We report the experimental observation of ultrafast demethylation in ethanol dimers following single ionization induced by a 400-nm femtosecond laser field, described by the reaction ${\left({\mathrm{C}}_2{\mathrm{H}}_5\mathrm{OH}\right)}_2+n\hslash \omega \to \mathrm{C}{\mathrm{H}}_3+\mathrm{C}{\mathrm{H}}_2\mathrm{O}·\left({\mathrm{C}}_2{\mathrm{H}}_5\mathrm{OH}\right){\mathrm{H}}^{+}+e^{-}$. This demethylation pathway is identified through the detection of the ionic fragment $\mathrm{C}{\mathrm{H}}_2\mathrm{O}·\left({\mathrm{C}}_2{\mathrm{H}}_5\mathrm{OH}\right){\mathrm{H}}^{+}$, accompanied by the coincident measurement of emitted electron. Analysis of the electron-nuclear joint kinetic energy spectrum reveals multiple diagonal features spaced by the photon energy, showing the essential role of electron-nuclear correlation in the demethylation process. The reaction timescale is determined by introducing a time-delayed 800-nm femtosecond probe pulse, yielding a characteristic time of approximately 0.95 ps. This duration is longer than that observed for demethylation following single ionization of ethanol monomers, highlighting the pronounced influence of intermolecular interactions in the dimeric system.

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• Atomic & molecular processes in external fields
• Laser-cluster interaction
• Molecular dissociation
• Multiphoton or tunneling ionization & excitation
• Strong field ionization & excitation
• Ultrafast phenomena
• Clusters
• Femtosecond laser irradiation
• Ultrafast femtosecond pump probe