Ultrafast Deformation of the Geometrical Structure of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">CO</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>Induced in Intense Laser Fields

Hishikawa, Akiyoshi; Iwamae, Atsushi; Yamanouchi, Kaoru

doi:10.1103/physrevlett.83.1127

Cited by 147 publications

(122 citation statements)

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“…By the development of the concept of enhanced ionization it became possible to explain the reason why the kinetic energy of fragment ions recorded by Coulomb explosion imaging was considerably lower than the kinetic energy expected, when the Coulomb explosion takes place at the equilibrium position of the ground state electronic potential energy surface of the neutral parent molecule [29][30][31][32][33]. Since then, the EI mechanism has been investigated extensively for diatomic molecules, e.g., [34][35][36][37], as well as for triatomic molecules [38][39][40][41].…”

Section: Introductionmentioning

confidence: 99%

Role of proton dynamics in efficient photoionization of hydrocarbon molecules

et al. 2014

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We experimentally investigate the ionization mechanism behind the formation of remarkably high charge states observed in the laser-pulse-induced fragmentation of different hydrocarbon molecules by Roither et al. [Phys. Rev. Lett. 106, 163001 (2011)], who suggested enhanced ionization occurring at multiple C-H bonds as the underlying ionization mechanism. Using multiparticle coincidence momentum imaging we measure the yield of multiply charged fragmenting ethylene and acetylene molecules at several intensities and pulse durations ranging from the few-cycle regime to 25 fs. We observe, at constant intensity, a strong increase of the proton energy with increasing laser pulse duration. It is shown that this is caused by a strong increase in the yield of highly charged parent molecular ions with pulse duration. Based on experimental evidence we explain this increase by the necessary population of precursor states in the parent ion that feature fast C-H stretch dynamics to the critical internuclear distance, where efficient ionization via enhanced ionization takes place. For increasing pulse duration these precursor ionic states are more efficiently populated, which leads in turn to a higher enhanced-ionization probability for longer pulses. Our work provides experimental evidence for the existence of a multiple-bond version of enhanced ionization in polyatomic molecules.

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Section: Introductionmentioning

confidence: 99%

Role of proton dynamics in efficient photoionization of hydrocarbon molecules

et al. 2014

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“…For CO 2 molecules we found the bond angle of the bent species reached 161°; this value should be compared to the 140°d etermined by Hishikawa et al 21 As the electric field is increased and ionization takes place, the TG signal decreases and gives way to a background signal caused by the plasma. In Figure 7e-g, we showed CO 2 molecules in the presence of an increasingly strong electric field.…”

Section: Discussionmentioning

confidence: 99%

“…These observations are consistent with Coulomb explosion measurements from our group and from other groups. 21,25,64 Two explanations for this deformation were discussed, one involving excited electronic states with bent geometry, and one dealing strictly with perturbations to the ground state potential. We plan to explore evidence of electronic state involvement by laser induced fluorescence after strong electric field interaction.…”

Section: Discussionmentioning

confidence: 99%

“…Mapping the distribution of the fragment ions gives information about the molecular structure prior to explosion. [17][18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33] While very powerful, it is very difficult to determine a sequence of events leading to the observed fragment distribution using the CE method. For example, it is important to determine if structural deformation takes place in the neutral molecules or it arises after ionization.…”

Section: Introductionmentioning

confidence: 99%

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Ultrafast Laser Induced Molecular Alignment and Deformation: Experimental Evidence from Neutral Molecules and from Fragment Ions

2003

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The alignment and molecular structure deformations induced by intense off-resonance excitation with ultrafast laser pulses are examined using femtosecond transient grating spectroscopy and by angle resolved multiphoton ionization in a molecular beam. The goal of this study is to correlate evidence obtained from the angular dependence of multiphoton ionization and from rotational recurrences observed in neutral molecules regarding alignment and molecular structure deformation. Structural parameters are determined by analysis of the fieldfree rotational recurrences, obtained by transient grating measurements, or by analysis of the anisotropy in the detected fragment ions, in the molecular beam experiments. Experimental data were obtained for CS 2 , CO 2 , acetylene, and benzene, for pulse intensities ranging from 10 11 to 10 14 W/cm 2 . The experimental results are consistent with molecular alignment resulting from a "kick" induced by the ultrafast off-resonance field. The results also provide evidence of molecular structure deformations. Results from transient grating experiments indicate that the electric field can induce alignment and bending in polyatomic molecules and that these effects can take place in the absence of ionization.

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“…[13][14][15] Among them, the laser-based Coulomb explosion has attracted much attention because it has the advantage of high temporal resolution. Now, laserbased Coulomb explosion has been demonstrated to be a) Email: cywu@pku.edu.cn b) Email: hongmei@iccas.ac.cn a feasible approach to image the structure of short-lived intermediates, 16,17 small van der Waals complexes, 18,19 as well as chiral molecules.…”

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confidence: 99%

Communication: Determining the structure of the N2Ar van der Waals complex with laser-based channel-selected Coulomb explosion

Song

et al. 2014

The Journal of Chemical Physics

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We experimentally reconstructed the structure of the N2Ar van der Waals complex with the technique of laser-based channel-selected Coulomb explosion imaging. The internuclear distance between the N2 center of mass and the Ar atom, i.e., the length of the van der Waals bond, was determined to be 3.88 Å from the two-body explosion channels. The angle between the van der Waals bond and the N2 principal axis was determined to be 90° from the three-body explosion channels. The reconstructed structure was contrasted with our high level ab initio calculations. The agreement demonstrated the potential application of laser-based Coulomb explosion in imaging transient molecular structure, particularly for floppy van der Waals complexes, whose structures remain difficult to be determined by conventional spectroscopic methods.

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Ultrafast Deformation of the Geometrical Structure ofCO2Induced in Intense Laser Fields

Cited by 147 publications

References 14 publications

Role of proton dynamics in efficient photoionization of hydrocarbon molecules

Role of proton dynamics in efficient photoionization of hydrocarbon molecules

Ultrafast Laser Induced Molecular Alignment and Deformation: Experimental Evidence from Neutral Molecules and from Fragment Ions

Communication: Determining the structure of the N2Ar van der Waals complex with laser-based channel-selected Coulomb explosion

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