Ozone detection by differential absorption spectroscopy at ambient pressure with a 9.6 μm pulsed quantum-cascade laser

We report direct absorption spectroscopic detection of ozone at ambient pressure with a pulsed, DFB quantum-cascade laser (QCL) tuned within 1044-1050 cm(-1) by temperature scanning. Wavelength calibration curves were derived from FTIR and CO2 spectra and interpreted with respect to the heat transfer from the heterostructure to the sink. The laser linewidth (similar to0.13 cm(-1) FWHM) was found to decrease with temperature, probably as a result of operation at constant current. Spurious spectral features due to baseline inaccuracies were successfully filtered out from the QCL O-3 spectra using differential absorption. Reference O-3 concentrations were obtained by applying the same method to UV spectra, simultaneously measured with a differential optical absorption spectrometer (DOAS). Column densities retrieved from QCL spectra are in fairly good agreement (+/-20%) with the DOAS values above 28 ppm m. The estimated QCL lowest detectable, absolute and differential absorptions, (7x10(-3) and 2x10(-3), respectively), entail effective detection limits of 14 and 25 ppm m, respectively. Ongoing improvements in the acquisition system should allow the achievement of detection limits at the level of commercial open-path DOAS systems (similar to2 ppm m) in the near future. Our results demonstrate the applicability of the differential absorption method to QCL spectroscopy at ambient pressure, and encourage its use for open path detection.