Transient coherent Raman scattering in the time and frequency domain

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

Vibrational lifetimes and intramolecular energy randomisation of polyatomic molecules in liquids

Transient experiments with picosecond laser pulses give valuable information on the dynamic properties of polyatomic molecules in the electronic ground state. In small molecules the decay of vibrational energy occurs via individual lower energy states; in large molecules the experimental data support a statistical model

Generation of chirp-free picosecond pulses

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

Proceedings of the Thirteenth International Conference on Time-Resolved Vibrational Spectroscopy

The thirteenth meeting in a long-standing series of “Time-Resolved Vibrational Spectroscopy” (TRVS) conferences was held May 19th to 25th at the Kardinal Döpfner Haus in Freising, Germany, organized by the two Munich Universities - Ludwig-Maximilians-Universität and Technische Universität München. This international conference continues the illustrious tradition of the original in 1982, which took place in Lake Placid, NY. The series of meetings was initiated by leading, world-renowned experts in the field of ultrafast laser spectroscopy, and is still guided by its founder, Prof. George Atkinson (University of Arizona and Science and Technology Advisor to the Secretary of State). In its current format, the conference contributes to traditional areas of time resolved vibrational spectroscopies including infrared, Raman and related laser methods. It combines them with the most recent developments to gain new information for research and novel technical applications. The scientific program addressed basic science, applied research and advancing novel commercial applications. The thirteenth conference on Time Resolved Vibrational Spectroscopy promoted science in the areas of physics, chemistry and biology with a strong focus on biochemistry and material science. Vibrational spectra are molecule- and bond-specific. Thus, time-resolved vibrational studies provide detailed structural and kinetic information about primary dynamical processes on the picometer length scale. From this perspective, the goal of achieving a complete understanding of complex chemical and physical processes on the molecular level is well pursued by the recent progress in experimental and theoretical vibrational studies. These proceedings collect research papers presented at the TRVS XIII in Freising, German

New Results on Ultrafast Coherent Excitation of Molecular Vibrations in Liquids

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

Time resolved observation of resonant and non-resonant contributions to the nonlinear susceptibility χ(3)

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

Terahertz quantum beats in molecular liquids

With ultrashort pulses of less than 100 fs it is possible to excite coherently several vibrational modes of polyatomic molecules simultaneously. The femtosecond time resolution of the experiment allows the study of pronounced high-frequency beat phenomena up to 10 THz. The frequency difference between vibrational modes separated by more than 300 cm−1 may be determined with high precision