Theory of time-resolved coherent Raman scattering with spectrally tailored noisy light

✍ Scribed by Darin J. Ulness; A. C. Albrecht

• Publisher: John Wiley and Sons
• Year: 1997
• Tongue: English
• Weight: 566 KB
• Volume: 28
• Category: Article
• ISSN: 0377-0486
• DOI: 10.1002/(sici)1097-4555(199708)28:8<571::aid-jrs129>3.0.co;2-u

✦ Synopsis

The theory for the application of spectrally tailored ("two colorÏ) noisy light in an interferometric coherent Raman scattering (CRS) experiment called I(2)CRS(3c) is presented. The theory is concerned with the purely resonant contribution to the intensity level I(2)CRS(3c) signal. The tailored beam is modeled as a sum of two Lorentzians where the center frequency of each Lorentzian is assumed to be under experimental control. It is found that not only are the coherent Stokes-Raman scattering (CSRS) and coherent anti-Stokes-Raman scattering (CARS) signals emitted, but a third "hybridÏ frequency is also contained in the signal. It o †ers the promise of a new way to up-convert low frequency Raman active modes, while the same dynamic information contained in the radiation di †erence oscillations (RDOs) of previous incoherent CRS experiments remains. More generally, it o †ers an additional degree of freedom that allows for arbitrary experimental control over the position in frequency space in which the hybrid signal will emerge. In addition it is shown that the hybrid signal frequency contains dynamically important information in its arbitrarily placed (in frequency space) signal. Plots of monochromatically detected I(2)CRS(3c) interferograms calculated for di †erent parameter sets are shown together with the signal spectra. 1997