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Four-wave mixing techniques have been used for the measurement of electronic transitions of cold transient species generated in a supersonic slit-jet discharge expansion. The origin band of the d(3)Pi(g)-a(3)Pi(u) system of C(2) and A(2)Pi(3/2)-X[combining tilde](2)Pi(3/2) electronic transition of HC(4)S were recorded. A signal-to-noise ratio of 10(4) in the spectra was achieved, resulting in detection limits of 10(10) cm(-3) for these two molecules. Application of selective two-color resonant four-wave mixing is used for the spectral assignment utilizing the double-resonance nature of the method. The combination of these techniques with a slit source proves to be a sensitive approach for the detection of transient molecules in a molecular beam discharge.

Degenerate four-wave mixing (DFWM) was used to record the spectra of charged and neutral carbon-containing radicals generated in a pulsed discharge source within a supersonic slit-jet expansion. Detection limits of approximately 10(9) molecules cm(-3) are achieved. The DFWM method allows a selective molecular detection by varying the discharge timings. Increased spectral selectivity is obtained by applying the two-color, doubly resonant four-wave mixing variant. This shows the potential of the techniques for sensitive and selective spectral analysis of radicals in discharges. The methods are successfully used for the detection of C(4)H, HC(2)S, and HC(4)H(+) with signal-to-noise in the range of 10(2)-10(4).

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