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This study investigates the uncertainties associated with estimates of the long-range transport SO2 (LRT-SO2) flow rate calculated hourly using Geostationary Environment Monitoring Spectrometer (GEMS) synthetic radiances. These radiances were simulated over the Korean Peninsula and the surrounding regions using inputs from the GEOS-Chem model for January, April, July, and October 2016. The LRT-SO2 calculation method, which requires SO2 vertical column densities, wind data, and planetary boundary layer information, was used to quantify the effects of the SO2 slant column density (SCD) retrieval error and uncertainties in wind data on the accuracy of the LRT-SO2 estimates. The effects were estimated for simulations of three anthropogenic and three volcanic SO2 transport events. When there were no errors in the GEMS SO2 SCD and wind data, the average true LRT-SO2 flow rates (standard deviation) and those calculated for these events were 1.17 (± 0.44) and 1.21 (±0.44) Mg/h, respectively. However, the averages of the true LRT-SO2 flow rates and those calculated for the three anthropogenic (volcanic) SO2 events were 0.61 (1.17) and 0.64 (1.20) Mg/h, respectively, in the presence of GEMS SO2 SCD errors. In the presence of both errors in the GEMS SO2 SCD and wind data, the averages of the true LRT-SO2 flow rates and those calculated for the three anthropogenic (volcanic) SO2 events were 0.61 (1.17) and 0.61 (1.04) Mg/h, respectively. This corresponds to differences of 2.1% to 23.1% between the simulated and true mean LRT-SO2 flow rates. The mean correlation coefficient (R), intercept, and slope between the true and simulated LRT-SO2 flow rates were 0.51, 0.43, and 0.45 for the six simulated events, respectively. This study demonstrates that SO2 SCD accuracy is an important factor in improving estimates of LRT-SO2 flow rates.

We investigate the effects of aerosol peak height (APH) and various parameters on the air mass factor (AMF) for SO2 retrieval. Increasing aerosol optical depth (AOD) leads to multiple scattering within the planetary boundary layer (PBL) and an increase in PBL SO2 AMF. However, under high AOD conditions, aerosol shielding effects dominate, which causes the PBL SO2 AMF to decrease with increasing AOD. The height of the SO2 layer and the APH are found to significantly influence the PBL SO2 AMF under high AOD conditions. When the SO2 and aerosol layers are of the same height, aerosol multiple scattering occurs dominantly within the PBL, which leads to an increase in the PBL SO2 AMF. When the APH is greater than the SO2 layer height, aerosol shielding effects dominate, which decreases the PBL SO2 AMF. When the SO2 and aerosol layers are of the same height under low AOD and solar zenith angle (SZA) conditions, increased surface reflectance is found to significantly increase the PBL SO2 AMF. However, high AOD dominates the surface reflectance contribution to PBL SO2 AMF. Under high SZA conditions, Rayleigh scattering contributes to a reduction in the light path length and PBL SO2 AMF. For volcanic SO2 AMF, high SZA enhances the light path length within the volcanic SO2 layer, as well as the volcanic SO2 AMF, because of the negligible photon loss by Rayleigh scattering at high altitudes. High aerosol loading and an APH that is greater than the SO2 peak height lead to aerosol shielding effects, which reduce the volcanic SO2 AMF. The SO2 AMF errors are also quantified as a function of uncertainty in the input data of AOD, APH, and surface reflectance. The SO2 AMF sensitivities and error analysis provided here can be used to develop effective error reduction strategies for satellite-based SO2 retrievals.

In the present study, we investigate the effects of signal to noise (SNR), slit function (FWHM), and aerosol optical depth (AOD) on the accuracy of formaldehyde (HCHO) vertical column density (HCHOVCD) using the ground-based direct-sun synthetic radiance based on differential optical absorption spectroscopy (DOAS). We found that the effect of SNR on HCHO retrieval accuracy is larger than those of FWHM and AOD. When SNR = 650 (1300), FWHM = 0.6, and AOD = 0.2, the absolute percentage difference (APD) between the true HCHOVCD values and those retrieved ranges from 54 (30%) to 5% (1%) for the HCHOVCD of 5.0 × 1015 and 1.1 × 1017 molecules cm−2, respectively. Interestingly, the maximum AOD effect on the HCHO accuracy was found for the HCHOVCD of 3.0 × 1016 molecules cm−2. In addition, we carried out the first ground-based direct-sun measurements in the ultraviolet (UV) wavelength range to retrieve the HCHOVCD using Pandora in Seoul. The HCHOVCD was low at 12:00 p.m. local time (LT) in all seasons, whereas it was high in the morning (10:00 a.m. LT) and late afternoon (4:00 p.m. LT), except in winter. The maximum HCHOVCD values were 2.68 × 1016, 3.19 × 1016, 2.00 × 1016, and 1.63 × 1016 molecules cm−2 at 10:00 a.m. LT in spring, 10:00 a.m. LT in summer, 1:00 p.m. LT in autumn, and 9:00 a.m. LT in winter, respectively. The minimum values of Pandora HCHOVCD were 1.63 × 1016, 2.23 × 1016, 1.26 × 1016, and 0.82 × 1016 molecules cm−2 at around 1:45 p.m. LT in spring, summer, autumn, and winter, respectively. This seasonal pattern of high values in summer and low values in winter implies that photo-oxidation plays an important role in HCHO production. The correlation coefficient (R) between the monthly HCHOVCD values from Pandora and those from the Ozone Monitoring Instrument (OMI) is 0.61, and the slope is 1.25.

