regime. We reproduce the energy release and the Newton plot momentum patterns of an experiment in which OCS is ionized to the 6+ charge state. Our results provide insight into the behavior of molecules during strong field multiple ionization, opening a way toward precision imaging of real-space molecular geometries using tabletop lasers.https://doi.org/10.1038/s42005-024-01863-8 |
| spellingShingle | Aydin Ashrafi-Belgabad Reza Karimi Mohammad Monfared Kaili Tian Parviz Parvin Benji Wales Éric Bisson Samuel Beaulieu Mathieu Giguère Jean-Claude Kieffer Philippe Lassonde François Légaré Heide Ibrahim Joseph H. Sanderson Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion Communications Physics |
| title | Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion |
| title_full | Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion |
| title_fullStr | Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion |
| title_full_unstemmed | Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion |
| title_short | Reconstructing real-space geometries of polyatomic molecules undergoing strong field laser-induced Coulomb explosion |
| title_sort | reconstructing real space geometries of polyatomic molecules undergoing strong field laser induced coulomb explosion |
| url | https://doi.org/10.1038/s42005-024-01863-8 |
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