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Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions
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10.1063/1.2751184
/content/aip/journal/jcp/127/4/10.1063/1.2751184
http://aip.metastore.ingenta.com/content/aip/journal/jcp/127/4/10.1063/1.2751184
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Schematic diagram of the energy level structure for the femtosecond CARS calculations for the transition in the fundamental (1,0) Raman band of the nitrogen molecule. The (, 1, 2, 3, and 4) transition strengths were varied to match the Raman cross section of .

Image of FIG. 2.
FIG. 2.

Temporal dependence of the real and imaginary components and the magnitude of the induced Raman coherence for the (a) , (b) , (c) , (d) , and (e) transitions in the fundamental (1,0) band of . The coherence matrix elements are normalized by dividing by the population of level prior to laser excitation. The difference between the central frequencies of the pump and Stokes lasers is . The Raman frequencies for the , , , , and transitions are 2329.8, 2329.4, 2328.0, 2325.8, and , respectively. The collisional dephasing rate for each Raman transition is , corresponding to a Raman linewidth of . The pump and Stokes laser temporal pulse shapes are both Gaussian with widths of (full width at half maximum). The pump and Stokes pulses are overlapped exactly in time. The peak irradiance for both the pump and Stokes pulses is .

Image of FIG. 3.
FIG. 3.

Temporal dependence of the phase of the induced Raman coherence for the , , and transitions in the fundamental (1,0) band of . The collisional dephasing rate and the pump and Stokes pulse parameters are the same as given in the caption of Fig. 2.

Image of FIG. 4.
FIG. 4.

Temporal dependence of the excited state populations and the normalized excited populations for the , , , , and transitions in the fundamental (1,0) Raman band of . The collisional dephasing rate and the pump and Stokes pulse parameters are the same as given in the caption of Fig. 2.

Image of FIG. 5.
FIG. 5.

Response of the Raman transition to excitation at two different irradiance levels. The real and imaginary components and the magnitude of the induced Raman coherence are plotted in (a) and (b) for peak pump and Stokes irradiances of and , respectively. The normalized excited level population is plotted in (c) and (d) for peak pump and Stokes irradiances of and , respectively. The transition frequency is , and the difference between the central frequencies of the pump and Stokes lasers is . All resonance and laser parameters are the same as listed in the caption of Fig. 2 except for the peak irradiances for the pump and Stokes pulses.

Image of FIG. 6.
FIG. 6.

Comparison of the results from the measurement of the FWM signal as a function of probe delay and DNI theoretical calculations for room air. For the experiment, the pump, Stokes, and probe pulse energies were 10, 100, and , respectively. The measured pulse widths were approximately . For the calculations, the peak irradiances for the pump, Stokes, and probe beams were , , and , respectively, corresponding to an estimated focal diameter for each beam. The collisional dephasing rate and the laser pulse parameters for the calculations are the same as given in the caption of Fig. 2.

Image of FIG. 7.
FIG. 7.

Calculation of the CARS signal from and CARS plus nonresonant background signal from room air. The peak irradiances for the pump, Stokes, and probe beams were (a) , , and , respectively; (b) , , and , respectively; (c) , , and , respectively; (d) , , and , respectively; and (e) , , and , respectively. The collisional dephasing rate and the laser pulse parameters for the calculations are the same as given in the caption of Fig. 2.

Image of FIG. 8.
FIG. 8.

Normalized CARS signal from room air. The CARS signal for peak irradiances of is the base case. For each curve, the calculated CARS signal is divided by the peak CARS signal for the base case, and by the normalized peak irradiance product . The peak irradiance products for each curve are indicated in the legend. The collisional dephasing rate and the laser pulse parameters for the calculations are the same as given in the caption of Fig. 2.

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/content/aip/journal/jcp/127/4/10.1063/1.2751184
2007-07-31
2014-04-21
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions
http://aip.metastore.ingenta.com/content/aip/journal/jcp/127/4/10.1063/1.2751184
10.1063/1.2751184
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