Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Degenerate four-wave mixing in a resonant homogeneously broadened system

Duncan G. Steel, Richard C. Lind, Jenny Lam

Published May 1, 1981• 49 citations
Publisher

Abstract

Detailed measurements have been made of degenerate four-wave mixing (DFWM) in a resonant homogeneously broadened gas. The measurements were performed in S${\mathrm{F}}_{6}$ using a pulsed C${\mathrm{O}}_{2}$ laser operated on the 10.4-\ensuremath{\mu} m branch. A pulse width of 1.2 nsec was used to reduce effects of collisional relaxation. Data are also presented for pulse widths of 140 nsec. At high-energy fluences (\ensuremath{\sim}0.1 J/${\mathrm{cm}}^{2}$) pulse breakup is observed and is believed to arise from multiple-photon effects. The data obtained with the short pulse width are compared to a four-level saturable-absorber model where excellent agreement is obtained when pump absorption is included. The qualitative behavior of DFWM due to dispersion is also demonstrated in the wings of the S${\mathrm{F}}_{6}$ absorption spectrum. Peak reflectivities of 38% were readily obtained. In addition contributions due to a coherent three-level nonlinearity are presented showing a contribution equal to the measured saturable contribution.

DOI
10.1103/physreva.23.2513

Related papers

Degenerate four-wave mixing spectroscopy with short-pulse lasers: theoretical analysis

Thomas A. Reichardt, Robert P. Lucht

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.

Journal of the Optical Society of America B•Dec 1, 1996•17 citations

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

Degenerate four-wave mixing with broad-bandwidth pulsed lasers

D. R. Meacher, A. Charlton, P. Ewart +2 more

The steady-state theory of degenerate four-wave mixing (DFWM) with broad-bandwidth lasers is extended to treat the time dependence of the interaction allowing calculation of the intensity dependence and saturation behavior of DFWM with pulsed lasers. An experimental study of this intensity dependence as a function of laser bandwidth is reported, showing qualitative agreement with the theory. The line shape of DFWM induced by broad-bandwidth pump fields, probed by a monochromatic probe, is shown to have a Doppler-broadened profile in agreement with the theoretical predictions.

Physical Review A•Sep 1, 1990•47 citations

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

Thomas A. Reichardt, Robert P. Lucht

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.

Journal of the Optical Society of America B•Jun 1, 1996•27 citations

Transient effects in degenerate four-wave mixing in saturable absorbers

Yaron R. Silberberg, I. Bar‐Joseph

The transient behavior of degenerate four-wave mixing (DFWM) in a three-level saturable absorber is analyzed and verified experimentally. A sharp peak of phase-conjugated reflectivity is predicted and observed at high pump intensities for pulsed beams. The influence of the time-dependent behavior of the conjugate wave signal on results of pulsed-beam experiments is studied. It is shown that transient effects could account for discrepancies between previous experimental results and steady-state theory.

IEEE Journal of Quantum Electronics•Sep 1, 1981•60 citations

Theory and measurement of degenerate four-wave mixing in a resonant three-level absorber

David E. Watkins, G. R. Phipps

The study of degenerate four-wave mixing (DFWM) in the doped alkali halide KCI:KReO4 was prompted by the observation that this material behaves like an ideal, homogeneously broadened two-level saturable absorber at CO2 laser wavelengths,1 for which a simple theory of DFWM exists.2

Conference on Lasers and Electro-Optics•Jan 1, 1982•0 citations
Detailed measurements have been made of degenerate four-wave mixing (DFWM) in a resonant homogeneously broadened gas. The measurements were performed in SF6{\mathrm{F}}_{6}F6​ using a pulsed CO2{\mathrm{O}}_{2}O2​ laser operated on the 10.4-\ensuremath{\mu} m branch. A pulse width of 1.2 nsec was used to reduce effects of collisional relaxation. Data are also presented for pulse widths of 140 nsec. At high-energy fluences (\ensuremath{\sim}0.1 J/cm2{\mathrm{cm}}^{2}cm2) pulse breakup is observed and is believed to arise from multiple-photon effects. The data obtained with the short pulse width are compared to a four-level saturable-absorber model where excellent agreement is obtained when pump absorption is included. The qualitative behavior of DFWM due to dispersion is also demonstrated in the wings of the SF6{\mathrm{F}}_{6}F6​ absorption spectrum. Peak reflectivities of 38% were readily obtained. In addition contributions due to a coherent three-level nonlinearity are presented showing a contribution equal to the measured saturable contribution.
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.
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 steady-state theory of degenerate four-wave mixing (DFWM) with broad-bandwidth lasers is extended to treat the time dependence of the interaction allowing calculation of the intensity dependence and saturation behavior of DFWM with pulsed lasers. An experimental study of this intensity dependence as a function of laser bandwidth is reported, showing qualitative agreement with the theory. The line shape of DFWM induced by broad-bandwidth pump fields, probed by a monochromatic probe, is shown to have a Doppler-broadened profile in agreement with the theoretical predictions.
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.
The transient behavior of degenerate four-wave mixing (DFWM) in a three-level saturable absorber is analyzed and verified experimentally. A sharp peak of phase-conjugated reflectivity is predicted and observed at high pump intensities for pulsed beams. The influence of the time-dependent behavior of the conjugate wave signal on results of pulsed-beam experiments is studied. It is shown that transient effects could account for discrepancies between previous experimental results and steady-state theory.