ALBERT

Description: Water vapor vertical profiles are important in numerical weather prediction, moisture transport, and vertical flux calculation. This study presents the Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) retrieval algorithm for water vapor vertical profiles and the retrieved results are validated with corresponding independent datasets under clear sky. The retrieved Vertical Column Densities (VCDs) and surface concentrations are validated with the Aerosol Robotic Network (AERONET) and National Climatic Data Centre (NCDC) datasets, achieving good correlation coefficients (R) of 0.922 and 0.876, respectively. The retrieved vertical profiles agree well with weekly balloon-borne radiosonde measurements. Furthermore, the retrieved water vapor concentrations at different altitudes (100–2000 m) are validated with the corresponding European Centre for Medium-range Weather Forecasts (ECMWF) ERA-interim datasets, achieving a correlation coefficient (R) varying from 0.695 to 0.857. The total error budgets for the surface concentrations and VCDs are 31% and 38%, respectively. Finally, the retrieval performance of the MAX-DOAS algorithm under different aerosol loads is evaluated. High aerosol loads obstruct the retrieval of surface concentrations and VCDs, with surface concentrations more liable to severe interference from such aerosol loads. To summarize, the feasibility of detecting water vapor profiles using MAX-DOAS under clear sky is confirmed in this work.

Description: The differential optical absorption spectroscopy (DOAS) method is a well-known remote sensing technique that is nowadays widely used for measurements of atmospheric trace gases, creating the need for harmonization and characterization efforts. In this study, an intercomparison exercise of DOAS retrieval codes from 17 international groups is presented, focusing on NO2 slant columns. The study is based on data collected by one instrument during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. As data from the same instrument are used by all groups, the results are free of biases due to instrumental differences, which is in contrast to previous intercomparison exercises.While in general an excellent correlation of NO2 slant columns between groups of  〉  99.98 % (noon reference fits) and  〉  99.2 % (sequential reference fits) for all elevation angles is found, differences between individual retrievals are as large as 8 % for NO2 slant columns and 100 % for rms residuals in small elevation angles above the horizon.Comprehensive sensitivity studies revealed that absolute slant column differences result predominantly from the choice of the reference spectrum while relative differences originate from the numerical approach for solving the DOAS equation as well as the treatment of the slit function. Furthermore, differences in the implementation of the intensity offset correction were found to produce disagreements for measurements close to sunrise (8–10 % for NO2, 80 % for rms residual). The largest effect of  ≈  8 % difference in NO2 was found to arise from the reference treatment; in particular for fits using a sequential reference. In terms of rms fit residual, the reference treatment has only a minor impact. In contrast, the wavelength calibration as well as the intensity offset correction were found to have the largest impact (up to 80 %) on rms residual while having only a minor impact on retrieved NO2 slant columns.

Description: In this paper, we present ship-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric trace gases' distribution along the Yangtze River during winter 2015. The measurements were performed along the Yangtze River between Shanghai and Wuhan, covering major industrial areas in eastern China. Tropospheric vertical column densities (VCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved using the air mass factor calculated by the radiative transfer model. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. In addition, spatial distributions of atmospheric pollutants are strongly affected by meteorological conditions; i.e., positive correlations were found between concentration of pollutants and wind speed over these areas, indicating strong influence of transportation of pollutants from high-emission upwind areas along the Yangtze River. Comparison of tropospheric NO2 VCDs between ship-based MAX-DOAS and Ozone Monitoring Instrument (OMI) satellite observations shows good agreement with each other, with a Pearson correlation coefficient (R) of 0.82. In this study, the NO2 ∕ SO2 ratio was used to estimate the relative contributions of industrial sources and vehicle emissions to ambient NO2 levels. Analysis results of the NO2 ∕ SO2 ratio show a higher contribution of industrial NO2 emissions in Jiangsu Province, while NO2 levels in Jiangxi and Hubei provinces are mainly related to vehicle emissions. These results indicate that different pollution control strategies should be applied in different provinces. In addition, multiple linear regression analysis of ambient carbon monoxide (CO) and odd oxygen (Ox) indicated that the primary emission and secondary formation of HCHO contribute 54.4 ± 3.7 % and 39.3 ± 4.3 % to the ambient HCHO, respectively. The largest contribution from primary emissions in winter suggested that photochemically induced secondary formation of HCHO is reduced due to lower solar irradiance in winter. Our findings provide an improved understanding of major pollution sources along the eastern part of the Yangtze River which are useful for designing specific air pollution control policies.

