Zinth, Wolfgang and Kaiser, Wolfgang
Raman spectroscopy with ultrashort coherent excitation. Narrowing of spectral lines beyond the dephasing linewidth.
3. New Zealand Symposium on Laser Physics, 17. - 23. Januar 1983, Hamilton, Neuseeland.
Spectroscopists are constantly faced with the task of improved spectral resolution. Two points are of major interest: (i) The precise frequency of the quantized transition and (ii) the detection of new neighboring transitions. Besides experimental factors the ultimate spectral resolution is determined by the inherent linewidth of the transition. Optical spectroscopists have to deal with different line-broadening processes; for instance with the Doppler effect or with collision broadening in gases, with dephasing processes in condensed systems and with the population relaxation which results in the natural linewidth. In recent years, different novel techniques have been devised which provide spectral resolution beyond the transition linewidth. For instance, Doppler broadening can be eliminated by saturation spectroscopy or by two counter-propagating beams for two-photon transitions/I/. Even measurements beyond the natural linewidth have been performed taking biased signals from the fluorescent decay /2-5/. Techniques have been proposed where the difference between the decay rates of the two states rather than their sum determines the linewidth /6,7/, and narrowing of the natural linewidth by decaying-pulse excitation has been discussed /8/. Very recently, we have demonstrated substantial line narrowing of Raman type transitions in condensed phases /9-11/. The lines were broadened by vibrational dephasing. New information was obtained in congestedspectral regions.