Assessment of the impact of NO₂ contribution on aerosol-optical-depth measurements at several sites worldwide

Abstract

This work aims at investigating the effect of NO2 absorption on aerosol-optical-depth (AOD) measurements and Ångström exponent (AE) retrievals of sun photometers by the synergistic use of accurate NO2 characterization for optical-depth estimation from co-located ground-based measurements. The analysis was performed for ∼ 7 years (2017–2023) at several sites worldwide for the AOD measurements and AE retrievals by Aerosol Robotic Network (AERONET) sun photometers which use OMI (Ozone Monitoring Instrument) climatology for NO2 representation. The differences in AOD and AE retrievals by NO2 absorption are accounted for using high-frequency columnar NO2 measurements by a co-located Pandora spectroradiometer belonging to the Pandonia Global Network (PGN). NO2 absorption affects the AOD measurements in UV-Vis (visible) range, and we found that the AOD bias is the most affected at 380 nm by NO2 differences, followed by 440, 340, and 500 nm, respectively. AERONET AOD was found to be overestimated in half of the cases, while also underestimated in other cases as an impact of the NO2 difference from “real” (PGN NO2) values. Overestimations or underestimations are relatively low. About one-third of these stations showed a mean difference in NO2 and AOD (at 380 and 440 nm) above 0.5 × 10−4 mol m−2 and 0.002, respectively, which can be considered a systematic contribution to the uncertainties in the AOD measurements that are reported to be of the order of 0.01. However, under extreme NO2 loading scenarios (i.e. 10 % highest differences) at highly urbanized/industrialized locations, even higher AOD differences were observed that were at the limit of or higher than the reported 0.01 uncertainty in the AOD measurement. PGN NO2-based sensitivity analysis of AOD difference suggested that for PGN NO2 varying between 2 × 10−4 and 8 × 10−4 mol m−2, the median AOD differences were found to rise above 0.01 (even above 0.02) with the increase in NO2 threshold (i.e. the lower limit from 2 × 10−4 to 8 × 10−4 mol m−2). The AOD-derivative product, AE, was also affected by the NO2 correction (discrepancies between the AERONET OMI climatological representation of NO2 values and the real PGN NO2 measurements) on the spectral AOD. Normalized frequency distribution of AE (at 440–870 and 340–440 nm wavelength pair) was found to be narrower for a broader AOD distribution for some stations, and vice versa for other stations, and a higher relative error at the shorter wavelength (among the wavelength pairs used for AE estimation) led to a shift in the peak of the AE difference distribution towards a higher positive value, while a higher relative error at a lower wavelength shifted the AE difference distribution to a negative value for the AOD overestimation case, and vice versa for the AOD underestimation case. For rural locations, the mean NO2 differences were found to be mostly below 0.50 × 10−4 mol m−2, with the corresponding AOD differences being below 0.002, and in extreme NO2 loading scenarios, it went above this value and reached above 1.00 × 10−4 mol m−2 for some stations, leading to higher AOD differences but below 0.005. Finally, AOD and AE trends were calculated based on the original AERONET AOD (based on AERONET OMI climatological NO2), and its comparison with the mean differences in the AERONET and PGN NO2-corrected AOD was indicative of how NO2 correction could potentially affect realistic AOD trends.