Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields
Dissociative ionization of tetrafluoromethane (CF4) in linearly polarized ω-2ω ultrashort intense laser fields (1.4 × 1014 W/cm2, 800 and 400 nm) has been investigated by three-dimensional momentum ion imaging. The spatial distribution of CF3+ produced by CF4 → CF3+ + F + e− exhibited a clear asymme...
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Frontiers Media S.A.
2022-04-01
|
| Series: | Frontiers in Chemistry |
| Subjects: | |
| Online Access: | https://www.frontiersin.org/articles/10.3389/fchem.2022.857863/full |
| _version_ | 1818490344647426048 |
|---|---|
| author | Hiroka Hasegawa Tiffany Walmsley Tiffany Walmsley Akitaka Matsuda Toru Morishita Lars Bojer Madsen Frank Jensen Oleg I. Tolstikhin Akiyoshi Hishikawa Akiyoshi Hishikawa |
| author_facet | Hiroka Hasegawa Tiffany Walmsley Tiffany Walmsley Akitaka Matsuda Toru Morishita Lars Bojer Madsen Frank Jensen Oleg I. Tolstikhin Akiyoshi Hishikawa Akiyoshi Hishikawa |
| author_sort | Hiroka Hasegawa |
| collection | DOAJ |
| description | Dissociative ionization of tetrafluoromethane (CF4) in linearly polarized ω-2ω ultrashort intense laser fields (1.4 × 1014 W/cm2, 800 and 400 nm) has been investigated by three-dimensional momentum ion imaging. The spatial distribution of CF3+ produced by CF4 → CF3+ + F + e− exhibited a clear asymmetry with respect to the laser polarization direction. The degree of the asymmetry varies by the relative phase of the ω and 2ω laser fields, showing that 1) the breaking of the four equivalent C-F bonds can be manipulated by the laser pulse shape and 2) the C-F bond directed along the larger amplitude side of the ω-2ω electric fields tends to be broken. Weak-field asymptotic theory (WFAT) shows that the tunneling ionization from the 4t2 second highest-occupied molecular orbital (HOMO-1) surpasses that from the 1t1 HOMO. This predicts the enhancement of the tunneling ionization with electric fields pointing from F to C, in the direction opposite to that observed for the asymmetric fragment ejection. Possible mechanisms involved in the asymmetric dissociative ionization, such as post-ionization interactions, are discussed. |
| first_indexed | 2024-12-10T17:15:37Z |
| format | Article |
| id | doaj.art-7cb619c50fe64e288a8a89be91c9a3ee |
| institution | Directory Open Access Journal |
| issn | 2296-2646 |
| language | English |
| last_indexed | 2024-12-10T17:15:37Z |
| publishDate | 2022-04-01 |
| publisher | Frontiers Media S.A. |
| record_format | Article |
| series | Frontiers in Chemistry |
| spelling | doaj.art-7cb619c50fe64e288a8a89be91c9a3ee2022-12-22T01:40:08ZengFrontiers Media S.A.Frontiers in Chemistry2296-26462022-04-011010.3389/fchem.2022.857863857863Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser FieldsHiroka Hasegawa0Tiffany Walmsley1Tiffany Walmsley2Akitaka Matsuda3Toru Morishita4Lars Bojer Madsen5Frank Jensen6Oleg I. Tolstikhin7Akiyoshi Hishikawa8Akiyoshi Hishikawa9Graduate School of Science, Nagoya University, Nagoya, JapanGraduate School of Science, Nagoya University, Nagoya, JapanSchool of Chemistry, University of Edinburgh, Edinburgh, United KingdomGraduate School of Science, Nagoya University, Nagoya, JapanInstitute for Advanced Science, The University of Electro-Communications, Chofu-shi, Tokyo, JapanDepartment of Physics and Astronomy, Aarhus University, Aarhus, DenmarkDepartment of Chemistry, Aarhus University, Aarhus, DenmarkMoscow Institute of Physics and Technology, Dolgoprudny, RussiaGraduate School of Science, Nagoya University, Nagoya, JapanResearch Center for Materials Science, Nagoya University, Nagoya, JapanDissociative ionization of tetrafluoromethane (CF4) in linearly polarized ω-2ω ultrashort intense laser fields (1.4 × 1014 W/cm2, 800 and 400 nm) has been investigated by three-dimensional momentum ion imaging. The spatial distribution of CF3+ produced by CF4 → CF3+ + F + e− exhibited a clear asymmetry with respect to the laser polarization direction. The degree of the asymmetry varies by the relative phase of the ω and 2ω laser fields, showing that 1) the breaking of the four equivalent C-F bonds can be manipulated by the laser pulse shape and 2) the C-F bond directed along the larger amplitude side of the ω-2ω electric fields tends to be broken. Weak-field asymptotic theory (WFAT) shows that the tunneling ionization from the 4t2 second highest-occupied molecular orbital (HOMO-1) surpasses that from the 1t1 HOMO. This predicts the enhancement of the tunneling ionization with electric fields pointing from F to C, in the direction opposite to that observed for the asymmetric fragment ejection. Possible mechanisms involved in the asymmetric dissociative ionization, such as post-ionization interactions, are discussed.https://www.frontiersin.org/articles/10.3389/fchem.2022.857863/fullcoherent controlintense laser fieldstunneling ionizationmolecular dissociationtetrafluoromethane |
| spellingShingle | Hiroka Hasegawa Tiffany Walmsley Tiffany Walmsley Akitaka Matsuda Toru Morishita Lars Bojer Madsen Frank Jensen Oleg I. Tolstikhin Akiyoshi Hishikawa Akiyoshi Hishikawa Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields Frontiers in Chemistry coherent control intense laser fields tunneling ionization molecular dissociation tetrafluoromethane |
| title | Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields |
| title_full | Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields |
| title_fullStr | Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields |
| title_full_unstemmed | Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields |
| title_short | Asymmetric Dissociative Tunneling Ionization of Tetrafluoromethane in ω − 2ω Intense Laser Fields |
| title_sort | asymmetric dissociative tunneling ionization of tetrafluoromethane in ω 2ω intense laser fields |
| topic | coherent control intense laser fields tunneling ionization molecular dissociation tetrafluoromethane |
| url | https://www.frontiersin.org/articles/10.3389/fchem.2022.857863/full |
| work_keys_str_mv | AT hirokahasegawa asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT tiffanywalmsley asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT tiffanywalmsley asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT akitakamatsuda asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT torumorishita asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT larsbojermadsen asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT frankjensen asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT olegitolstikhin asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT akiyoshihishikawa asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields AT akiyoshihishikawa asymmetricdissociativetunnelingionizationoftetrafluoromethaneinō2ōintenselaserfields |