Abstract
The gain characteristics and spectral properties of transient stimulated Raman scattering are investigated in the non-resonant case. For moderate amplification of the input Stokes pulses by a factor of approximately 2 two distinct frequency bands appear in the output Stokes spectrum at the input and resonant frequency positions. The intensity ratio of the two components sensitively depends on pump intensity, frequency off-set and, most important, details of the dynamical properties of the molecular transition. For a quantitative description the simple case of purely exponential dephasing considered previously has to be replaced by a more general theory with correlation time τ4 (relevant for short times) and the asymptotic decay timeT 2. It is shown that the spectral properties of stimulated Raman scattering are strongly effected by τ4. Experimental data for theν 1 CH2 vibration of liquid CH2BrCl are presented. For the first time, τ4 is determined from transient stimulated amplification yielding τ4 = 0.7 ± 0.2ps. Our results on non-exponential dephasing are also relevant for other nonlinear Raman techniques.
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References
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