Abstract. By combining tunable broadband pulse generation with nonlinear spectral compression, we demonstrate a prototype scheme for highly selective coherent standoff sensing of air molecules and discuss its coupling to the recently demonstrated backward atmospheric lasing.Many applications in environmental science and security call for standoff chemical identification of airborne pollutants by their signature molecular vibrations. Raman LIDARs, relying on the observation of incoherent wide-angle scattering, have limitations in their practicability. The success of heterodyne detection as a cornerstone concept of the existing coherent LIDAR approaches motivate the development of optical remote sensing schemes where the coherence would be used to provide a highly directional backward optical signal through stimulated Raman scattering, thus enhancing the sensitivity and selectivity of standoff detection. Coherently-enhanced Raman scattering processes, such as Coherent Anti-Stokes Raman Scattering (CARS) and Stimulated Raman Scattering (SRS), open the possibility of recording signals carried in a laser-like beam. Generation of a backward phase-matched Raman signal is simple in the presence of reflective or diffuse objects capable of bouncing the laser beam back. However, an observer who sends out a laser pulse to interrogate an optically transparent atmosphere has to find an alternative way of initiating a backward-propagating laser beam and to solve the problem of phase matching. The recent experimental demonstration of a remotely pumped atmospheric backward laser using O 2 (λ=845 nm) [1] or N 2 (λ=337 and 357 nm) [2] has sparked proposals for coherent standoff Raman spectroscopies [3].In this work we experimentally and theoretically investigate a prototype for SRS in air which will be ultimately based on the 337-nm atmospheric N 2 laser (Fig.1a). The interim model (Fig.1b) is based on a solid-state ultrafast laser system from which we derive a narrowband third harmonic Stokes pulse at ~340 nm, imitating the N 2 laser emission, and a synchronized tunable narrowband
EPJ Web of Conferences