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Journal of the Optical Society of America B

Effect of Doppler broadening on quantitative concentration measurements with degenerate four-wave mixing spectroscopy

Thomas A. Reichardt, Robert P. Lucht

Published Jun 1, 1996• 27 citations
Publisher

Abstract

The effect of Doppler broadening on degenerate four-wave mixing (DFWM) signal intensities in the regime of high pump and probe laser intensities is investigated theoretically. DFWM reflectivities are calculated by solving the time-dependent density-matrix equations for a two-level system interacting with three laser fields. The density-matrix equations are integrated directly in the time domain on a grid of spatial locations along the phase-matching axis; the DFWM signal level is then calculated by summation of the polarization contribution (with the appropriate phase factor) from each of the spatial grid points. For the case in which the Doppler and the collisional linewidths are comparable, the DFWM reflectivity is found to be inversely proportional to the factor 1 + (bΔωD/ΔωC)2, where ΔωD is the Doppler width, ΔωC is the collisional width, and b is weakly dependent on the pump and the probe laser powers. We developed an analytical expression for the reflectivity of a line that is both collision and Doppler broadened by dividing the widely used Abrams and Lind expression for homogeneous reflectivity Rhom by the factor 1 + (bΔωD/ΔωC)2. This modified reflectivity expression is found to give accurate results for the DFWM reflectivity over a wide range of values for the ratio of Doppler to collisional width. With this modified Abrams–Lind expression, strategies for quantitative DFWM concentration measurements in flames and plasmas are proposed and analyzed. We conclude that, by selection of the appropriate rotational transition, a DFWM reflectivity that is directly proportional to the square of the total species number density can be obtained over a wide range of temperature for constant-laser-intensity spatial profile mapping in flames.

DOI
10.1364/josab.13.001107

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

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The present paper deals with a three-level model of interaction with three cross-polarized and co-propagating fields having the same frequency. The two pump waves have arbitrary intensities and the third one (the probe wave) is assumed to be non-saturating. Using the radiative renormalization method, density matrix equations are solved analytically. The forward degenerate four-wave mixing (FDFWM) signal is calculated under thermodynamic conditions where collisional and Doppler broadenings are comparable. The calculation also takes into account crossed-polarization effects. The FDFWM intensity is computed as a function of power densities and pressure. FDFWM experimental spectra of the - (0 - 0) band of OH obtained in a welding torch flame are compared to theoretical profiles. For incident laser intensities in the range of a few , a good agreement is obtained between calculated and experimental profiles. Discrepancies arise under stronger conditions of saturation, showing the limits of application of our model. However, because there is little virtue in using higher laser powers, the model should be extremely useful in practical applications. In particular, we demonstrate that the signal intensity is optimal and the pressure dependence is minimized when the saturation parameter is unity.

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We present a revision of the theory of finite laser bandwidth effects on degenerate four-wave mixing (DFWM) of Alber, Cooper, and Ewart (ACE) [Phys. Rev. A 31, 2344 (1985)]. The same model is used for intense, broad-bandwidth pump lasers interacting with a weak monochromatic probe in a medium composed of two-level atoms. The density-matrix equations describing the time evolution of the atomic polarization coupled to fluctuating fields are solved using an appropriate decorrelation approximation. A steady-state analytical solution is found for resonant and near-resonant DFWM, for intensities that do not saturate the medium. For more intense fields it is found to be necessary to form a more complicated set of differential equations for all products of the field and atomic density-matrix elements. The results show that as in the ACE theory, increasing the bandwidth b leads to an increased effective saturation intensity. However, we find the DFWM reflectivity scales as 1/${b}^{2}$ when the probe is monochromatic and not 1/b as in the ACE theory. Furthermore, the saturation behavior of nonresonant DFWM is found to differ from the predictions of ACE. Atomic motion effects are shown to yield a Doppler-broadened line shape and also to affect the saturation behavior of the signal.

