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IEEE Journal of Quantum Electronics

Quantitative nonlinear spectroscopy: a direct comparison of degenerate four-wave mixing with cavity ring-down spectroscopy applied to NaH

Lucia Lehr, P. Hering

Published Jan 1, 1997• 21 citations

Abstract

Cavity ring-down spectroscopy and degenerate four-wave mixing have been applied for spectroscopic studies, temperature determination, and measurement of relative dipole transition moments of photochemically produced sodium hydride. In our experiment, NaH was formed within a heat-pipe oven after 3p excitation of sodium in a hydrogen atmosphere with a second dye laser. The reaction product NaH was probed in the near ultraviolet part of the spectrum at 382 nm with 1-4-/spl mu/s delay to the excitation pulse using both a linear and nonlinear spectroscopic technique with a pulsed dye laser source (pulsewidth 15-ns full-width half-maximum). The strengths and limitations of these two spectroscopic techniques are discussed. Since the two processes depend on different parameters and the image-forming beams have different properties, it is difficult to define a single criterion for comparison. But our measurements indicate that cavity ring-down spectroscopy is a powerful tool with a sensitivity better than 10/sup 9/ particles per cm/sup 3/ and quantum state which is comparable to degenerate four-wave mixing in our case.

DOI: 10.1109/3.622624

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Cavity ring-down spectroscopy and degenerate four-wave mixing have been applied for spectroscopic studies, temperature determination, and measurement of relative dipole transition moments of photochemically produced sodium hydride. In our experiment, NaH was formed within a heat-pipe oven after 3p excitation of sodium in a hydrogen atmosphere with a second dye laser. The reaction product NaH was probed in the near ultraviolet part of the spectrum at 382 nm with 1-4-/spl mu/s delay to the excitation pulse using both a linear and nonlinear spectroscopic technique with a pulsed dye laser source (pulsewidth 15-ns full-width half-maximum). The strengths and limitations of these two spectroscopic techniques are discussed. Since the two processes depend on different parameters and the image-forming beams have different properties, it is difficult to define a single criterion for comparison. But our measurements indicate that cavity ring-down spectroscopy is a powerful tool with a sensitivity better than 10/sup 9/ particles per cm/sup 3/ and quantum state which is comparable to degenerate four-wave mixing in our case.

Degenerate four-wave mixing (D4WM) is presented as a simple nonlinear laser method with spectral resolution high enough to resolve isotope/hyperfine lines and detection sensitivity sufficient for sub-ppb or sub-attomole detection in various atomizers and detection cells. Two counterpropagating pump beams and a probe beam are mixed inside the nonlinear medium that consists of analyte atomic or molecular species, and the phase conjugate signal beam is generated as the wavefront-reversed replica of the probe beam. Optical alignment is relatively simple, and optical signal collection is highly efficient since the signal is a laser beam. Continuous sample introduction is possible using an air-acetylene flame as the atomizer. When a relatively low-pressure demountable discharge cell is used as the atomizer, Lorentzian (pressure) broadening is also minimized in addition to cancellation of Doppler broadening. Degenerate four-wave mixing is also effective in detecting trace amounts of analytes in the condensed phase at room temperature using continuously flowing capillary cells that are suitable for interfacing to liquid chromatography and capillary electrophoresis. In addition to pulsed lasers, such as excimer- and Nd:YAG-pumped dye lasers, one can also use relatively low-power continuous-wave lasers such as argon-ion lasers or single-frequency ring dye lasers.

Degenerate four-wave mixing (DFWM) in excited atoms is investigated as a probe of the excited-state density produced by collision-assisted transitions. Sodium atoms are excited to the 3P state by absorption of light in the extreme blue wing of the D lines in the presence of He, Ne and Ar perturbers. The rare-gas pressure dependence of the DFWM signals, resonantly enhanced by the 3P-4D transition, is studied to determine the regime where the signals give an unambiguous measure of the excited-state (3P) density. The observed behaviour is compared with a simple model of DFWM in absorbing media. Good qualitative agreement is obtained and the results illustrate the role of absorption, saturation and finite laser bandwidth. The technique allows small excited-state densities ( approximately 10 9 cm -3 ) to be detected with good temporal and spatial resolution.

Degenerate four-wave mixing (DFWM) spectroscopy is a promising diagnostic technique [1-3], but significant questions remain regarding its application for quantitative concentration measurements in combustion environments with typical laser systems. In this paper we present a summary of two numerical investigations with the goal of quantifying the measurement technique for common experimental situations. Specifically, we investigate both (1) probing a degenerate-level (multistate) resonance with a single-mode laser and (2) probing a two-state resonance with a multimode laser. DFWM signal levels are calculated by solving the time-dependent density matrix equations using direct numerical integration (DNI) [4, 5] for a two or more level system interacting with three laser beams.

Accurate measurements were made of lasing and 4-wave mixing processes in Na-vapor inside a double heatpipe oven. Scanning Nd:YAG pumped pulsed dye laser through the two-photon resonance 3s{sup 2}S{sub 1/2} {yields} 5s{sup 2}S{sub 1/2}, and a high resolution double-monochromator near the 5s - 4p{sup 2}P{sub 1/2,3/2} single photon resonance, we easily distinguished the two lasing multiplets due to J = {1/2} and 3/2 populations emitting blue 330 nm light. We also observed two other components. By varying the laser polarization, intensity and Na density these were determined to be parametric 4-wave mixing lines with maximum intensity for slight phase mismatch. As the dye laser was scanned, the wavelengths of the lasing and 4-wave mixing peaks shifted, each pair with its own slope, and crossed - a process providing a spectroscopic pump mechanism to populate the {vert_bar}M{sub J} {>=}{vert_bar} + {1/2} > magnetic substate of the ground state. Similar experiments are underway for other 4 wave mixing processes.

The population of the 3P state in atomic sodium produced by absorption in the extreme blue wing of the D lines is measured by excited-state degenerate four-wave mixing (ESDFWM). The strength of this ESDFWM signal is shown to give a measure of the pressure-broadened extreme-wing absorption coefficient alpha ( omega ). Relative values of alpha ( omega ) for the rare gases He, Ne and Ar are measured and compared with values calculated from theoretical interatomic potentials and from extreme-wing emission data. Very good agreement is found demonstrating the ability of this nonlinear technique to make accurate measurements of small excited-state densities with excellent spatial and temporal resolution. Advantages of the method for other applications are briefly discussed.