ALBERT

Description: We present a new aerosol extinction profile retrieval algorithm for multi-axis differential optical absorption spectrometer (MAX-DOAS) measurements at high-altitude sites. The algorithm is based on the lookup table method. It is applied to retrieve aerosol extinction profiles from the long-term MAX-DOAS measurements (February 2012 to February 2016) at the Environmental Research Station Schneefernerhaus (UFS), Germany (47.417∘ N, 10.980∘ E), which is located near the summit of Zugspitze at an altitude of 2650 m. The lookup table consists of simulated O4 differential slant column densities (DSCDs) corresponding to numerous possible aerosol extinction profiles. The sensitivities of O4 absorption to several parameters were investigated for the design and parameterization of the lookup table. In the retrieval, simulated O4 DSCDs for each possible profile are derived by interpolating the lookup table to the observation geometries. The cost functions are calculated for each aerosol profile in the lookup table based on the simulated O4 DSCDs, the O4 DSCD observations, and the measurement uncertainties. Valid profiles are selected from all the possible profiles according to the cost function, and the optimal solution is defined as the weighted mean of all the valid profiles. A comprehensive error analysis is performed to better estimate the total uncertainty. Based on the assumption that the lookup table covers all possible profiles under clear-sky conditions, we determined a set of O4 DSCD scaling factors for different elevation angles and wavelengths. The profiles retrieved from synthetic measurement data can reproduce the synthetic profile. The results also show that the retrieval is insensitive to measurement noise, indicating the retrieval is robust and stable. The aerosol optical depths (AODs) retrieved from the long-term measurements were compared to coinciding and co-located sun photometer observations. High correlation coefficients (R) of 0.733 and 0.798 are found for measurements at 360 and 477 nm, respectively. However, especially in summer, the sun photometer AODs are systematically higher than the MAX-DOAS retrievals by a factor of ∼2. The discrepancy might be related to the limited measurement range of the MAX-DOAS and is probably also related to the decreased sensitivity of the MAX-DOAS measurements at higher altitudes. The MAX-DOAS measurements indicate the aerosol extinction decreases with increasing altitude during all seasons, which agrees with the co-located ceilometer measurements. Our results also show maximum AOD and maximum Ångström exponent in summer, which is consistent with observations at an AERONET station located ∼43 km from the UFS.

Description: Using a convective-cloud differential (CCD) method, developed in-house and applied to retrievals of total ozone and cloud data from three European satellite instruments (viz. GOME/ERS-2, 1995–2003; SCIAMACHY/Envisat, 2002–2012 and GOME-2/MetOp-A, 2007–2015), monthly mean tropical tropospheric columns of ozone (TTCO) have been retrieved, which are in good agreement with ozonesondes (biases less than 6 DU). As small differences in TTCO between the individual instruments were evident, it was necessary to develop a scheme to harmonise the three datasets into one consistent time series starting from 1996 until 2015. Correction offsets (biases) between the instruments using SCIAMACHY as intermediate reference have been calculated and six different harmonisation or merging scenarios have been evaluated. Depending on the merging approach, the magnitude, pattern and uncertainty in the trends strongly vary. The harmonisation or merging represents an additional source of uncertainty in the trends (2 DU decade−1 on average, in most of the cases exceeding the uncertainty from the regression). For studying further details on tropospheric ozone trends on various spatial scales in the tropics, we stick with one preferred merged dataset that shows best agreement with ozonesondes. In this merged dataset, no correction was applied for GOME, and mean biases with respect to SCIAMACHY in the overlapping period (2007–2012) were calculated and applied for GOME-2 in each grid box (2.5°  × 5°). In contrast with other studies we found that the tropospheric trend averaged over the tropics (−15° S to 15° N) is not statistically significant. The mean tropospheric ozone trend equals −0.2 ± 0.6 DU decade−1 (2σ). Regionally, tropospheric ozone has a statistically significant increase of  ∼  3 DU decade−1 over southern Africa ( ∼ 1.5 % yr−1), the southern tropical Atlantic ( ∼ 1.5 % yr−1), southeastern tropical Pacific Ocean ( ∼ 1 % yr−1), and central Oceania ( ∼ 2 % yr−1) and by  ∼ 2 DU decade−1 over central Africa (2–2.5 % yr−1) and south India ( ∼ 1.5 % yr−1). On the other hand, tropospheric O3 decreases by  ∼ 3 DU decade−1 over the Caribbean Sea and parts of the North Pacific Ocean ( ∼ 2 % yr−1), and by less than 2 DU decade−1 over some regions of the southern Pacific and Indian oceans ( ∼ 0.5–1 % yr−1).

