Gas cells for tunable diode laser absorption spectroscopy employing optical diffusers. Part 2: Integrating spheres

We have studied the effects of random laser speckle and self-mixing interference on TDLS based gas measurements made using integrating spheres. Details of the theory and TDLS apparatus are given in Part 1 of this paper and applied here to integrating spheres. Experiments have been performed using two commercial integrating spheres with diameters of 50 mm and 100 mm for the detection of methane at 1651 nm. We have calculated the expected levels of laser speckle related uncertainty, considered to be the fundamental limiting noise, and imaged subjective laser speckle in a sphere using different sized apertures. For wavelength modulation spectroscopy, noise equivalent absorbances (NEAs) of around 5×10^?5 were demonstrated in both cases, corresponding to limits of detection of 1.2 ppm methane and 0.4 ppm methane respectively. Longer-term drift was found to be at an NEA of 4×10^?4. This lies within our broad range of expectations. For a direct spectral scan with no wavelength dither, a limit of detection of 75 ppm or fractional measured power uncertainty of 3×10^?3 corresponded well with our prediction for the objective speckle uncertainty.