(Color online) Energetics of ionization and fragmentation of OClO (all values are given in eV), displaying also the ionization potentials (IPs) and appearance potentials (APs) for the different channels. Schematically indicated also are the excited states involved in the dynamics. For the pump and probe photons, typical values are shown.
(Color online) Ion signals as a function of the delay time between the pump and probe pulses on (a) the long-time scale and (b) the short-time scale. The contribution denoted by describes the decay of the initially excited state with the time constant . The decay time of the small contribution to the signal is . The term reflects the population of the intermediate states and , while characterizes the formation of the dissociation products. A small contribution (nr) due to nonresonant absorption of pump and probe photons is necessary to satisfy the fit of the ion signals near the delay time zero. The superposition of the fit curves (thin solid lines) of the different contributions reveals the resultant ion signal (thick line) of each species. The scales of the ordinates for the different species reflect their true size relations.
(Color online) Coherent oscillation of time-dependent ion signals of and excited at and ionized at [cf. Fig. 2(b)]. The oscillation periods of for and for correspond to the respective vibronic frequency differences of the two isotopes. The diamonds and circles represent the experimental data, and full lines represent the best fit using a single frequency, damped oscillation. As shown in the inset, no oscillation is observed for a slightly changed pump wavelength of .
(Color online) Time-dependent ion signals of OClO and its fragmentation products Cl and ClO vs delay time between pump and probe pulses on (a) the long-time scale and (b) the short-time scale. The decay time of the preferentially excited state [contribution ] is , while the weakly populated state decays with ; otherwise as Fig. 2.
(Color online) Ion signals of OClO and its fragmentation products as a function of the delay time between pump and probe pulses on (a) the long-time scale and (b) the short-time scale. Here the main contribution decays with and the small contribution with ; otherwise as Fig. 2.
(Color online) Ion signals of OClO and its fragmentation products vs delay time between pump and probe pulses. The contribution decays with , while the population decays with ; otherwise as Fig. 2.
Time constants , , and obtained for photodissociation of OClO molecules excited at different wavelengths ; nm—nonmeasurable.
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