Description: Aircraft measurements of NO2 using an imaging differential optical absorption spectrometer (iDOAS) instrument over the South African Highveld region in August 2007 are presented and compared to satellite measurements from OMI and SCIAMACHY. In situ aerosol and trace-gas vertical profile measurements, along with aerosol optical thickness and single-scattering albedo measurements from the Aerosol Robotic Network (AERONET), are used to devise scenarios for a radiative transfer modelling sensitivity study. Uncertainty in the air-mass factor due to variations in the aerosol and NO2 profile shape is constrained and used to calculate vertical column densities (VCDs), which are compared to co-located satellite measurements. The lower spatial resolution of the satellites cannot resolve the detailed plume structures revealed in the aircraft measurements. The airborne DOAS in general measured steeper horizontal gradients and higher peak NO2 vertical column density. Aircraft measurements close to major sources, spatially averaged to the satellite resolution, indicate NO2 column densities more than twice those measured by the satellite. The agreement between the high-resolution aircraft instrument and the satellite instrument improves with distance from the source, this is attributed to horizontal and vertical dispersion of NO2 in the boundary layer. Despite the low spatial resolution, satellite images reveal point sources and plumes that retain their structure for several hundred kilometres downwind.

Description: The TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor (S5P) satellite launched in October 2017 yields a wealth of atmospheric composition data, including retrievals of total column ozone (TCO3) that are provided in near-real-time (NRT) and off-line. The NRT TCO3 retrievals (v1.0.0–v1.1.2) have been included in the data assimilation system of the Copernicus Atmosphere Monitoring Service (CAMS), and tests to monitor the data and to carry out first assimilation experiments with them have been performed for the period 26 November 2017 to 30 November 2018. The TROPOMI TCO3 data agree to within 2 % with the CAMS analysis over large parts of the globe between 60∘ N and 60∘ S and also with TCO3 retrievals from the Ozone Monitoring Instrument (OMI) and the Global Ozone Monitoring Experiment-2 (GOME-2) that are routinely assimilated by CAMS. However, the TCO3 NRT data from TROPOMI show some retrieval anomalies at high latitudes, at low solar elevations and over snow/ice (e.g. Antarctica and snow-covered land areas in the Northern Hemisphere), where the differences with the CAMS analysis and the other data sets are larger. These differences are particularly pronounced over land in the NH during winter and spring (when they can reach up to 40 DU) and come mainly from the surface albedo climatology that is used in the NRT TROPOMI TCO3 retrieval. This climatology has a coarser horizontal resolution than the TROPOMI TCO3 data, which leads to problems in areas where there are large changes in reflectivity from pixel to pixel, e.g. pixels covered by snow/ice or not. The differences between TROPOMI and the CAMS analysis also show some dependency on scan position. The assimilation of TROPOMI TCO3 has been tested in the CAMS system for data between 60∘ N and 60∘ S and for solar elevations greater than 10∘ and is found to have a small positive impact on the ozone analysis compared to Brewer TCO3 data and an improved fit to ozone sondes in the tropical troposphere and to IAGOS aircraft profiles at West African airports. The impact of the TROPOMI data is relatively small because the CAMS analysis is already well constrained by several other ozone retrievals that are routinely assimilated. When averaged over the periods February–April and September–October 2018, differences between experiments with and without assimilation of TROPOMI data are less than 2 % for TCO3 and less than 3 % in the vertical for seasonal mean zonal mean O3 mixing ratios, with the largest relative differences found in the troposphere.

