Schematic representation of the apparatus used to generate few-cycle pulses in the present experiments (see text). Pulses 10 fs long and of 150 μJ energy were focused using a 5 cm curved mirror located within an ultrahigh vacuum chamber so as to yield peak laser intensities in the 1015 W cm−2 range at focused spot where the laser-molecular interaction occurred. Ions formed in this interaction were accelerated into a 20 cm long time-of-flight (TOF) spectrometer. A typical TOF spectrum showing H2 + ions from H2O is shown. Also shown are typical traces of the laser pulse duration and the phase, as deduced by SPIDER (see text).
Two-dimensional contour plots of the potential energy surface of H2O2+ for θ = 30°, 60°, 90°, and 120° clearly showing the two dissociation channels OH+ + H+ and H+ + OH+.
A section through the fitted potential energy surface of the H2O2+ dication along with ab initio data points at θ = 30°, 60°, 90°, and 120° for r 12 = 2.0 au. Inset shows the coordinate system used for PES calculation.
A section through the dication potential energy surface along with ab initio data points at θ = 30°, 60°, 90°, and 120° with r 12 (au) and r 13 (au) changing simultaneously.
Three-dimensional probability density plots for the wave packet at different time intervals for γ = 90° (left) andγ = 175° (right) during evolution for an initial wave packet at t = 0. Inset shows the Jacobi coordinate system.
Norm calculated for the evolving wave packet in the H2 + channel (r < 3.0 au and R > 2.0 au).
Expectation value of r and R calculated at each time step in the H2 + channel.
Parameters of the H2O2+ potential energy surface, in Å.
Grid parameters used in the present study.
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