Controlling the strong field fragmentation of ClCHO+ using two laser pulses -an ab initio molecular dynamics simulation
© 2018 Wiley Periodicals, Inc.
| Veröffentlicht in: | Journal of computational chemistry. - 1984. - 40(2019), 1 vom: 05. Jan., Seite 200-205 |
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| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2019
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| Zugriff auf das übergeordnete Werk: | Journal of computational chemistry |
| Schlagworte: | Journal Article Born-Oppenheimer molecular dynamics Strong field chemistry aligned molecules mode selective chemistry wavelet analysis |
| Zusammenfassung: | © 2018 Wiley Periodicals, Inc. For a single, intense 7 μm linearly polarized laser pulse, we found that the branching ratio for the fragmentation of ClCHO+ → Cl + HCO+ , H + ClCO+ , HCl+ +CO depended strongly on the orientation of the molecule (J. Phys. Chem. Lett. 2012, 3 2541). The present study explores the possibility of controlling the branching ratio for fragmentation by using two independent pulses with different frequencies, alignment and delay. Born-Oppenheimer molecular dynamics simulations in the laser field were carried out with the B3LYP/6-311G(d,p) level of theory using combinations of 3.5, 7 and 10.5 μm sine squared pulses with field strengths of 0.03 au (peak intensity of 3.15×1013 W/cm2 ) and lengths of 560 fs. A 3.5 μm pulse aligned with the C-H bond and a 10.5 μm pulse perpendicular to the C-H bond produced a larger branching ratio for HCl+ +CO than a comparable single 7 μm pulse. When the 10.5 μm pulse was delayed by one quarter of the pulse envelope, the branching ratio for the high energy product, (HCl+ +CO 73%) was a factor of three larger than the low energy product (Cl + HCO+ , 25%). By contrast, when the 3.5 μm pulse was delayed by one quarter of the pulse envelope, the branching ratio was reversed (HCl+ +CO 38%; Cl + HCO+ , 60%). Continuous wavelet analysis was used to follow the interaction of the laser with the various vibrational modes as a function of time. © 2018 Wiley Periodicals, Inc |
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| Beschreibung: | Date Revised 20.11.2019 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1096-987X |
| DOI: | 10.1002/jcc.25576 |