Surface NO2 volume mixing ratio (VMR) at a specific time (13:45 Local time) (NO2 VMRST) and monthly mean surface NO2 VMR (NO2 VMRM) are estimated for the first time using three regression models with Ozone Monitoring Instrument (OMI) data in four metropolitan cities in South Korea: Seoul, Gyeonggi, Daejeon, and Gwangju. Relationships between the surface NO2 VMR obtained from in situ measurements (NO2 VMRIn-situ) and tropospheric NO2 vertical column density obtained from OMI from 2007 to 2013 were developed using regression models that also include boundary layer height (BLH) from Atmospheric Infrared Sounder (AIRS) and surface pressure, temperature, dew point, and wind speed and direction. The performance of the regression models is evaluated via comparison with the NO2 VMRIn-situ for two validation years (2006 and 2014). Of the three regression models, a multiple regression model shows the best performance in estimating NO2 VMRST and NO2 VMRM. In the validation period, the average correlation coefficient (R), slope, mean bias (MB), mean absolute error (MAE), root mean square error (RMSE), and percent difference between NO2 VMRIn-situ and NO2 VMRST estimated by the multiple regression model are 0.66, 0.41, −1.36 ppbv, 6.89 ppbv, 8.98 ppbv, and 31.50%, respectively, while the average corresponding values for the other two models are 0.75, 0.41, −1.40 ppbv, 3.59 ppbv, 4.72 ppbv, and 16.59%, respectively. All three models have similar performance for NO2 VMRM, with average R, slope, MB, MAE, RMSE, and percent difference between NO2 VMRIn-situ and NO2 VMRM of 0.74, 0.49, −1.90 ppbv, 3.93 ppbv, 5.05 ppbv, and 18.76%, respectively.

Surface NO2 volume mixing ratio (VMR) at a specific time (13:45 Local time) (NO2 VMRST) and monthly mean surface NO2 VMR (NO2 VMRM) are estimated for the first time using three regression models with Ozone Monitoring Instrument (OMI) data in four metropolitan cities in South Korea: Seoul, Gyeonggi, Daejeon, and Gwangju. Relationships between the surface NO2 VMR obtained from in situ measurements (NO2 VMRIn-situ) and tropospheric NO2 vertical column density obtained from OMI from 2007 to 2013 were developed using regression models that also include boundary layer height (BLH) from Atmospheric Infrared Sounder (AIRS) and surface pressure, temperature, dew point, and wind speed and direction. The performance of the regression models is evaluated via comparison with the NO2 VMRIn-situ for two validation years (2006 and 2014). Of the three regression models, a multiple regression model shows the best performance in estimating NO2 VMRST and NO2 VMRM. In the validation period, the average correlation coefficient (R), slope, mean bias (MB), mean absolute error (MAE), root mean square error (RMSE), and percent difference between NO2 VMRIn-situ and NO2 VMRST estimated by the multiple regression model are 0.66, 0.41, -1.36 ppbv, 6.89 ppbv, 8.98 ppbv, and 31.50%, respectively, while the average corresponding values for the other two models are 0.75, 0.41, -1.40 ppbv, 3.59 ppbv, 4.72 ppbv, and 16.59%, respectively. All three models have similar performance for NO2 VMRM, with average R, slope, MB, MAE, RMSE, and percent difference between NO2 VMRIn-situ and NO2 VMRM of 0.74, 0.49, -1.90 ppbv, 3.93 ppbv, 5.05 ppbv, and 18.76%, respectively. [ABSTRACT FROM AUTHOR]