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Volume 194, 2016
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Visualization of bond rearrangements in acetylene using near single-cycle laser pulses

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Abstract

The migration of hydrogen atoms resulting in the isomerization of hydrocarbons is an important process which can occur on ultrafast timescales. Here, we visualize the light-induced hydrogen migration of acetylene to vinylidene in an ionic state using two synchronized 4 fs intense laser pulses. The first pulse induces hydrogen migration, and the second is used for monitoring transient structural changes via Coulomb explosion imaging. Varying the time delay between the pulses reveals the migration dynamics with a time constant of 54 ± 4 fs as observed in the H+ + H+ + CC+ channel. Due to the high temporal resolution, vibrational wave-packet motions along the CC- and CH-bonds are observed. Even though a maximum in isomerization yield for kinetic energy releases above 16 eV is measured, we find no indication for a backwards isomerization — in contrast to previous measurements. Here, we propose an alternative explanation for the maximum in isomerization yield, namely the surpassing of the transition state to the vinylidene configuration within the excited dication state.

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Publication details

The article was received on 15 Apr 2016, accepted on 10 May 2016 and first published on 10 May 2016


Article type: Paper
DOI: 10.1039/C6FD00082G
Citation: Faraday Discuss., 2016,194, 495-508
  • Open access: Creative Commons BY license
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    Visualization of bond rearrangements in acetylene using near single-cycle laser pulses

    C. Burger, N. G. Kling, R. Siemering, A. S. Alnaser, B. Bergues, A. M. Azzeer, R. Moshammer, R. de Vivie-Riedle, M. Kübel and M. F. Kling, Faraday Discuss., 2016, 194, 495
    DOI: 10.1039/C6FD00082G

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