Description: Glyoxal (CHOCHO) and formaldehyde (HCHO) trace gases were successfully retrieved from a multi-axis differential optical absorption spectroscopy (MAX-DOAS) system in Beijing (39.95°N, 116.32°E) and Baoding (39.15°N, 115.40°E), China. The measurements of these trace gases span the period from May 2017 to April 2018. Higher levels of trace gases were observed in Beijing most likely due to increased transport and industrial activities compared to Baoding. Different time scales were analyzed from seasonal to daily levels. Seasonal variation categorized by wintertime maximum and summertime minimum was observed for CHOCHO, while for HCHO maximum values were recorded during summer at both observation points. Variations in the diurnal cycle of trace gases were examined. The results are consistent with strong links to photo-oxidations of VOCs for HCHO production, whereas the CHOCHO diurnal variation can be related to anthropogenic effects in the evening. Weekends didn’t have any significant effect on both HCHO and CHOCHO. We investigated the temperature dependency of HCHO and CHOCHO. HCHO shows positive correlation with air temperature, which strengthened the argument that HCHO production is linked to photo-oxidation of VOCs. CHOCHO is anti-correlated with air temperature. This suggests that photolysis is a major sink for CHOCHO in Beijing and Baoding. We also investigated the relationship between CHOCHO and HCHO VCDs with enhanced vegetation index (EVI) data obtained from MODIS, which represents a direct relation with biogenic emissions. The positive correlations were observed among monthly mean HCHO VCDs and monthly mean EVI at both monitoring stations. The strong correlation of HCHO with EVI found, suggests that oxidation of isoprene and HCHO production is strongly related, while negative correlation was observed among CHOCHO VCDs and EVI.

Description: In this paper, we present ship-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric trace gases distribution along Yangtze River during winter 2015. The measurements were performed along Yangtze River between Shanghai and Wuhan covering major industrial areas in eastern China. Tropospheric vertical column densities (VCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved using air mass factor calculated by radiative transfer model. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over Yangtze River. In addition, spatial distributions of atmospheric pollutants are strongly affected by meteorological conditions, i.e., positive correlations were found between concentration of pollutants and wind speed over these areas indicating strong influence of transportation of pollutants from high-emission upwind areas along Yangtze River. Comparison of tropospheric NO2 VCDs between ship-based MAX-DOAS and OMI satellite observations shows good agreement with each other with Pearson correlation coefficient (R) of 0.82. In this study, NO2/SO2 ratio was used to estimate the relative contributions of industrial sources and vehicle emissions to ambient NO2 levels. Analysis results of NO2/SO2 ratio shows that higher contribution of industrial NO2 emissions in Jiangsu province, while NO2 levels in Jiangxi and Hubei provinces are mainly related to vehicle emissions. These results indicate that different pollution control strategies should be applied in different provinces. In addition, multiple linear regression analysis of ambient carbon monoxide (CO) and odd oxygen (Ox) indicated that the primary emission and secondary formation of HCHO contribute 54.4 ± 3.7 % and 39.3 ± 4.3 % to the ambient HCHO, respectively. The largest contribution from primary emissions in winter suggested that photochemically induced secondary formation of HCHO is reduced due to lower solar irradiance in winter. Our findings provide an improved understanding of major pollution sources along the eastern part of Yangtze River which are useful for designing specific air pollution control policies.

