Study of Unimolecular Reactions by Coulomb Explosion Imaging: The Nondecaying Vinylidene

Levin, J. J.; Feldman, H.; Baer, A.; Ben-Hamu, D.; Heber, O.; Zajfman, D.; Vager, Z.

doi:10.1103/physrevlett.81.3347

Cited by 98 publications

(89 citation statements)

References 15 publications

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“…Once the laser strips electrons from the molecule, the remaining positively charged structure can explode, creating a molecular plasma cloud. Coulomb explosion can be used to generate bright keV x-ray photons [14,15], highly energetic electrons [16], and for imaging [17][18][19].The strong-field ionization and fragmentation of hydrocarbon molecules is a prototypical example of the Coulomb explosion of polyatomic molecules, and it has been the subject of several experiments [9,11,[20][21][22][23]]. An important quantity measured in these experiments is the kinetic energy distribution of the protons ejected during the fragmentation.…”

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Strong laser-pulse-driven ionization and Coulomb explosion of hydrocarbon molecules

et al. 2012

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Field ionization and Coulomb explosion of small hydrocarbon molecules driven by intense laser pulses are studied in a combined theoretical and experimental framework. The spectra of ejected protons calculated by the time-dependent density functional approach are in good agreement with the experimental data. The results of the simulations give detailed insight into the correlated electron and nuclear dynamics and complement the experiment with a time-dependent physical picture. It is demonstrated that the Coulomb explosion in the studied molecular systems is a sudden, all-at-once fragmentation where the ionization step is followed by a simultaneous ejection of the charged fragments. [7], and Coulomb explosion [8,9]. Highly energetic dissociation of a molecule or solid due to multiple ionization, known as the Coulomb explosion, is a particularly interesting process because it exposes the key physical mechanisms associated with the electron and nuclear dynamics and ionization [9][10][11][12][13]. Once the laser strips electrons from the molecule, the remaining positively charged structure can explode, creating a molecular plasma cloud. Coulomb explosion can be used to generate bright keV x-ray photons [14,15], highly energetic electrons [16], and for imaging [17][18][19].The strong-field ionization and fragmentation of hydrocarbon molecules is a prototypical example of the Coulomb explosion of polyatomic molecules, and it has been the subject of several experiments [9,11,[20][21][22][23]]. An important quantity measured in these experiments is the kinetic energy distribution of the protons ejected during the fragmentation. Proton energies in excess of 30 eV at only very moderate peak intensities of the driving laser pulses have been reported for both large [11] and small hydrocarbon molecules [9]. The proton kinetic cutoff energies depend sensitively on the laser intensity and saturate at intensities that depend on the molecular species [9,11]. Earlier, this behavior was attributed to the creation of a long-lived charge localization state [11]. A more recent experiment [9], in contrast, suggested that the high kinetic proton energies originate from Coulomb explosions from a high molecular charge state. It was suggested [9] that a multibond version of the enhanced ionization process [24,25] is responsible for reaching the observed high charge states, from which the protons are ejected simultaneously in a concerted Coulomb explosion process resulting in complete molecular fragmentations. A recent theoretical study [26] using a one-dimensional model of acetylene, C 2 H 2 , confirms the proposed ionization mechanism leading to the high charge states, but it did not investigate the fragmentation dynamics. While the experimental approaches allow the study of important aspects of the Coulomb explosion of molecules by analyzing the properties of the resulting fragments, they do not provide a complete, dynamical description of the internal mechanism taking place during the fragmentation.In this work, the intense laser puls...

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Strong laser-pulse-driven ionization and Coulomb explosion of hydrocarbon molecules

et al. 2012

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“…We would like to discuss our work in light of a recent study of vinylidene by Coulomb explosion imaging, 37 where it was found that 3.5 s after production of vinylidene, the population of the vinylidene isomer is still 50%. The framework given by the authors of Ref.…”

Section: H 2 Results-density Of States Analysismentioning

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Rovibrational spectroscopy of the v=6 manifold in C212H2 and C213H2

Srivastava

Conjusteau

Mabuchi

et al. 2000

The Journal of Chemical Physics

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We recorded rovibrational spectra of the 006 ϩ level of 12 C 2 H 2 and the 2131 1 1 Ϫ1 level of 13 C 2 H 2 in the ground electronic state using a two-photon sequential double resonance technique with a resolution of 15 MHz. Owing to the g/u symmetry of acetylene, the levels that we observe are inaccessible from the ground state by single photon techniques, and observation of these levels is reported here for the first time. Upper state rotational constants were derived from whole band fits of the observed lines, and compare favorably with expected values. Both spectra exhibit signs of local perturbations, and a density of states analysis leads us to believe that we are observing couplings to the full density of vibrational states one would expect from acetylene in this energy region. Despite the high resolution of our spectrometer, and the high excitation energy, no evidence for acetylene hydrogen permutation exchange isomerization ͑which is predicted to proceed through the vinylidene minimum on the potential͒ has been observed, implying that the rate of exchange isomerization is more than four orders-of-magnitude below the rate predicted by RRKM ͑Rice, Ramsperger, Kassel, and Marcus͒ theory.

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“…First, consider once again the acetylene-vinylidene isomerization. In Coulomb explosion experiments, 46 the molecule is prepared in the The Dance of Molecules Kellman and Tyng vinylidene form. Astonishingly, the system appears to cycle back and forth between the vinylidene and acetylene forms of Figure 6 for several microseconds.…”

Section: Energy Flow and Chemical Reactivitymentioning

confidence: 99%

The Dance of Molecules: New Dynamical Perspectives on Highly Excited Molecular Vibrations

Kellman

Tyng

2007

Acc. Chem. Res.

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At low energies, molecular vibrational motion is described by the normal modes model. This model breaks down at higher energy, with strong coupling between normal modes and onset of chaotic dynamics. New anharmonic modes are born in bifurcations, or branchings of the normal modes. Knowledge of these new modes is obtained through the window of frequency-domain spectroscopy, using techniques of nonlinear classical dynamics. It may soon be possible to "watch" molecular rearrangement reactions spectroscopically. Connections are being made with reaction rate theories, condensed phase systems, and motions of electrons in quantum dots.

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Study of Unimolecular Reactions by Coulomb Explosion Imaging: The Nondecaying Vinylidene

Cited by 98 publications

References 15 publications

Strong laser-pulse-driven ionization and Coulomb explosion of hydrocarbon molecules

Strong laser-pulse-driven ionization and Coulomb explosion of hydrocarbon molecules

Rovibrational spectroscopy of the v=6 manifold in C212H2 and C213H2

The Dance of Molecules: New Dynamical Perspectives on Highly Excited Molecular Vibrations

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