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We have studied the effect on 2nd harmonic wavelength modulation spectroscopy of the use of integrating spheres as multipass gas cells. The gas lineshape becomes distorted at high concentrations, as a consequence of the exponential pathlength distribution of the sphere, introducing nonlinearity beyond that expected from the Beer-Lambert law. We have modelled this numerically for methane absorption at 1.651μm, with gas concentrations in the range of 0-2.5%vol in air. The results of this model compare well with experimental measurements. The nonlinearity for the 2f WMS measurements is larger than that for direct scan measurements; if this additional effect were not accounted for, the resulting error would be approximately 20% of the reading at a concentration of 2.5 %vol methane

Using integrating spheres with wavelength modulation spectroscopy: effect of pathlength distribution on 2nd harmonic signals