Description: In this paper, we present long-term observations of atmospheric nitrogen dioxide (NO2) and formaldehyde (HCHO) in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument. Ground-based MAX-DOAS measurements were performed from April 2013 to February 2017. The MAX-DOAS measurements of NO2 and HCHO vertical column densities (VCDs) are used to validate ozone monitoring instrument (OMI) satellite observations over Nanjing. The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient (R) of 0.91. However, OMI observations are on average a factor of 3 lower than the MAX-DOAS measurements. Replacing the a priori NO2 profiles by the MAX-DOAS profiles in the OMI NO2 VCD retrieval would increase the OMI NO2 VCDs by ∼30 % with correlation nearly unchanged. The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99. An age-weighted backward-propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time. The reconstructed NO2 fields show a distinct agreement with OMI satellite observations. However, due to the short atmospheric lifetime of HCHO, the backward-propagated HCHO data do not show a strong spatial correlation with the OMI HCHO observations. The result shows that the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta, indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants. The MAX-DOAS data are also used to evaluate the effectiveness of air pollution control measures implemented during the Youth Olympic Games 2014. The MAX-DOAS data show a significant reduction of ambient aerosol, NO2 and HCHO (30 %–50 %) during the Youth Olympic Games. Our results provide a better understanding of the transportation and sources of pollutants over the Yangtze River Delta as well as the effect of emission control measures during large international events, which are important for the future design of air pollution control policies.

Description: In October 2017, the Sentinel-5 Precursor (S5P) mission was launched, carrying the TROPOspheric Monitoring Instrument (TROPOMI), which provides a daily global coverage at a spatial resolution as high as 7 km × 3.5 km and is expected to extend the European atmospheric composition record initiated with GOME/ERS-2 in 1995, enhancing our scientific knowledge of atmospheric processes with its unprecedented spatial resolution. Due to the ongoing need to understand and monitor the recovery of the ozone layer, as well as the evolution of tropospheric pollution, total ozone remains one of the leading species of interest during this mission. In this work, the TROPOMI near real time (NRTI) and offline (OFFL) total ozone column (TOC) products are presented and compared to daily ground-based quality-assured Brewer and Dobson TOC measurements deposited in the World Ozone and Ultraviolet Radiation Data Centre (WOUDC). Additional comparisons to individual Brewer measurements from the Canadian Brewer Network and the European Brewer Network (Eubrewnet) are performed. Furthermore, twilight zenith-sky measurements obtained with ZSL-DOAS (Zenith Scattered Light Differential Optical Absorption Spectroscopy) instruments, which form part of the SAOZ network (Système d'Analyse par Observation Zénitale), are used for the validation. The quality of the TROPOMI TOC data is evaluated in terms of the influence of location, solar zenith angle, viewing angle, season, effective temperature, surface albedo and clouds. For this purpose, globally distributed ground-based measurements have been utilized as the background truth. The overall statistical analysis of the global comparison shows that the mean bias and the mean standard deviation of the percentage difference between TROPOMI and ground-based TOC is within 0 –1.5 % and 2.5 %–4.5 %, respectively. The mean bias that results from the comparisons is well within the S5P product requirements, while the mean standard deviation is very close to those limits, especially considering that the statistics shown here originate both from the satellite and the ground-based measurements. Additionally, the TROPOMI OFFL and NRTI products are evaluated against already known spaceborne sensors, namely, the Ozone Mapping Profiler Suite, on board the Suomi National Polar-orbiting Partnership (OMPS/Suomi-NPP), NASA v2 TOCs, and the Global Ozone Monitoring Experiment 2 (GOME-2), on board the Metop-A (GOME-2/Metop-A) and Metop-B (GOME-2/Metop-B) satellites. This analysis shows a very good agreement for both TROPOMI products with well-established instruments, with the absolute differences in mean bias and mean standard deviation being below +0.7 % and 1 %, respectively. These results assure the scientific community of the good quality of the TROPOMI TOC products during its first year of operation and enhance the already prevalent expectation that TROPOMI/S5P will play a very significant role in the continuity of ozone monitoring from space.

