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Sample text

6) to (9) . ) is the sum of four types of terms : a zero-frequency term, high frequency terms, "broadband" terms, and a resonance term. That whioh interests us here is the resonant part of J(6)1) - i . , JROCllf) Notably, JR(IWI) oan be readily isolated from the other (undesirable) Fourier terms . (6) is the Raman susoeptibility of the sample, f 1(6) and f 2(6) are the spectral densities of the laser outputs (before the interferometer), and it has been assumed that every frequency of ooherent ly soat tered light is detected with unit effioiency.

The NLRS eroded and the lnnit:ing dynamical function becomes under :incoherent tnne resolved excitation (a » 'Yp » rj) the not are an which resembles a bnnolecular reaction. The coefficient is :independent of the detun:ing, contrary to the coherent case and the short component (NLRS) disappears. As a model system we explored the consequences of the high resolution spectrum of pyraz:ine-h4 , which was studied by Kommandeur et al. 13 These spectra exh:ibit a multitude of molecular eigenstates. We snnulated excitation of the two members P(l) and R(o) of the , B3U (0-0) transition by a 5 nsec pulse.

It is apparent that only the amplitude of each of J jj' decreases (proportionally to a), so that the general pattern of the PCR is preserved when the pulse is highly stochastic. v. g. O0 Time Time Fig. 3. The PCR for the P(l) line of a pyrazine excited by a short laser pulse (5 nsec) , on resonance (~w = 0) with various slow diffusion rates. The inset shows the spectrum taken from ref. (13). R(O) t p o 5nsec 6 ... 8 u i ~ Q. 6 .. 2 .. 4 E ~ 0 ,2 OO~'-L~~~-L~~~~~ o 40 80 120 160 200 0 Time 40 80 120 Time Fig.

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