Physical Review A•Nov 1, 1989•52 citations
The effect of Doppler broadening on degenerate four-wave mixing (DFWM) signal intensities in the regime of high pump and probe laser intensities is investigated theoretically. DFWM reflectivities are calculated by solving the time-dependent density-matrix equations for a two-level system interacting with three laser fields. The density-matrix equations are integrated directly in the time domain on a grid of spatial locations along the phase-matching axis; the DFWM signal level is then calculated by summation of the polarization contribution (with the appropriate phase factor) from each of the spatial grid points. For the case in which the Doppler and the collisional linewidths are comparable, the DFWM reflectivity is found to be inversely proportional to the factor 1 + (bΔωD/ΔωC)2, where ΔωD is the Doppler width, ΔωC is the collisional width, and b is weakly dependent on the pump and the probe laser powers. We developed an analytical expression for the reflectivity of a line that is both collision and Doppler broadened by dividing the widely used Abrams and Lind expression for homogeneous reflectivity Rhom by the factor 1 + (bΔωD/ΔωC)2. This modified reflectivity expression is found to give accurate results for the DFWM reflectivity over a wide range of values for the ratio of Doppler to collisional width. With this modified Abrams–Lind expression, strategies for quantitative DFWM concentration measurements in flames and plasmas are proposed and analyzed. We conclude that, by selection of the appropriate rotational transition, a DFWM reflectivity that is directly proportional to the square of the total species number density can be obtained over a wide range of temperature for constant-laser-intensity spatial profile mapping in flames.
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.
The use of picosecond lasers for degenerate four-wave mixing (DFWM) diagnostics of atmospheric pressure flames has been suggested as a means of overcoming the complicated collision-rate dependence of the DFWM signal in the nanosecond-laser pulse-length regime. In this paper DFWM spectroscopy in the regime in which the laser pulse length (τL) is less than the characteristic collisional time (τC) is investigated theoretically. DFWM signal levels for the phase-conjugate geometry (counterpropagating pump beams) are calculated by integration of the time-dependent density-matrix equations at numerous grid points along the phase-matching axis and by summing of the polarization contribution from each of these grid points. Both purely homogeneously broadened resonances and resonances that are both collision broadened and Doppler broadened are considered. DFWM signal generation for these two types of resonances in the fully transient regime (τL≪τC) is strikingly different. For a homogeneously broadened resonance, the DFWM signal persists long after the laser beam has passed through the medium. The decay rate of the DFWM signal is determined by the collision rate in the medium, and the integrated DFWM signal is still dependent on the collision rate even in this fully transient regime. However, when the Doppler broadening of the resonance is much greater than the collisional broadening, the DFWM signal decays with a fall time close to that of the laser pulse. For τL≪τC, we find that it is the laser spectral width, rather than the collisional width, that dictates the range of velocity groups with which the pulses effectively interact. The signal decays with a fall time close to that of the laser pulse because the excited velocity groups radiate out of phase with one another. In a medium in which the Doppler width is much greater than the collisional width, the DFWM reflectivity is independent of collision rate for τL≪τC, but the signal level is dependent on the Doppler width. Finally, we investigate the effect of different laser pulse lengths on reflectivity saturation curves for resonances with different levels of Doppler broadening.
Nowadays degenerate four wave mixing (DFWM) with forward geometry (FDFWM) has found increasing usage, for example, in the gas phase detection. In the fields of theoretical development of DFWM, most of the studies have been concentrated on the understanding of phase-conjugated DFWM. However, few theories have dealt with FDFWM. These models calculated the signal directly from the off-diagonal element of the density matrix by assuming optically thin medium. In the paper we obtain a theoretical model for FDFWM in Doppler broadened two-level absorbers including propagation effect and discuss the Doppler effect on the signal intensity and lineshape. Assuming that probe and signal field amplitudes are small compared with those of the pump fields and pump field amplitudes are constant in the interaction volume, we obtain the following coupled equations from the Maxwell equation using the slowly varying envelope approximation and the paraxial approximation.
The interaction of two closely spaced resonances in degenerate four-wave-mixing spectra is investigated theoretically. Degenerate four-wave-mixing spectra for the phase-conjugate geometry (counterpropagating pump beams) are calculated by integrating the time-dependent density-matrix equations at numerous grid points along the phase-matching axis and summing the polarization contribution from each of these grid points. Both purely homogeneously broadened resonances and resonances that are both collision and Doppler broadened are considered. The homogeneously broadened results are found to agree with the results of the widely used Abrams–Lind expression for the case of stationary absorbers exposed to a steady-state excitation. We examine the effects of power broadening, pressure broadening, transition dipole moment, and population on the spectra of two neighboring homogeneously broadened resonances. As the laser power is increased, the real parts of the resonance susceptibilities destructively interfere with each other in the region between the lines, resulting in a significant and persistent dip in reflectivity. When Doppler broadening is included in the calculations, similar interference effects are observed, although at first the interference dip begins to disappear until the homogeneous part of the line shapes is broadened significantly by saturation. Using this numerical approach, we obtain good agreement with experimental results of primarily Doppler-broadened neighboring resonances.
The present paper deals with a three-level model of interaction with three cross-polarized and co-propagating fields having the same frequency. The two pump waves have arbitrary intensities and the third one (the probe wave) is assumed to be non-saturating. Using the radiative renormalization method, density matrix equations are solved analytically. The forward degenerate four-wave mixing (FDFWM) signal is calculated under thermodynamic conditions where collisional and Doppler broadenings are comparable. The calculation also takes into account crossed-polarization effects. The FDFWM intensity is computed as a function of power densities and pressure. FDFWM experimental spectra of the - (0 - 0) band of OH obtained in a welding torch flame are compared to theoretical profiles. For incident laser intensities in the range of a few , a good agreement is obtained between calculated and experimental profiles. Discrepancies arise under stronger conditions of saturation, showing the limits of application of our model. However, because there is little virtue in using higher laser powers, the model should be extremely useful in practical applications. In particular, we demonstrate that the signal intensity is optimal and the pressure dependence is minimized when the saturation parameter is unity.
We present a revision of the theory of finite laser bandwidth effects on degenerate four-wave mixing (DFWM) of Alber, Cooper, and Ewart (ACE) [Phys. Rev. A 31, 2344 (1985)]. The same model is used for intense, broad-bandwidth pump lasers interacting with a weak monochromatic probe in a medium composed of two-level atoms. The density-matrix equations describing the time evolution of the atomic polarization coupled to fluctuating fields are solved using an appropriate decorrelation approximation. A steady-state analytical solution is found for resonant and near-resonant DFWM, for intensities that do not saturate the medium. For more intense fields it is found to be necessary to form a more complicated set of differential equations for all products of the field and atomic density-matrix elements. The results show that as in the ACE theory, increasing the bandwidth b leads to an increased effective saturation intensity. However, we find the DFWM reflectivity scales as 1/b2{b}^{2}b2 when the probe is monochromatic and not 1/b as in the ACE theory. Furthermore, the saturation behavior of nonresonant DFWM is found to differ from the predictions of ACE. Atomic motion effects are shown to yield a Doppler-broadened line shape and also to affect the saturation behavior of the signal.