Fourier-based approach to overcome anomalies in high-resolution spectra of vibrational CARS measurements of gases

In this work, we report on an unconventional experimental procedure useful for thermometric measurements on the basis of high-resolution vibrational coherent anti-Stokes Raman scattering (CARS) generated using conventional lasers. The high spectral dispersion of 0.02 cm-1/pixel is achieved by means of some specific spectral arrangements (single-mode pump laser and diffraction grating providing spectra at the sixth order) and is further strengthened by the use of a relay lens system mounted before the charge-coupled device camera. Surprisingly, at the high spectral dispersion of our measurements, a significant and persistent thermometric inaccuracy is observed. The effect arises from an inevitable spectral modulation of defined frequency hidden in the main CARS signal of the gas under study, and to secure a good thermometric evaluation, we describe a Fourier approach that is experimentally demonstrated for the typical nitrogen CARS spectrum measured at room temperature. Copyright © 2014 John Wiley & Sons, Ltd.