Single-shot, spatially-resolved stand-off detection of atomic hydrogen via backward lasing in flames

We report on an experimental demonstration of spatially-resolved detection of atomic hydrogen in flames using a single-ended configuration yielding 656-nm lasing in the backward direction upon 2-photon pumping with 205-nm femtosecond laser pulses. Spatial resolution is achieved by temporally-resolved detection of the backward lasing using a streak camera. The method is demonstrated in CH₄/O₂ flames; both in a setup consisting of two flames, with variable spacing between the flames, and in a single flame. Results from the two-flame experiment show that the backward lasing technique is able to determine changes in the separation between the flames as this distance was altered. By maximizing the temporal resolution of the streak camera, obtaining a highest spatial resolution of 1.65 mm, it is possible to resolve the hydrogen signal present in the two reaction zones in the single flame, where the separation between the reaction zones is ~2 mm. The lasing signal is strong enough to allow single-shot measurements. Results obtained by backward lasing are compared with 2-photon planar laser-induced fluorescence (LIF) images recorded with detection perpendicular to the laser beam path and the results from the two methods qualitatively agree. Although further studies are needed in order to extract quantitative hydrogen concentrations, the present results indicate great potential for spatially resolved single-ended measurements, which would constitute a very valuable asset for combustion diagnostics in intractable geometries with limited optical access. It appears feasible to extend the technique to detection of any species for which resonant two-photon-excited lasing effect has been observed, such as O, N, C, CO and NH₃.