LAUSR

We studied resonantly enhanced third-harmonic generation, induced by midinfrared, spectrally narrow-band, nanosecond laser pulses tuned in the vicinity of rovibrational molecular resonances. As we drive the frequency conversion process simultaneously close to single-, two-, and three-photon resonances, we get strong resonance enhancements of the third-harmonic yield by several orders of magnitude. The experimental setup requires only a single midinfrared laser beamline; the signal wavelength is easily separable from the much longer driving laser wavelength. We performed extended, systematic studies on the third-harmonic yield, spectral line shape and linewidth with laser intensity, frequency, and pressure. We determined a detection limit of ${10}^{15}$ $\mathrm{molecules}/{\mathrm{cm}}^{3}$, which indicates the potential of the approach for realistic applications in trace gas detection.