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Communication: Ultrafast time-resolved ion photofragmentation spectroscopy of photoionization-induced proton transfer in phenol-ammonia complex
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46.The pump pulses (∼7–10 μJ/pulse) were tightly focused by a f = 30 cm lens, while the probe pulses (∼6–9 μJ/pulse) were only loosely focused by adjusting a telescope placed upstream in the probe beam path.
47.Ionization of the PhOH-NH3 S1 state requires absorption of two probe photons, which leads to the conventional excitation-MPI detection for measuring S1-state dynamics. Note that, even if this contribution is not negligible, it does not interfere with the temporal behaviors observed in the early-time transients, because the PhOH-NH3 S1-state lifetimes in this energy region are at least a few hundred picoseconds.
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Photoionization-induced proton transfer (PT) in phenol-ammonia (PhOH-NH3) complex has been studied using ultrafast time-resolved ion photofragmentation spectroscopy. Neutral PhOH-NH3 complexes prepared in a free jet are photoionized by femtosecond [1+1] resonance-enhanced multiphoton ionization via the S1 state, and the subsequent dynamics occurring in the cations is probed by delayed pulses that result in ion fragmentation. The observed temporal evolutions of the photofragmentation spectra are consistent with an intracomplex PT reaction. The experiments revealed that PT in [PhOH-NH3]+ cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the reaction may take a much longer time scale to complete.
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