Time-resolving the ultrafast H2 roaming chemistry and H3 + formation using extreme-ultraviolet pulses

Ester Livshits, Itamar Luzon, Krishnendu Gope, Roi Baer, Daniel Strasser*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

30 Scopus citations

Abstract

The time scales and formation mechanisms of tri-hydrogen cation products in organic molecule ionization processes are poorly understood, despite their cardinal role in the chemistry of the interstellar medium and in other chemical systems. Using an ultrafast extreme-ultraviolet pump and time-resolved near-IR probe, combined with high-level ab initio molecular dynamics calculations, here we report unambiguously that H3 + formation in double-ionization of methanol occurs on a sub 100 fs time scale, settling previous conflicting findings of strong-field Coulomb explosion experiments. Our combined experimental–computational studies suggest that ultrafast competition, between proton-transfer and long-range electron-transfer processes, determines whether the roaming neutral H2 dynamics on the dication result in H3+ or H2+ fragments respectively.

Original languageAmerican English
Article number49
JournalCommunications Chemistry
Volume3
Issue number1
DOIs
StatePublished - 1 Dec 2020

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© 2020, The Author(s).

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