Description: Long-term continuous measurements of speciated atmospheric mercury were conducted at Hefei, a mid-latitude inland city in east central China, from July 2013 to June 2014. The mean concentrations (± standard deviation) of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) were 3.95 ± 1.93 ng m−3, 2.49 ± 2.41 pg m−3 and 23.3 ± 90.8 pg m−3, respectively, during non-haze days, and 4.74 ± 1.62 ng m−3, 4.32 ± 8.36 pg m−3 and 60.2 ± 131.4 pg m−3, respectively, during haze days. Potential source contribution function (PSCF) analysis suggested that the atmospheric mercury pollution during haze days was caused primarily by local mercury emissions, instead of via long-range mercury transport. In addition, the disadvantageous diffussion during haze days will also enhance the level of atmospheric mercury. Compared to the GEM and RGM, change in PBM was more sensitive to the haze pollution. The mean PBM concentration during haze days was 2.5 times that during non-haze days due to elevated concentrations of particulate matter. A remarkable seasonal trend in PBM was observed with concentration decreasing in the following order in response to the frequency of haze days: autumn, winter, spring, summer. A distinct diurnal relationship was found between GEM and RGM during haze days, with the peak values of RGM coinciding with the decline in GEM. Using HgOH as an intermediate product during GEM oxidation, our results suggest that NO2 aggregation with HgOH could explain the enhanced production of RGM during the daytime in haze days. Increasing level of NOx will potentially accelerate the oxidation of GEM despite the decrease of solar radiation.

Description: Long-term continuous measurements of speciated atmospheric mercury were conducted from July 2013 to June 2014 in Hefei, a midlatitude inland city in eastern central China that experiences frequent haze pollution. The mean concentrations (±standard deviation) of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particle-bound mercury (PBM) were 3.95 ± 1.93 ng m−3, 2.49 ± 2.41 and 23.3 ± 90.8 pg m−3, respectively, on non-haze days, and 4.74 ± 1.62 ng m−3, 4.32 ± 8.36 and 60.2 ± 131.4 pg m−3, respectively, on haze days. Potential source contribution function (PSCF) analysis suggested that atmospheric mercury pollution on haze days was caused primarily by local emissions, instead of via long-range transport. The poorer mixing conditions on haze days also favored the accumulation of atmospheric mercury. Compared to GEM and GOM, PBM was especially sensitive to haze pollution. The mean PBM concentration on haze days was 2.5 times that on non-haze days due to elevated concentrations of particulate matter. PBM also showed a clear seasonal trend; its concentration was the highest in fall and winter, decreased rapidly in spring and was the lowest in summer, following the same order in the frequency of haze days in different seasons. On both non-haze and haze days, GOM concentrations remained low at night, but increased rapidly just before sunrise, which could be due to diurnal variation in air exchange between the boundary layer and free troposphere. However, non-haze and haze days showed different trends in daytime GEM and GOM concentrations. On non-haze days, GEM and GOM declined synchronously through the afternoon, probably due to the retreat of the free tropospheric air as the height of the atmospheric boundary layer increases. In contrast, on haze days, GOM and GEM showed opposite trends with the highest GOM and lowest GEM observed in the afternoon, suggesting the occurrence of photochemical oxidation. This is supported by simple box-model calculations, which showed that oxidation of GEM to GOM does occur and that the transport of free tropospheric GOM alone is not large enough to account for the observed increase in daytime GOM. Our results further postulate that NO2 aggregation with the HgOH intermediate may be a potential mechanism for the enhanced production of GOM during daytime.

Description: The Differential Optical Absorption Spectroscopy (DOAS) method is a well-known remote sensing technique that is nowadays widely used for measurements of atmospheric trace gases, creating the need for harmonization and characterization efforts. In this study, an intercomparison exercise of DOAS retrieval codes from 17 international groups is presented focusing on NO2 slant columns. The study is based on data collected by one instrument during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. As data from the same instrument is used by all groups, the results are free of biases due to instrumental differences, which is in contrast to previous intercomparison exercises. While in general an excellent correlation of NO2 slant columns between groups of 〉 99.98 % (noon reference fits), and 〉 99.2 % (sequential reference fits) for all elevation angles is found, differences between individual retrievals are as large as 8 % for NO2 slant columns and 100 % for RMS residuals. Two kinds of disagreements were identified: (1) Absolute slant column differences were found to result predominantly from the choice of the reference spectrum. (2) Relative differences were found to originate from the numerical approach for solving the DOAS equation as well as the treatment of the slit function. Differences in the implementations of the intensity offset correction lead to disagreements for retrievals close to sunrise (8–10 % for NO2, 80 % for RMS residual). Apart from this, the largest effect of ≈ 8 % difference in NO2 was found to arise from the reference treatment, in particular for fits using a sequential reference. In terms of RMS fit residual, the reference treatment has only a minor impact. In contrast, the wavelength calibration as well as the intensity offset correction were found to have the largest impact (up to 80 %) on RMS residual while having only a minor impact on retrieved NO2 slant columns.