Description: Aircraft measurements of NO2 using an imaging differential optical absorption spectrometer (iDOAS) instrument over the South African Highveld region in August 2007 are presented and compared to satellite measurements from OMI and SCIAMACHY. In-situ aerosol and trace-gas vertical profile measurements, along with aerosol optical thickness and single-scattering albedo measurements from the Aerosol Robotic Network (AERONET), are used to devise scenarios for a radiative-transfer modelling sensitivity study. Uncertainty in the air-mass factor due to variations in the aerosol and NO2 profile shape is constrained, and used to calculate vertical column densities (VCD), which are compared to co-located satellite measurements. The lower spatial resolution of the satellites cannot resolve the detailed plume structures revealed in the aircraft measurements. The airborne DOAS in general measured steeper horizontal gradients and higher peak NO2 vertical column density. Aircraft measurements close to major sources, spatially-averaged to the satellite resolution, indicate NO2 column densities more than twice those measured by the satellite. The agreement between the high-resolution aircraft instrument and the satellite instrument improves with distance from the source. Despite their low spatial resolution, satellite images reveal point sources and plumes that retain their structure for several hundred kilometers downwind.

Description: We present a new aerosol profile retrieval algorithm for Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at high altitude sites. The study is based on the long-term measurement (February 2012 to February 2016) at the Environmental Research Station Schneefernerhaus (UFS), Germany, which is located near the summit of Zugspitze, at an altitude of 2,650 m. Due to the low signal to noise ratio, commonly used MAX-DOAS retrieval algorithms based on the optimal estimation method are not suitable for the retrieval of high altitude measurements. We developed a new retrieval algorithm using an O4 differential slant column density (DSCD) look-up table. The look-up table consists of simulated O4 DSCDs corresponding to numerous possible aerosol profiles. The sensitivities of O4 absorption to several parameters were investigated for the design and parameterization of the look-up table. In the retrieval, the simulated O4 DSCDs for each possible profile are derived by interpolating the look-up table to the observation geometries. The cost functions are calculated for each aerosol profile in the look-up table based on the simulated O4 DSCDs, the O4 DSCD observations as well as the measurement uncertainties. Valid profiles are selected from all the possible profiles according to the cost function, and the optimal solution is defined as the weighted mean of all valid profiles. A comprehensive error analysis is performed to better estimate the total uncertainty. Based on the assumption that the look-up table covers all the possible profiles under clear sky conditions, we determined a set of O4 DSCD scaling factors for different elevation angles and wavelengths. The dependence of the scaling factors on elevation angle might be partly related to the specific properties of the high altitude station, e.g. the highly structured topography, horizontal gradients of the aerosol extinction and the systematic dependence of the surface albedo on altitude. The retrieved aerosol optical depths (AODs) are compared to coincident and co-located sun photometer observations. High correlation coefficients of 0.733 and 0.798 are found for measurements at 360 and 477 nm, respectively. However, especially in summer the sun photometer AODs are systematically higher than the MAX-DOAS retrievals by a factor of 2. The discrepancy might be related to the limited measurement range of the MAX-DOAS, and is probably also related to the decreased sensitivity of the MAX-DOAS measurements at higher altitudes. Our results also show maximum AOD and maximum Ångström exponent in summer which is consistent with observations from an AERONET station located ~ 43 km of the MAX-DOAS.

