Three-dimensional momentum imaging of dissociation in flight of metastable molecules

Jochim, Bethany; Erdwien, Reid; Malakar, Y.; Severt, T.; Berry, Ben; Feizollah, Peyman; Rajput, Jyoti; Kaderiya, B.; Pearson, W. L.; Carnes, K. D.; Rudenko, Artem; Ben‐Itzhak, I.

doi:10.1088/1367-2630/aa81ab

Cited by 14 publications

(6 citation statements)

References 59 publications

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“…Longer lifetimes would be detected as dissociation in flight (see, for example Ref. [115]). The lower limit set by the rotational period is ≈33 ps for the J=1 state for each of the X 3 Σ − g , 1 ∆ g and 1 Σ + g electronic states of CO 2+ 2 , which we estimated using the spectroscopic constants reported in Ref.…”

Section: Resultsmentioning

confidence: 99%

Strong-field-induced bond rearrangement in triatomic molecules

et al. 2019

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A comparative study of bond rearrangement is reported for the double ionization of three triatomic molecules: carbon dioxide, carbonyl sulfide, and water (D2O). Specifically we study the formation of the molecular cation AC + from the edge atoms of a triatomic molecular dication ABC 2+ following double ionization by intense, short (23 fs, 790 nm) laser pulses. The comparison is made using the double ionization branching ratio of each molecule, thereby minimizing differences due to differing ionization rates. The rearrangement branching ratio is highest for water, which has a bent initial geometry, while CO2 and OCS are linear molecules. The angular distribution of O + 2 fragments arising from CO2 is essentially isotropic, while SO + from OCS and D + 2 from D2O are aligned with the laser polarization. In the CO2 and D2O cases, the angular distributions of the bond rearrangement channels are different from the angular distributions of the dominant dissociative double ionization channels CO + + O + and OD + + D + . Only the angular distribution of SO + from OCS is both aligned with the laser polarization and similar to the angular distribution of the largest dissociative channel, CO + + S + . The mixed behavior observed from the angular distributions of the different molecules stands in contrast to the relative consistency of the magnitude of the bond rearrangement branching ratio.I.

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Section: Resultsmentioning

confidence: 99%

Strong-field-induced bond rearrangement in triatomic molecules

et al. 2019

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“…The lifetimes of these states are also crucial to the interpretation of the data, as they must lie between the rotational period and a few-nanosecond maximum imposed by the imaging setup [40]. The relevant rotation period depends on the angular momentum imparted to the CO 2+ in the first breakup step.…”

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Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation

et al. 2018

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A key question concerning the three-body fragmentation of polyatomic molecules is the distinction of sequential and concerted mechanisms, i.e., the stepwise or simultaneous cleavage of bonds. Using laser-driven fragmentation of OCS into O^{+}+C^{+}+S^{+} and employing coincidence momentum imaging, we demonstrate a novel method that enables the clear separation of sequential and concerted breakup. The separation is accomplished by analyzing the three-body fragmentation in the native frame associated with each step and taking advantage of the rotation of the intermediate molecular fragment, CO^{2+} or CS^{2+}, before its unimolecular dissociation. This native-frame method works for any projectile (electrons, ions, or photons), provides details on each step of the sequential breakup, and enables the retrieval of the relevant spectra for sequential and concerted breakup separately. Specifically, this allows the determination of the branching ratio of all these processes in OCS^{3+} breakup. Moreover, we find that the first step of sequential breakup is tightly aligned along the laser polarization and identify the likely electronic states of the intermediate dication that undergo unimolecular dissociation in the second step. Finally, the separated concerted breakup spectra show clearly that the central carbon atom is preferentially ejected perpendicular to the laser field.

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“…In addition, regarding dissociation due to the decay of populated A 2 state vibrational resonances, one must account for the influence of tunneling lifetimes. Specifically, do the dissociating vibrational resonances decay completely and does dissociation in flight [88] affect our observation? These questions must be examined for each particular target molecule and set of experimental conditions.…”

Section: Perturbation Theorymentioning

confidence: 97%

Importance of one- and two-photon transitions in the strong-field dissociation of NO2+

et al. 2021

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Employing a coincidence three-dimensional momentum imaging technique, we investigate the ultrafast, intense laser-induced dissociation of a metastable NO 2+ ion beam into N + + O + . Based on the kinetic energy release and angular distributions, measured using both 774-nm and second-order-harmonic 387-nm pulses, we show that the main processes driving dissociation in pulses of about 10 14 W/cm 2 peak intensity are one-and two-photon transitions from the X 2 + ground state to the A 2 first-excited state. First-order perturbation theory calculations also corroborate these findings.

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Three-dimensional momentum imaging of dissociation in flight of metastable molecules

Cited by 14 publications

References 59 publications

Strong-field-induced bond rearrangement in triatomic molecules

Strong-field-induced bond rearrangement in triatomic molecules

Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation

Importance of one- and two-photon transitions in the strong-field dissociation of NO2+

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