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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 H 3  +  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 H 2  dynamics on the dication result in    $${\mathrm{H}}_3^ +$$  H 3 + or    $${\mathrm{H}}_2^ +$$  H 2 + fragments respectively.

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