Description: In this paper, we present long term observations of atmospheric nitrogen dioxide (NO2) and formaldehyde (HCHO) in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument. Ground based MAX-DOAS measurements were performed from April 2013 to February 2017. The MAX-DOAS measurements of NO2 and HCHO vertical column densities (VCDs) are used to validate OMI satellite observations over Nanjing. The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient (R) of 0.91. However, OMI observations are on average a factor of 3 lower than the MAX-DOAS measurements. Replacing the a priori NO2 profiles by the MAX-DOAS profiles in the OMI NO2 VCD retrieval would increase the OMI NO2 VCDs by ~ 30 % with correlation nearly unchanged. The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99. We developed a new technique to assemble the source contribution map using backward trajectory analysis. The age weighted backward propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time. The reconstructed NO2 fields show a distinct agreement with OMI satellite observations. However, due to the short atmospheric lifetime of HCHO, the backward propagated HCHO data does not show a strong spatial correlation with the OMI HCHO observations. The result shows the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta, indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants. The MAX-DOAS data are also used to evaluate the effectiveness of air pollution control measures implemented during the Youth Olympic Games 2014. The MAX-DOAS data show a significant reduction of ambient aerosol, NO2 and HCHO (30 %–50 %) during the Youth Olympic Games. Our results provide a better understanding of the transportation and sources of pollutants in over the Yangtze River Delta as well as the effect of emission control measures during large international event, which are important for the future design of air pollution control policies.

Description: In October 2017, the Sentinel-5 Precursor (S5p) mission was launched, carrying the TROPOspheric Monitoring Instrument, TROPOMI, which provides a daily global coverage at a spatial resolution as high as 7 km × 3.5 km and is expected to extend the European atmospheric composition record initiated with GOME/ERS-2 in 1995, bringing up significant new components to the scientific knowledge of atmospheric processes. Due to the ongoing need to understand and monitor the recovery of the ozone layer, as well as the evolution of tropospheric pollution, total ozone remains one of the leading species of interest during this mission. In this work the TROPOMI Near-Real Time, NRTI, and Offline, OFFL, total ozone column (TOC) products are presented and compared to daily ground-based quality-assured Brewer and Dobson TOC measurements deposited in the World Ozone and Ultraviolet Radiation Data Centre (WOUDC). Additional comparisons to individual Brewer measurements from the Canadian Brewer Network and the European Brewer Network (Eubrewnet) are performed. Furthermore, twilight zenith-sky measurements obtained with ZSL-DOAS (Zenith Scattered Light Differential Optical Absorption Spectroscopy) instruments, that form part of the SAOZ network (Système d'Analyse par Observation Zénitale), are used for the validation. The quality of the TROPOMI TOC data is evaluated in terms of the influence of location, solar zenith and viewing angles, season, effective temperature, surface albedo and clouds. For this purpose, globally distributed ground-based measurements have been utilized as the background truth. The overall statistical analysis of the global comparison shows that the mean bias and the mean standard deviation of the percentage difference between TROPOMI and ground-based TOC is within 0–1.5 % and 2.5–4.5 %, respectively. The mean bias that results from the comparisons is well within the S5p product requirements, while the mean standard deviation is very close to those limits, especially considering that the statistics shown here originate both from the satellite and the ground-based measurements. Additionally, the TROPOMI OFFL and NRTI products are evaluated against already known space-borne sensors, namely, the Ozone Mapping Profiler Suite on board the Suomi National Polar-orbiting Partnership (OMPS/Suomi-NPP), NASA v2 TOCs, and the Global Ozone Monitoring Experiment–2 (GOME-2) on board the MetοpΑ (GOME-2/MetοpΑ) and MetopB (GOME-2/MetopB) satellites. This analysis shows a very good agreement for both TROPOMI products to well established instruments, with the absolute differences in mean bias and mean standard deviation being below 0.7 % and 1 %, respectively. These results assure the scientific community of the good quality of the TROPOMI TOC products during its first year of operation and enhance the already high expectations that S5p TROPOMI will play a very significant role in the continuity of the ozone monitoring from space.