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AIP conference proceedings

Field and pressure induced four-wave mixing line shapes

W. M. Schreiber, N. Chencinski, Alfred M. Levine, A. N. Weizmann, Yehiam Prior

Published Jan 1, 1988• 0 citations
Publisher
DOI
10.1063/1.37365

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Four-wave mixing line shapes in sodium

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A recently presented treatment of four-wave mixing for fields of arbitrary strength1 is applied to the 3S–3P transitions of sodium. The line shapes associated with ordinary resonances, and with both pressure-induced and field-induced extra resonances are investigated. In sodium, the two lower levels (g,t) are very close, i.e., their separation is 0.059 cm-1. Thus decays from the upper (k,j) levels to each of the lower levels are expected to contribute significantly. Also, contributions associated with (g,t) population exchange because of the close proximity of these states are incorporated. The influence of the decay pattern and of the respective values of the decay constants is studied, especially as compared to the line shapes that would result if all decays were dominantly to the ground state. Regions of enhancement for the more complex decay pattern are found for field-induced extra resonances. The relative effects of spontaneous decay (T1) and proper dephasing (T2) on the line shapes is examined. It is found that (T2) dominates for weak field conditions but that both contribute significantly for strong field situations.

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Saturation effects in gas-phase degenerate four-wave mixing spectroscopy: nonperturbative calculations

Robert P. Lucht, Roger L. Farrow, David J. Rakestraw

Saturation effects in gas-phase degenerate four-wave mixing (DFWM) are investigated for conditions of interest for diagnostic applications in flames and plasmas. In particular, the case in which Doppler and collisional broadening are comparable, as is often the case for flame species such as NO and OH, is investigated. DFWM line shapes and signal intensities are calculated nonperturbatively and compared with high-resolution laser measurements. In the nonperturbative calculations the time-dependent density-matrix equations for a two-level system interacting with three laser fields are integrated directly on a grid of spatial locations along the phase-matching axis. The electric-field amplitude for the DFWM signal is determined by multiplying the time-varying, laser-induced polarization at each grid point by the appropriate phase factor and then by summing over all grid points. The calculations are in excellent agreement with measurements of DFWM line shapes and signal intensities for NO in a buffer gas of He over a wide range of He pressure. Under saturation conditions the pressure dependence of the DFWM signal is reduced greatly compared with the unsaturated case. The signal level is still dependent on the ratio of pure dephasing to quenching collisions, even for saturation conditions. From the standpoint of minimal dependence on collisional processes it appears that operation with pump-laser intensities approximately equal to the saturation intensity is optimal. The dependence of the DFWM line shape and signal intensity on the ratio of probe to pump-laser intensity is also investigated.

Journal of the Optical Society of America B•Sep 1, 1993•75 citations
A recently presented treatment of four-wave mixing for fields of arbitrary strength1 is applied to the 3S–3P transitions of sodium. The line shapes associated with ordinary resonances, and with both pressure-induced and field-induced extra resonances are investigated. In sodium, the two lower levels (g,t) are very close, i.e., their separation is 0.059 cm-1. Thus decays from the upper (k,j) levels to each of the lower levels are expected to contribute significantly. Also, contributions associated with (g,t) population exchange because of the close proximity of these states are incorporated. The influence of the decay pattern and of the respective values of the decay constants is studied, especially as compared to the line shapes that would result if all decays were dominantly to the ground state. Regions of enhancement for the more complex decay pattern are found for field-induced extra resonances. The relative effects of spontaneous decay (T1) and proper dephasing (T2) on the line shapes is examined. It is found that (T2) dominates for weak field conditions but that both contribute significantly for strong field situations.
Saturation effects in gas-phase degenerate four-wave mixing (DFWM) are investigated for conditions of interest for diagnostic applications in flames and plasmas. In particular, the case in which Doppler and collisional broadening are comparable, as is often the case for flame species such as NO and OH, is investigated. DFWM line shapes and signal intensities are calculated nonperturbatively and compared with high-resolution laser measurements. In the nonperturbative calculations the time-dependent density-matrix equations for a two-level system interacting with three laser fields are integrated directly on a grid of spatial locations along the phase-matching axis. The electric-field amplitude for the DFWM signal is determined by multiplying the time-varying, laser-induced polarization at each grid point by the appropriate phase factor and then by summing over all grid points. The calculations are in excellent agreement with measurements of DFWM line shapes and signal intensities for NO in a buffer gas of He over a wide range of He pressure. Under saturation conditions the pressure dependence of the DFWM signal is reduced greatly compared with the unsaturated case. The signal level is still dependent on the ratio of pure dephasing to quenching collisions, even for saturation conditions. From the standpoint of minimal dependence on collisional processes it appears that operation with pump-laser intensities approximately equal to the saturation intensity is optimal. The dependence of the DFWM line shape and signal intensity on the ratio of probe to pump-laser intensity is also investigated.