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Molecular Crystals and Liquid Crystals Incorporating Nonlinear Optics

3-Beam Degenerate 4-Wave Mixing Using Incoherent Light

X. Cheng, Takayoshi Kobayashi

Published May 1, 1990• 2 citations
Publisher

Abstract

Signal intensity as a function of mutual delay time of three incoherent pump beams in the degenerate four-wave mixing (DFWM) process has been calculated with the second-order correlation time of the fields being much shorter than both the dephasing time T 2 and the inverse of the inhomogeneous broadening width δω. The results show that when broadening is purely homogeneous and extremely inhomogeneous, the curve of the DFWM signal intensity as a function of the delay time τ shows no peak shift, while when the inhomogeneous broadening is finite, the peak shift is related to the dephasing time T 2 and the inhomogeneous width δω, and can thus be used to estimate T 2.

DOI
10.1080/00268949008047795

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MULTILEVEL THEORY OF TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT——INHOMO-GENEOUS BROADENING CASE

ZHANG RUI-HUA, Xin Mi, ZHOU HAI-TIAN +3 more

In this paper, our multi-level theory of time-delay four wave mixing with incoherent light (TDFWM-IL) developed previously for the case of homogeneous broadening system has been extended to a generally inhomogeneous broadening case. From the present theory, a general expression of signal intensity for absorption band with both homogeneous and inhomogeneous broadening is given as a function of mutual time delay τ between two pump beams. Photon echo with incoherent light under the condition of extremely inhomogeneous broadening is discussed, and the difference of results obtained scperately from multi-level and two-level theory is pointed out. It has been demonstrated that the experiment of TDFWM-IL can also be analysed approximately by using an effective two-level model when a weak effect of inhomogeneous broadening of absorption band exists. Finally, our experimental results of TDFWM-IL obtained at zero-phonon line of ruby and absorption edge of cresyl violet film in PMMA are also presented and compared with the theory mentioned above.

Acta Physica Sinica•Jan 1, 1991•0 citations

STUDY OF TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT IN ABSORPTION BANDS I: Theory

Peixian Ye, Ruihua Zhang, Xin Mi +2 more

A multilevel model, including homogeneous and inhomogeneous broadening, is proposed for the study of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands consisting of a series of vibrational transitions. A theory of TDFWM-IL is developed for this model, and a general formula for the delay-time dependence of the signal intensity Is(τ), considering both the homogeneous and inhomogeneous broadening of the transitions, is deduced. Special analyses are given to the homogeneous and inhomogeneous limits. The differences between Is(τ) derived from multilevel theory and from two-level theory, are pointed out. When the homogeneous broadening of individual transitions is much smaller than the frequency interval of adjacent transitions, Is(τ) in the multilevel theory is modulated periodically and the envelope is close to that in the two-level theory for both the homogeneous and inhomogeneous limits. When the individual transitions are homogeneously broadened enough so that an unresolved continuous band is formed, an effective two-level model can still be used approximately for the studies of TDFWM-IL in this continuous band, with both homogeneous and inhomogeneous broadening. However, the dephasing time [Formula: see text] in the formula of Is(τ) in this effective two-level model is not the real dephasing time of an individual transition of the band, but the effective one which reflects the behavior of the whole band.

Journal of Nonlinear Optical Physics & Materials•Apr 1, 1992•3 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

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

Interference effects in time-delayed degenerate four-wave mixing with broadband noisy light

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Journal of the Optical Society of America B•Jun 1, 2000•11 citations

Theoretical study of ultrafast dephasing by four-wave mixing

Claudine Katan, J. P. Lavoine, A. A. Villaeys

Microscopic dynamics. of materials can be studied by time delayed four-wave mixing spectroscopy. Dephasing constants can be measured by such experiments. Experimental results are easily analysed when the correlation time r of the exciting electric field is much shorter than the dephasing time ''2 However when these quantities are on the same time scale numerical fits are necessary. In the present work we analysed theoretically a time delayed four-wave mixing experiment. The material is described by an ensemble of two-level systems and a large inhomogeneous broadening is assumed. Using the third order term of the density matrix we establish a relation between 1''2 -r and ''Tm the time delay for which the maximum of the diffracted light intensity is observed. The conditions to obtain an estimate of T2 from the measurement of Tm are discussed.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 1, 1991•0 citations
Signal intensity as a function of mutual delay time of three incoherent pump beams in the degenerate four-wave mixing (DFWM) process has been calculated with the second-order correlation time of the fields being much shorter than both the dephasing time T 2 and the inverse of the inhomogeneous broadening width δω. The results show that when broadening is purely homogeneous and extremely inhomogeneous, the curve of the DFWM signal intensity as a function of the delay time τ shows no peak shift, while when the inhomogeneous broadening is finite, the peak shift is related to the dephasing time T 2 and the inhomogeneous width δω, and can thus be used to estimate T 2.
In this paper, our multi-level theory of time-delay four wave mixing with incoherent light (TDFWM-IL) developed previously for the case of homogeneous broadening system has been extended to a generally inhomogeneous broadening case. From the present theory, a general expression of signal intensity for absorption band with both homogeneous and inhomogeneous broadening is given as a function of mutual time delay τ between two pump beams. Photon echo with incoherent light under the condition of extremely inhomogeneous broadening is discussed, and the difference of results obtained scperately from multi-level and two-level theory is pointed out. It has been demonstrated that the experiment of TDFWM-IL can also be analysed approximately by using an effective two-level model when a weak effect of inhomogeneous broadening of absorption band exists. Finally, our experimental results of TDFWM-IL obtained at zero-phonon line of ruby and absorption edge of cresyl violet film in PMMA are also presented and compared with the theory mentioned above.
A multilevel model, including homogeneous and inhomogeneous broadening, is proposed for the study of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands consisting of a series of vibrational transitions. A theory of TDFWM-IL is developed for this model, and a general formula for the delay-time dependence of the signal intensity Is(τ), considering both the homogeneous and inhomogeneous broadening of the transitions, is deduced. Special analyses are given to the homogeneous and inhomogeneous limits. The differences between Is(τ) derived from multilevel theory and from two-level theory, are pointed out. When the homogeneous broadening of individual transitions is much smaller than the frequency interval of adjacent transitions, Is(τ) in the multilevel theory is modulated periodically and the envelope is close to that in the two-level theory for both the homogeneous and inhomogeneous limits. When the individual transitions are homogeneously broadened enough so that an unresolved continuous band is formed, an effective two-level model can still be used approximately for the studies of TDFWM-IL in this continuous band, with both homogeneous and inhomogeneous broadening. However, the dephasing time [Formula: see text] in the formula of Is(τ) in this effective two-level model is not the real dephasing time of an individual transition of the band, but the effective one which reflects the behavior of the whole band.
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 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.
Microscopic dynamics. of materials can be studied by time delayed four-wave mixing spectroscopy. Dephasing constants can be measured by such experiments. Experimental results are easily analysed when the correlation time r of the exciting electric field is much shorter than the dephasing time ''2 However when these quantities are on the same time scale numerical fits are necessary. In the present work we analysed theoretically a time delayed four-wave mixing experiment. The material is described by an ensemble of two-level systems and a large inhomogeneous broadening is assumed. Using the third order term of the density matrix we establish a relation between 1''2 -r and ''Tm the time delay for which the maximum of the diffracted light intensity is observed. The conditions to obtain an estimate of T2 from the measurement of Tm are discussed.