Ionization and fragmentation dynamics of benzene in intense laser fields by tandem mass spectroscopy

Itakura, Ryuji; Watanabe, Jun; Hishikawa, Akiyoshi; Yamanouchi, Kaoru

doi:10.1063/1.1352619

Cited by 66 publications

(52 citation statements)

References 47 publications

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“…This demonstration suggests that not only could this previously unseen resonant multiphoton process have been observed in data taken elsewhere (Ref. [19] and references therein), but previous experimental data collected for other systems could also be reanalyzed by using MPE. The red triangles have been obtained by weighting the postsaturation signal over the presaturation signal to favor fitting after saturation.…”

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confidence: 65%

Reconstruction of ionization probabilities from spatially averaged data inNdimensions

2010

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We present an analytical inversion technique which can be used to recover ionization probabilities from spatially averaged data in an N-dimensional detection scheme. The solution is given as a power series in intensity. For this reason, we call this technique a multiphoton expansion (MPE). The MPE formalism was verified with an exactly solvable inversion problem in 2D, and probabilities in the postsaturation region, where the intensity-selective scanning approach breaks down, were recovered. In 3D, ionization probabilities of Xe were successfully recovered with MPE from simulated (using the ADK tunneling theory) ion yields. Finally, we tested our approach with intensity-resolved benzene ion yields showing a resonant multiphoton ionization process. By applying MPE to this data (which was artificially averaged) the resonant structure was recoveredsuggesting that the resonance in benzene may have been observable in spatially averaged data taken elsewhere.

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confidence: 65%

Reconstruction of ionization probabilities from spatially averaged data inNdimensions

2010

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“…31 The correlation between ionization and structural deformation plays a key role in fragmentation or reaction processes. [32][33][34] In other words, the competition between ionization and fragmentation governs the fate of the molecule in an intense field. One interesting example is C 60 .…”

Section: Introductionmentioning

confidence: 99%

Theoretical Investigations of the Electronic and Nuclear Dynamics of Molecules in Intense Laser Fields: Quantum Mechanical Wave Packet Approaches

Kono

Satô

Kanno

et al. 2006

Bulletin of the Chemical Society of Japan

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We have developed a method for describing the reaction dynamics of a polyatomic molecule in intense laser fields. First, the dynamical behavior of H 2 þ and H 2 in near-infrared, intense laser fields (I > 10 13 W cm À2 and ! > 700 nm) was examined; accurate evaluation of the electronic and nuclear wave packet was achieved by the dual transformation method that we developed. Using ''field-following'' time-dependent adiabatic states defined as eigenfunctions of the ''instantaneous'' electronic Hamiltonian, we have clarified the dynamics of bound electrons, ionization processes, Coulomb explosion processes, and molecular vibrations of H 2 þ and H 2 . The analyses indicate that the multielectron dynamics and nuclear dynamics of polyatomic molecules in intense fields can be described by using the potential surfaces of time-dependent adiabatic states and the nonadiabatic coupling elements between those states. To obtain time-dependent adiabatic states of a molecule, one can diagonalize the electronic Hamiltonian including the interaction with the instantaneous laser electric field by ab initio molecular orbital (MO) methods. The time-dependent adiabatic potentials obtained are used to evaluate the multichannel nuclear dynamics until the next ionization process. We have applied the time-dependent adiabatic state approach to reveal the characteristic features of the dynamics of structural deformations of CO 2 and its cations in a near-infrared intense laser field. The experimentally observed stretched and bent structure of CO 2 3þ just before Coulomb explosions originates from the structural deformation of CO 2 2þ . We also revealed the mechanism of the experimentally observed bond dissociation of C 2 H 5 OH; we found that the relative probability of C-O bond cleavage to that of C-C bond cleavage becomes smaller with decreases in the pulse length. This example clearly shows that field-induced nonadiabatic transitions play a decisive role in the reaction dynamics of molecules in an intense laser field.

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“…While there is clearly a trend of decreasing indirect ionisation with gap energy, there is also a significant spread of ratios around each gap energy. Earlier work has noted the importance of ionic resonances in determining whether dissociation occurs in SFI [31,32,33,34]. While the energy separations and transition dipole moments between ionic states at the Franck Condon (FC) point for vertical ionization are important, vibrational dynamics during the ionisation process can also lead to dynamic resonances and transitions between ionic Figure 3: R IF−P , fragment production from excitation of parent ion divided by total parent ion production.…”

Section: Indirect Fragment Vs Parentmentioning

confidence: 99%

Removing electrons from more than one orbital: direct and indirect pathways to excited states of molecular cations

Zhao

Sándor

Rozgonyi

et al. 2014

J. Phys. B: At. Mol. Opt. Phys.

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Abstract. We use velocity map imaging of photoelectrons in coincidence with molecular cations to determine which ionic states are populated via strong field ionisation, and whether the ionisation to excited ionic states proceeds indirectly via the ground ionic state or directly from the neutral. We carry out measurements on a series of molecules that have different energy gaps between the ground ionic state and dissociative excited states. We measure both direct and indirect ionisation to excited states of the molecular cations, and find that the energy gap between non-dissociative and dissociative states plays an important role in determining the amount of excited state ionisation. Direct ionisation to dissociative states is generally comparable to ionization to the ground state for gap energies less than the photon energy, but is suppressed for gap energies larger than the photon energy.

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Ionization and fragmentation dynamics of benzene in intense laser fields by tandem mass spectroscopy

Cited by 66 publications

References 47 publications

Reconstruction of ionization probabilities from spatially averaged data inNdimensions

Reconstruction of ionization probabilities from spatially averaged data inNdimensions

Theoretical Investigations of the Electronic and Nuclear Dynamics of Molecules in Intense Laser Fields: Quantum Mechanical Wave Packet Approaches

Removing electrons from more than one orbital: direct and indirect pathways to excited states of molecular cations

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