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Time-Resolved Nonlinear Laser Spectroscopy: Development of a Picosecond 4-BEAM Stimulated Raman Gain Set-Up and Theoretical Analysis of the Dephasing Signal.

Martine M. De Maziere

Published Jan 1, 1986• 0 citations
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Quantum theory of （femtosecond）time-resolved stimulated Raman scattering

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A detailed theoretical analysis is presented of the dephasing signal measured in four-beam picosecond time-resolved stimulated-Raman-gain experiments. The analytical expressions derived are successful in simulating observations on the CS2 model system under various experimental conditions. It is established that the tail of the curve for sufficiently long delay times is uniquely determined by the vibrational Raman term that yields the vibrational dephasing time T2. It is also found that the rotational dephasing time cannot be fundamentally determined from the rotational Raman peak centered around zero delay. Furthermore, it is shown that the coherence properties of the stimulating laser fields, as distinguished from their pure pulse-envelope properties, are crucially important in determining the time resolution of the experiments and for explaining several experimental phenomena observed under mismatched excitation-pulse conditions. In this respect, the domain model for mode-locked pulses has proved to be useful. It is found that the time resolution of the dephasing measurements is determined by the combined pulse-coherence time of the driving fields and not by the cross-correlation width of the pulse envelopes.
The pump and probe variant of the stimulated Raman gain technique permits the measurement of picosecond dephasing times with low-power, continuous-wave mode-locked lasers, but it suffers by its susceptibility to inevitable randomly induced fluctuations in the relative phases of the interacting laser fields. The resulting severe requirements on optical stability can be circumvented through application of a double-modulation–detection scheme that we have developed. It is based on rms detection of the T2 signal as generated through application of a low-frequency phase modulation of precise amplitude, additional to the commonly applied rf modulation with corresponding lock-in detection. A detailed description of the method and its experimental realization is presented. T2 measurements on the 656 cm−1 vibration of liquid CS2 illustrate its performance. In comparison with previous techniques, precision is improved by about a factor of 4. But more important is the fact that the technique permits to make a continuous recording of the T2 signal, while achieving at the same time a reduction in measurement time by an order of magnitude. Furthermore, optimization of the optical setup is possible, through direct monitoring of the dephasing signal at any delay. Automating the data taking and processing should be straightforward.
We theoretically investigate a scheme in which stimulated Raman scattering (SRS) can be suppressed by coherently controlling the coupling between molecular states. In conventional SRS, two laser beams at different frequencies interact resonantly with molecular vibration to induce a gain and a loss for the two beams, respectively. In our scheme, a third beam is introduced to couple the vibrational state to another coupling state. As a result, SRS is suppressed in a way analogous to electromagnetically induced transparency. We calculated the SRS signal analytically by the density matrix approach, and investigated the feasibility of this scheme for real molecular imaging. In SRS microscopy, a donut-shaped coupling laser can be used to suppress the SRS signal from the rim part of the focal spot, leading to super-resolution. Based on our numerical studies, the lateral resolution starts to be enhanced when the coupling laser intensity exceeds 0.1TW/cm20.1\phantom{\rule{0.16em}{0ex}}\mathrm{TW}/\mathrm{c}{\mathrm{m}}^{2}0.1TW/cm2 at picosecond pulse duration.