Spin-Orbit State-Selective C-I Dissociation Dynamics of the CH3I+ X̃ Electronic State Induced by Intense Few-Cycle Laser Fields
Studies of ultrafast molecular dynamics induced by intense laser fields can reveal new approaches to manipulating chemical reactions in the strong-field regime. Here, we show that intense few-cycle laser pulses can induce the spin-orbit state-selective C-I dissociation of the iodomethane cation (CH3...
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| Vydáno v: | The journal of physical chemistry letters Ročník 8; číslo 24; s. 6067 |
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| Hlavní autoři: | , , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
| Vydáno: |
21.12.2017
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| ISSN: | 1948-7185, 1948-7185 |
| On-line přístup: | Zjistit podrobnosti o přístupu |
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| Shrnutí: | Studies of ultrafast molecular dynamics induced by intense laser fields can reveal new approaches to manipulating chemical reactions in the strong-field regime. Here, we show that intense few-cycle laser pulses can induce the spin-orbit state-selective C-I dissociation of the iodomethane cation (CH3I+) in the X̃ electronic state. Irradiation of CH3I by 6 fs laser pulses with peak intensities of 1.9 × 1014 W/cm2 followed by femtosecond extreme ultraviolet probing of the iodine 4d core-level transitions reveals dissociation of the CH3I+ X̃ 2E1/2 state with a time constant of 0.76 ± 0.16 ps. By contrast, the X̃ 2E3/2 spin-orbit ground state does not exhibit any appreciable dissociation on the picosecond time scale. The observed spin-orbit state-selective dissociation of the X̃ state is rationalized in terms of the laser-induced coupling to the à state. Our results suggest that the intense-laser control of photodissociation channels can be potentially extended to spin-orbit split states.Studies of ultrafast molecular dynamics induced by intense laser fields can reveal new approaches to manipulating chemical reactions in the strong-field regime. Here, we show that intense few-cycle laser pulses can induce the spin-orbit state-selective C-I dissociation of the iodomethane cation (CH3I+) in the X̃ electronic state. Irradiation of CH3I by 6 fs laser pulses with peak intensities of 1.9 × 1014 W/cm2 followed by femtosecond extreme ultraviolet probing of the iodine 4d core-level transitions reveals dissociation of the CH3I+ X̃ 2E1/2 state with a time constant of 0.76 ± 0.16 ps. By contrast, the X̃ 2E3/2 spin-orbit ground state does not exhibit any appreciable dissociation on the picosecond time scale. The observed spin-orbit state-selective dissociation of the X̃ state is rationalized in terms of the laser-induced coupling to the à state. Our results suggest that the intense-laser control of photodissociation channels can be potentially extended to spin-orbit split states. |
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| Bibliografie: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 1948-7185 1948-7185 |
| DOI: | 10.1021/acs.jpclett.7b03022 |