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The electronic and nuclear dynamics in methanol, following 156~nmphotoexcitation, are investigated by combining a detailed analysis oftime-resolved photoelectron spectroscopy experiments with electronic structurecalculations. The photoexcitation pump pulse is followed by a delayed 260~nmphotoionization probe pulse, to produce photoelectrons that are analyzed byvelocity map imaging. The yield of mass-resolved ions, measured with similarexperimental conditions, are found to exhibit the same time-dependence asspecific photoelectron spectral features. Energy-resolved signal onset anddecay times are extracted from the measured photoelectron spectra to achievehigh temporal resolution, beyond the 20~fs pump and probe pulse durations. Whencombined with {\it ab initio} calculations of selected cuts through the excitedstate potential energy surfaces, this information allows the dynamics of thetransient excited molecule, which exhibits multiple nuclear and electronicdegrees of freedom, to be tracked on its intrinsic few-femtosecond timescale.Within 15~fs of photoexcitation, we observe nuclear motion on the initiallybound photoexcited 2$^{1}$A$''$ (S$_2$) electronic state, through a conicalintersection with the 1$^{1}$A$'$ (S$_3$) state, which reveals paths tophotodissociation following C--O stretch and C--O--H angle opening.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Ultrafast Photodissociation Dynamics and Nonadiabatic Coupling Between  Excited Electronic States of Methanol Probed by Time-Resolved Photoelectron  Spectroscopy