Acetylene-vinylidene isomerization in ultrashort intense laser fields studied by triple ion-coincidence momentum imaging

Hishikawa, Akiyoshi; Matsuda, Akihiro; Takahashi, Eiji J.; Fushitani, Mizuho

doi:10.1063/1.2828557

Cited by 42 publications

(31 citation statements)

References 29 publications

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“…Isomerization of acetylene (HCCH) to form vinylidene (H 2 CC) has been studied in the neutral molecule, as well as singly and doubly charged acetylene ions 1,2,[24][25][26][27][28][29][30][31][32][33][34][35][36] . Acetylene cations are important not only as a model for molecular dynamics and radiation damage investigations, but also in a range of applications, from plasma devices 37 , combustion 38 , semiconductor manufacturing 39 and to understanding planetary atmospheres 40 .…”

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confidence: 99%

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Ultrafast isomerization initiated by X-ray core ionization

et al. 2015

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Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a 'molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.

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“…The mechanism of the unexpectedly fast isomerization could not be probed by the measurements reported in refs 1,2, because they were not time resolved. This process has been studied in time-resolved optical laser experiments coupled with three-and four-particle coincident detection 30,32,33,36 .…”

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confidence: 99%

Ultrafast isomerization initiated by X-ray core ionization

et al. 2015

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“…This isomerization has been invoked in the dissociative electroionization of C 2 H 2 in the C + , C 2 + and CH 2 + dissociation channels [25]. The same process has been invoked for the dissociation of doubly [26,27] and triply ionized [28] acetylene. However, to our knowledge, no experimental evaluation of the energy difference between the two singly ionized isomers exists in the literature.…”

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confidence: 99%

A photoionization mass spectrometric and threshold photoelectron-photoion coincidence study of vinylbromide (C2H3Br) in the vacuum ultraviolet range of 6–21eV

Hoxha

Locht

et al. 2011

Chemical Physics

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The dissociative photoionization of vinyl bromide (C 2 H 3 Br) has been investigated by photoionization mass spectrometry (PIMS) and time-of-flight threshold photoelectronphotoion coincidence (TOF-TPEP-ICO) spectrometry using synchrotron radiation. The photoionization efficiency curves of the three most abundant ions, i.e. C 2 H 3 Br + , C 2 H 3 + and C 2 H 2 + , are measured and analyzed in detail. A C 2 H 3 + /Br -photoion-pair formation process has been detected for the first time. Some arguments are provided in favor of the electronic excitation of the C 2 H 3 + fragment and of the isomerization of the C 2 H 2 + ions. The breakdown diagram for these ions in the 9.8-21 eV photon energy range, derived from TOF-TPEPICO mass spectra, is discussed. The involvement of the successive C 2 H 3 Br + ionic states and the role of autoionization of C 2 H 3 Br Rydberg states are emphasized. For the two minor HBr + and Br + fragment ions only the breakdown diagrams are measured and appearance energies are derived.

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“…Electron and heavy-ion beams, synchrotron, and laser radiation have been used [3][4][5][6][7][8] to produce double ionization either directly via the ejection of two valence electrons or indirectly via inner-shell ionization followed by the Auger decay [9,10]. In the present work, we report on the fragmentation of the ethyne dication via the C + -H + fragmentation channel formed following inner-shell ionization by electron impact, studied by Auger electron-ion-ion coincidence spectroscopy.…”

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Effect of the charge localization in theC+−H+fragmentation pathway of the ethyne dication

et al. 2011

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The C + -H + channel in the fragmentation of the ethyne dication following inner-shell ionization has been studied by Auger electron-ion-ion coincidence spectroscopy. The ion-ion coincidence map shows a peculiar feature which corresponds to the emission of both the H + and C + ions in the same direction. The analysis of the data, complemented by ab initio calculations, suggests an interpretation in terms of a two-step, asynchronous concerted reaction, in which the charge of the ethynyl intermediate ion localizes on the terminal carbon atom.

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Acetylene-vinylidene isomerization in ultrashort intense laser fields studied by triple ion-coincidence momentum imaging

Cited by 42 publications

References 29 publications

Ultrafast isomerization initiated by X-ray core ionization

Ultrafast isomerization initiated by X-ray core ionization

A photoionization mass spectrometric and threshold photoelectron-photoion coincidence study of vinylbromide (C2H3Br) in the vacuum ultraviolet range of 6–21eV

Effect of the charge localization in theC+−H+fragmentation pathway of the ethyne dication

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