Experimental layout of the ps time-resolved electronically delayed two-color pump-probe system. Both transient absorption and transient Raman detection setups are shown. The solid lines show the optical paths. The dashed lines refer to electronic connections (timing): (BS) beamsplitter; (DBM) double balanced phase mixer; (FI) Faraday isolator; (HWP) wave-plate; (M) mirror; (FL) focusing lens; (F) glass filter; (BBO) BBO crystal; (BC) beam combiner; (NF) Raman notch filter; (MC) monochromator; and (PC) computer.
Time (phase) delay calibration curve of the phase shifter in the fundamental phase-locked loop. The horizontal axis is the dc voltage applied to the phase shifter.
Experimental layout of the ps regenerative amplifier: (L) convex fused silica lens (Thorlabs); , crystal (Crystal Systems); (M1) output coupler ( at , CVI); (M2–M3) high-reflectivity flat mirror (, CVI); (CM1–CM6) high-reflectivity concave mirror (, CVI; CM1, CM2, CM3, CM6, ; CM4, CM5, ); (CD1–CD2) acoustic optical fused silica Bragg cell (APE Berlin); (QS) acoustic optical crystal quartz -switch (NEOS); (IM1–IM2) injection mirror (CVI); (EM1–EM2) ejection mirror (CVI); (PD) ET-2020 photodiode (EOT), monitoring the amplifier cavity properties.
Autocorrelation and spectral comparisons between the amplified pulses and seed pulses at a wavelength of . (a) Autocorrelation comparison. The solid line is the autocorrelation from the amplified pulses, which corresponds to a (FWHM) pulse. The dashed line is the autocorrelation from the seed pulses, which also corresponds to a (FWHM) pulse. (b) The solid line is the spectral comparison of the amplifier pulses, and the dashed line is the spectrum of the seed pulses.
Output power as a function of wavelength for the ps regenerative amplifier at a repetition rate of using a multiline laser pump and pulse ejection after 20 round trips. The wavelength range is limited by the seed laser, which does not contain broad band optical mirrors. The ps regenerative amplifier is designed with all high-reflectivity mirrors that have peak reflectivity near with bandwidth .
The polarized pump-probe signal decay of HH in borate buffer . The solid line is the calculated signal obtained using the parallel and perpendicular signals and Eq. (8). The pump wavelength is ; the pump energy is ; and the pump pulse width is (FWHM). The probe wavelength is ; the probe energy is ; and the probe pulse width is (FWHM). Both the pump beam and the probe beam are focused to at the sample position.
The calculated anisotropy decay of HH in borate buffer . The polarized pump-probe data are taken from Fig. 6. The solid line is a single exponential fit to the average of the various decays. The fitting parameters yield an amplitude of 0.053 and a time constant of .
The magic angle pump-probe rebinding kinetics signal of HH in borate buffer . The signal is normalized to 1 at . The pump and the probe energy are 4.0 and , respectively. All other conditions are the same as in Fig. 6.
(a) Pump-probe signal of HH in borate buffer with an extended time window from ps to ms. The open squares are the data from Fig. 8. The open circles are the data obtained using a laser flash photolysis instrument (unpolarized pulses pump and cw probe). The solid line is a fit to the data using the MEM. The fitting time constant distributions are shown in (b). All signals are normalized to 1 at . (b) The MEM fitting time constant distributions of HH associated with the experimental data from (a).
Summary of ps geminate phase, ns geminate phase, and bimolecular phase for oxygen binding to myoglobin (the are the time constants and the are the corresponding amplitudes associated with the various kinetic rebinding phases).
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