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Physical Review A

Sensitive detection of sodium in a flame using parametric four-wave mixing and seeded parametric four-wave mixing

Mark J. Fernée, P. F. Barker, Alan E. W. Knight, Halina H. Rubinsztein-Dunlop

Published Apr 1, 1998• 0 citations
Publisher

Abstract

Two-photon resonant parametric four-wave mixing and a newly developed variant called seeded parametric four-wave mixing are used to detect trace quantities of sodium in a flame. Both techniques are simple, requiring only a single laser to generate a signal beam at a different wavelength which propagates collinearly with the pump beam, allowing efficient signal recovery. A comparison of the two techniques reveals that seeded parametric four-wave mixing is more than two orders of magnitude more sensitive than parametric four-wave mixing, with an estimated detection sensitivity of $5\ifmmode\times\else\texttimes\fi{}{10}^{9}$ atoms/${\mathrm{cm}}^{3}$. Seeded parametric four-wave mixing is achieved by cascading two parametric four-wave mixing media such that one of the parametric fields generated in the first high-density medium is then used to ``seed'' the same four-wave mixing process in a second medium in order to increase the four-wave mixing gain. The behavior of this seeded parametric four-wave mixing is described using semiclassical perturbation theory. A simplified small-signal theory is found to model most of the data satisfactorily. However, an anomalous saturationlike behavior is observed in the large signal regime. The full perturbation treatment, which includes the competition between two different four-wave mixing processes coupled via the signal field, accounts for this apparently anomalous behavior.

DOI
10.1103/physreva.57.2802

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Two-photon resonant parametric four-wave mixing and a newly developed variant called seeded parametric four-wave mixing are used to detect trace quantities of sodium in a flame. Both techniques are simple, requiring only a single laser to generate a signal beam at a different wavelength which propagates collinearly with the pump beam, allowing efficient signal recovery. A comparison of the two techniques reveals that seeded parametric four-wave mixing is more than two orders of magnitude more sensitive than parametric four-wave mixing, with an estimated detection sensitivity of 5\ifmmode×\else\texttimes\fi1095\ifmmode\times\else\texttimes\fi{}{10}^{9}5\ifmmode×\else\texttimes\fi109 atoms/cm3{\mathrm{cm}}^{3}cm3. Seeded parametric four-wave mixing is achieved by cascading two parametric four-wave mixing media such that one of the parametric fields generated in the first high-density medium is then used to ``seed'' the same four-wave mixing process in a second medium in order to increase the four-wave mixing gain. The behavior of this seeded parametric four-wave mixing is described using semiclassical perturbation theory. A simplified small-signal theory is found to model most of the data satisfactorily. However, an anomalous saturationlike behavior is observed in the large signal regime. The full perturbation treatment, which includes the competition between two different four-wave mixing processes coupled via the signal field, accounts for this apparently anomalous behavior.
The nonlinear response of sodium vapor with a laser tuned near the 4D two-photon resonance is investigated over a large range of sodium concentrations and pump intensities with emphasis on the influence of coherent cancellation effects on the induced polarizations and the primary mechanism for the generation of the new frequencies. Over a wide range of circumstances, the response of the medium is dominated by parametric four-wave mixing as compared to amplified spontaneous emission or stimulated electronic hyper-Raman scattering. Secondary four-wave-mixing fields are generated by stimulated Raman scattering of one parametric four-wave-mixing field and a coupling of these fields with the driving laser field. A sharp onset of saturation of the parametric four-wave-mixing signals with sodium number density and a transition from a quadratic to a linear power dependence is observed. Both effects are explained in terms of the two-photon cancellation effect.
Study of a two-photon near resonant four wave difference mixing (FWDM) in Na in a CH4/air flame has been performed to understand the FWDM process reported by Singh and Yueh (1992). The FWDM signal was measured with reduced flame length and with the focal point at the center and also at one end of the flame to pinpoint the region in which the signal is generated. A partial contribution in the third peak was from the nonresonant background. A FWDM signal is generated slightly away from the focal point and nonresonant background, at the focal point in the present experimental conditions. An absorption spectrum of the Na D-lines at different dye laser energy was recorded to study the depletion of Na ground state at higher dye laser intensity. Comparative study of the FWDM signal with a narrow and broad bandwidth dye laser shows that a lower Na concentration detection limit could be achieved with a narrow linewidth probe laser tuned to about 9/cm lower frequency from the center of the D1 line. The two minima in the FWDM spectrum corresponding to Na D lines have been explained, qualitatively, with the saturation effect in the Na D-lines transition. 27 refs.
For the first time, we study the parametric amplification process of multi-wave mixing (PA-MWM) signal and cascaded-nonlinearity process (CNP) in sodium vapors both theoretically and experimentally, based on a conventional phase-conjugate MWM and a self-diffraction four-wave mixing (SD-FWM) processes, which are pumped by laser or amplified spontaneous emission (ASE), respectively. For laser pumping case, SD-FWM process serves as a quantum linear amplifier (a CNP) out (inside) of the resonant absorption region. While for ASE case, only the CNP occurs and the output linewidth is much narrower than that of the MWM signal due to the second selected effect of its electromagnetically induced transparency window. In addition, the phase-sensitive amplifying process seeded by two MWM processes is discussed for the first time. Theoretical fittings agree well with the experiment. The investigations have important potential applications in quantum communication.
We demonstrate an ultrafast parametric four-wave mixing method for the collisional-quenching-free detection of atomic hydrogen. Two photons of 243 nm light resonantly excite the n = 1 to n = 2 transition of atomic hydrogen, and a third probe photon scatters from the electronic coherence to generate the parametric emission of a degenerate signal photon. Laser-induced photofragmentation fluorescence from water, also excited with the same 243 nm pulses, is used as a convenient method to visualize beam overlap in space and time. The femtosecond time resolution enables the suppression of unwanted nonresonant contributions to the signal and separation from resonant mixing in water molecules because of the significantly different coherence lifetimes. A folded BOXCARS phase-matching configuration yields a spatially isolated, laser-like, signal beam, amenable to measurements in highly luminous backgrounds. Measurements in an H2/CH4/air flame demonstrate quantitative agreement with simulated H-atom concentration profiles. A coherence decay time constant of 42 ps is recorded in the atmospheric pressure flame.