Single-pulse nonlinear Raman

The Application oi Single-Pulse Nonlinear Raman Techniques to a Liquid Photolytic Reaction... 

This chapter describes the application of these techniques to a liquid photolytic reaction. The motivation was the assessment of the capabilities and limitations of single-pulse nonlinear Raman spectroscopy as a probe of fast reactions in energetic materials. 

Dudovich, N., Oron, D., and Silberberg, Y. 2002. Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy. Nature 418 512-14. 

Lim, S. H., Gaster, A. G., and Leone, S. R. 2005. Single-pulse coherently controlled nonlinear Raman scattering spectroscopy. Phys. Rev. A 72 0418031. 

Such single-mode lasers, often pulse amplified by dye laser amplifiers pumped by injection-locked Nd YAG lasers, are used in nonlinear Raman techniques by which an instrumental resolution better than 0.001 cm is achieved (Esherick and Owyoung (1982), Schrotter et al. (1988a)). 

The implementation of time-resolved CARS for microspectroscopy and its application for vibrational imaging based on RFID was first demonstrated by Volkmer et al. [64] using three incident pulses that are much shorter than the relevant material time scale. Here, a pair of temporally overlapped pump and Stokes femtosecond pulses was used to impulsively polarize the molecular vibrations in the sample. Impulsive excitation with a single ultrashort pulse is also possible provided that the spectral bandwidth of the pulse exceeds the Raman shift of the molecular vibration of interest [152]. The relaxation of the induced third-order nonlinear polarization is then probed by scattering of another pulse at a certain delay time, r. A measurement of the RFID consists of the CARS signal collected at a series of delay times. 

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