Recommendations for spectral fitting of SO2 from miniature multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements

Autor: Z. Y. W. Davis, R. McLaren
Jazyk: angličtina
Rok vydání: 2020
Předmět:
Zdroj: Atmospheric Measurement Techniques, Vol 13, Pp 3993-4008 (2020)
Druh dokumentu: article
ISSN: 1867-1381
1867-8548
DOI: 10.5194/amt-13-3993-2020
Popis: Fitting sulfur dioxide (SO2) differential slant column densities (dSCDs) from multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of scattered sunlight is challenging because actinic light intensity is low in the wavelength regions where the SO2 absorption features are strongest. SO2 dSCDs were fit with different wavelength windows (λlow to λhigh) from ambient measurements with calibration cells of 2.2×1017 and 2.2×1016 molec. cm−2 inserted in the light path at different viewing elevation angles using an Ocean Optics USB2000 spectrometer in a miniature MAX-DOAS instrument. SO2 dSCDs were the least accurate, and fit errors were highest for fitting windows with λlow λlow > 312 nm. The SO2 dSCDs also exhibited an inverse relationship with the depth of the differential features in the SO2 absorption cross section for fitting windows with λlow α=2∘) exhibited less accurate SO2 dSCDs for the same fitting windows compared with higher angles. The use of a 400 nm short-pass filter or a polynomial to account for stray light (the offset function) increased the accuracy of the SO2 dSCDs for many different fitting windows, decreased fit errors, and decreased the dSCDs' dependence on the depth of the SO2 differential absorption features. These results suggest that the radiance at shorter wavelengths was increased by stray light. The inaccuracies at lower fitting wavelengths were increased by stray light originating from light with λ > 400 nm. Deviation of the SO2 dSCD from the true value depended on the SO2 concentration for some fitting windows rather than exhibiting a consistent bias. Uncertainties in the SO2 dSCD reported by the fit algorithm were more than 50 % less than the true error for many windows, particularly for the measurements without the filter or offset function. For retrievals with the filter or offset function, increasing λhigh > 320 nm tended to decrease the reported fit uncertainty but did not increase the accuracy. Based on the results of this study, a short-pass filter and a fitting window of 307.5 λ SO2 SCDs from miniature MAX-DOAS measurements. If a filter is not available or conflicts with other species to be determined (e.g., NO2 or HCHO), the offset function should be enabled, and a fit window 307.5 λ
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