Fluctuating pulse durations considerably influence the time resolution of probing experiments. The commonly used arithmetic averaging the experimental data changes the shape of the signal curves and gives longer decay times in the wings. Methods are presented to reduce the effect of fluctuating pulse durations.

Coherent Raman probe scattering experiments are performed to study dynamical processes of polyatomic liquids at 300 K. For single homogeneous transitions the dephasing timeT 2 is readily obtained from time resolved investigations. Spectral studies show an interesting time dependent shift in scattered frequency. After the excitaiton the vibrating molecules are shown to relax freely with their resonance frequency. Multiple, equally spaced transitions exhibit a beating phenomenon which provides the dephasing time and the frequency interval between neighboring vibrational states. Inhomogeneously broadened systems do not allow a ready determination of the dephasing time by the present probing technique. Previous experiments on the subject have to be reconsidered.

The presented theoretical model for a mode-locked Nd-glass laser simultaneously takes into account dynamics of the mode-locking dye, amplification saturation and radiation background. A systematic variation of laser parameters gives insight into the pulse formation process and allows to improve the laser design. The calculations show that it should be possible to decrease considerably the duration of light pulses of a mode-locked Nd-glass laser. Using a new mode-locking dye with a switching time of τ=2.7×10−12 s we obtained stable laser operation and a pulse duration of 1.7×10−12s.

The density of rotational transitions for a polyatomic molecule is so large that in general many such

transitions are hidden under the Doppler profile, this being a fundamental limit of conventional high

resolution electronic spectroscopy. We present here the first Doppler-free cw two-photon spectrum of a

polyatomic molecule. In the case of benzene, 400 lines are observed of which 300 are due to single rotational

transitions, their spacing being weil below the Doppler profile. The resolution so achieved is 1.5 X 10'.

Benzene is a prototype planar molecule taken to have D •• symmetry in the ground as weil as in the first

excited state. From our ultra-high resolution results it is found that benzene in the excited SI state i8 a

symmetrical rotor to a high degree. A negative inertial defect is found for the excited state. The origin of this

inertial defect is discused.

The nonresonant contributions to the nonlinear susceptibility χ(3) produce a frequency chirp during stimulated Raman scattering. In the case of transient stimulated Raman scattering, the spectrum of the generated Stokes pulse is found at higher frequencies than expected from spontaneous Raman data. The frequency difference can be calculated from the theory of stimulated Raman scattering.

A new type of Raman spectroscopy is presented: After transient excitation of molecular modes coherently scattered Raman spectra are investigated in a depayed probing experiment. The spectral position of the Raman mode is observed after long delay times. The dephasing time is obtained from the time dependence of the scattered amplitudes. Frequency disturbing non-resonant susceptibilities are eliminated. We report on first experimental results of transient coherent Raman spectroscopy of liquid CH3CCl3.

The second harmonic beam generated in a noncollinear arrangement allows the observation of the autocorrelation functio: A compact optical beam splitter and imaging system eliminates alignment problems. Single pulses of 1 ps duration and approximately 10−8 joule energy are readily observed using an optical multichannel analyser.

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The resonant and nonresonant part of χ(3) are distinguished by their different time behavior. The medium is coherently excited by two picosecond light pulses of defined frequency difference and the state of the system is monitored by a third properly delayed probe pulse. Results are presented on neat liquids of carbontetrachloride and cyclohexane and on the mixture of CCl4: C6H12.

The frequency spectrum of moderately chirped laser pulses depends upon the portion of the beam which is accepted by the spectrometer. Observation of the development of the chirp in a mode-locked pulse train allows to determine the small incipient chirp of early pulses. A product, bandwidth times pulse duration, of 0.47 ± 0.03 is consistently observed for single pulses switched from a passively mode-locked Nd-glass system.