The experimental data on CTTS reaction from I to polar protic solvents were published by Okuyama et al. (18). The internal conversion of eaq was newly measured in the present work. A 15-μm-diameter liquid microjet was injected into the vacuum and illuminated at 1 mm downstream from the nozzle with three laser pulses for synthesis, pump, and probe of eaq. The driving laser was a 10-kHz one box Ti:sapphire laser with 35-fs pulse duration. The synthesis pulses (200 nm) excited Br in a 0.3 M NaBr aqueous solution to create eaq by the CTTS reaction. The eaq thus created were thermalized for 500 ps, and the pump pulses (720 nm) excited them to the p state. Last, the probe pulses (270 nm) interrogated the time evolution of the nonstationary state using photoemission. Since the VBE of liquid water [11.3 eV; (34)] is far greater than the probe photon energy, no background signal was created from water. The photoelectrons were detected using a TOF electron energy analyzer with the detection axis perpendicular to the liquid jet and laser beams. All of the laser pulses were linearly polarized, and their polarization directions were parallel to the electron detection axis. The pulse duration of the 200-nm synthesis pulse was stretched using a 45-mm-thick synthetic quartz block to minimize multiphoton excitation. The laser pulse energies were 13, 185, and 41 nJ for the synthesis, pump, and probe pulses, respectively. Streaming potential was canceled by applying a voltage to the liquid-discharging nozzle.

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