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Biomass burning releases large amounts of aerosols and chemical species into the atmosphere, representing a major source of air pollutants. Emissions and by-products can be transported over long distances, presenting challenges in quantification. This is mainly done using satellites, which offer global coverage and data acquisition for places that are difficult to access. In this study, ground-based observations are used to assess the abundance of trace gases and aerosols. On 24 November 2020, a significant increase in formaldehyde was observed with a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument located in Montevideo (Uruguay), and its vertical column densities reached values of 2.4×1016 molec. cm -2 , more than twice the values observed during the previous days. This was accompanied by an increase in the aerosol levels measured by an AErosol RObotic NETwork (AERONET) photometer located at the same site. The aerosol optical depth (AOD) at 440 nm reached values close to 1, an order of magnitude larger than typical values in Montevideo. Our findings indicate that the increase was associated with the passage of a plume originating from distant biomass burning. This conclusion is supported by TROPOspheric Monitoring Instrument (TROPOMI) satellite observations as well as HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) simulations. The profiles of the gases and aerosols retrieved from the MAX-DOAS observations are consistent with the HYSPLIT analysis, showing the passage of a plume over Montevideo on 24 November located at a height of ∼ 1.5 km. This corroborates the finding that biomass burning events occurring about 800 km north of Montevideo can affect the local atmosphere through long-distance emissions transport. This study underscores the potential of ground-based atmospheric monitoring as a tool for detection of such events. Furthermore, it demonstrates greater sensitivity compared to satellite when it comes to detection of relatively small amounts of carbonyls like glyoxal and formaldehyde. [ABSTRACT FROM AUTHOR]

Instruments for air quality observations on geostationary satellites provide multiple observations per day and allow for the analysis of the diurnal variation of important air pollutants such as nitrogen dioxide (NO2) over large areas. The South Korean instrument GEMS on the GK2B satellite was launched in February 2020 and is the first instrument in geostationary orbit that delivers hourly daytime observations of NO2. The measurements with a spatial resolution of 3.5 km x 8 km cover a large part of Asia. This study compares one year of tropospheric NO2 vertical column density (VCD) observations of the operational GEMS L2 product, the scientific GEMS IUP-UB product, the operational TROPOMI product, and ground-based DOAS measurements in South Korea. The GEMS L2 tropospheric NO2 VCDs overestimate the VCDs retrieved from the ground-based observations with a median relative difference of +64 % and a correlation coefficient of 0.75. The median relative difference is -1 % for the GEMS IUP-UB product and -14 % for the TROPOMI product. The evaluation of the GEMS IUP-UB product and the operational TROPOMI product with ground-based measurements is in good agreement with correlation coefficients of 0.82 and 0.88. The scatter in the GEMS products can be reduced when observations are limited to the TROPOMI overpass time. The observed diurnal variations of the tropospheric NO2 VCDs show a maximum of NO2 during the late morning for urban sites, whereas rural sites show weak or almost no diurnal changes. Investigations of the seasonal diurnal variability show with a minimum in the observed tropospheric NO2 VCDs around noon the importance of chemical loss of NO2 in summer. Most variability is seen in spring and autumn, which dominate the average annual diurnal cycle. Observations under low wind conditions show strong enhancements of NO2 over the day, especially at polluted sites during winter. This indicates that under calm conditions, dilution and the less effective chemical loss in winter do not balance the accumulating emissions. The impact of transport processes is illustrated by the diurnal variability at a rural site following mean wind patterns for specific seasons and observation times. Analyzing the weekday-weekend effect, good agreement was found between the different products. However, the GEMS L2 product while agreeing with the other data sets during weekdays shows significantly less reduction on weekends. Our investigations show that the observed diurnal evolution of NO2 varies significantly at the different measurement sites, with good agreement between the GEMS IUP-UB and ground-based observations. The diurnal variability of tropospheric NO2 VCDs depends on chemistry, emissions, and transport into and out of the measurement region. To interpret the sources and sinks of NO2 requires that all of these factors are considered. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) is the most important anthropogenic greenhouse gas. Its atmospheric concentration has increased by almost 50 % since the beginning of the industrial era, causing climate change. Fossil fuel combustion is responsible for most of the atmospheric CO2 increase, which originates to a large extent from localized sources such as power stations. Independent estimates of the emissions from these sources are key to tracking the effectiveness of implemented climate policies to mitigate climate change. We developed an automatic procedure to quantify CO2 emissions from localized sources based on a cross-sectional mass-balance approach and applied it to infer CO2 emissions from the Bełchatów Power Station (Poland) using atmospheric observations from the Orbiting Carbon Observatory 3 (OCO-3) in its snapshot area map (SAM) mode. As a result of the challenge of identifying CO2 emission plumes from satellite data with adequate accuracy, we located and constrained the shape of emission plumes using TROPOspheric Monitoring Instrument (TROPOMI) NO2 column densities. We automatically analysed all available OCO-3 overpasses over the Bełchatów Power Station from July 2019 to November 2022 and found a total of nine that were suitable for the estimation of CO2 emissions using our method. The mean uncertainty in the obtained estimates was 5.8 Mt CO 2 yr -1 (22.0 %), mainly driven by the dispersion of the cross-sectional fluxes downwind of the source, e.g. due to turbulence. This dispersion uncertainty was characterized using a semivariogram, made possible by the OCO-3 imaging capability over a target region in SAM mode, which provides observations containing plume information up to several tens of kilometres downwind of the source. A bottom-up emission estimate was computed based on the hourly power-plant-generated power and emission factors to validate the satellite-based estimates. We found that the two independent estimates agree within their 1σ uncertainty in eight out of nine analysed overpasses and have a high Pearson's correlation coefficient of 0.92. Our results confirm the potential to monitor large localized CO2 emission sources from space-based observations and the usefulness of NO2 estimates for plume detection. They also illustrate the potential to improve CO2 monitoring capabilities with the planned Copernicus Anthropogenic CO2 Monitoring (CO2M) satellite constellation, which will provide simultaneously retrieved XCO2 and NO2 maps. [ABSTRACT FROM AUTHOR]

Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN–MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tgyr-1), which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+ 13 %) and anthropogenic VOCs (- 17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50 ∘ N but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism, leading to differences of up to 10 % in the total emissions. However, the top-down emissions are very sensitive to the bias correction of the observed columns, as the biogenic emissions are 3 times lower when the correction is not applied. Furthermore, the use of different a priori biogenic emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. The sensitivity run using CAMS-GLOB-BIOv3.1 as a priori emissions in the inversion results in 30 % lower emissions with respect to the optimization using MEGAN–MOHYCAN. In regions with large temperature and cloud cover variations, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments. [ABSTRACT FROM AUTHOR]

Biomass burning releases large amounts of aerosols and chemical species into the atmosphere, which represents a major source of air pollutants. Emissions and by-products can be transported over long distances, presenting challenges in quantification. This is mainly done using satellites, which offer global coverage and data acquisition for places that are difficult to access. In this study, ground-based observations play an important role in assessing the abundance of trace gases and aerosols. On November 24, 2020, a significant increase in formaldehyde was observed, with a MAX-DOAS instrument located in Montevideo (Uruguay). Vertical column densities reached values of 2.4x1016 molec. cm-2, more than twice the values observed during the previous days. This was accompanied by an increase in the aerosol levels measured by an AERONET photometer located at the same site. For example, the AOD at 440 nm reached values close to 1, one order of magnitude larger than typical values in Montevideo. Our findings indicate that the cause of the increase was associated with the passage of a plume originating from distant biomass burning. This conclusion is supported using TROPOMI satellite observations as well as HYSPLIT trajectory simulations. The profiles of the gases and aerosols retrieved from the MAX-DOAS observations are consistent with the HYSPLIT analysis, showing the passage of a plume over Montevideo on November 24 located at a height of ∼1.5 km. This corroborates that biomass burning events that occur about 800 km north of Montevideo can affect the local atmosphere due to long-distance transport of emissions. This study underscores the potential of ground-based atmospheric monitoring as a tool for detection of such events. Furthermore, it demonstrates the greater sensitivity compared to satellite when it comes to detection of relatively small amounts of carbonyls like glyoxal and formaldehyde. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) is the most important anthropogenic greenhouse gas. Its atmospheric concentration has increased by almost 50 % since the beginning of the industrial era, causing climate change. Fossil fuel combustion is responsible for most of the atmospheric CO2 increase, which originates to a large extent from localized sources such as power stations. Independent estimates of the emissions from these sources are key to tracking the effectiveness of implemented climate policies to mitigate climate change. We developed a procedure to quantify CO2 emissions from localized sources based on a cross-sectional mass-balance approach and applied it to infer CO2 emissions from the Bełchatów Power Station, in Poland, using atmospheric observations from the Orbiting Carbon Observatory 3 (OCO-3) in its Snapshot Area Map (SAM) mode. As a result of the challenge of identifying CO2 emission plumes from satellite data with adequate accuracy, we located and constrained the shape of emission plumes using TROPOspheric Monitoring Instrument (TROPOMI) NO2 column densities. We analysed all available OCO-3 overpasses over the Bełchatów Power Station from July 2019 to November 2022 and found a total of 9 that were suitable for the estimation of CO2 emissions using our method. The mean uncertainty of the obtained estimates was 5.8 Mt CO2 y−1 (22.0 %), mainly driven by the dispersion of the cross-sectional fluxes downwind of the source, e.g. due to turbulence. This dispersion uncertainty was characterized using a semivariogram, possible thanks to the OCO-3 imaging capability over a target region in SAM mode, which provides observations containing plume information up to several tens of kilometres downwind of the source. A bottom-up emission estimate was computed based on the hourly power plant generated power and emission factors to validate the satellite-based estimates. We found that the two independent estimates agree within their 1 sigma uncertainty in 8 out of 9 analysed overpasses and have a high Pearson's correlation coefficient of 0.92. Our results confirm the potential for monitoring large localized CO2 emission sources from space-based observations and the usefulness of NO2 estimates for plume detection. They illustrate as well the potential to improve CO2 monitoring capabilities with the planned Copernicus Anthropogenic CO2 Monitoring (CO2M) satellite constellation, which will provide simultaneously retrieved XCO2 and NO2 maps. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) is the most important anthropogenic greenhouse gas. Its atmospheric concentration has increased by almost 50% since the beginning of the industrial era, causing climate change. Fossil fuel combustion is responsible for most of the atmospheric CO2 increase, which originates to a large extent from localized sources such as power stations. Independent estimates of the emissions from these sources are key to tracking the effectiveness of implemented climate policies to mitigate climate change. We developed a procedure to quantify CO2 emissions from localized sources based on a cross-sectional mass-balance approach and applied it to infer CO2 emissions from the Bełchatów Power Station, in Poland, using atmospheric observations from the Orbiting Carbon Observatory 3 (OCO-3) in its Snapshot Area Map (SAM) mode. As a result of the challenge of identifying CO2 emission plumes from satellite data with adequate accuracy, we located and constrained the shape of emission plumes using TROPOspheric Monitoring Instrument (TROPOMI) NO2 column densities. We analysed all available OCO-3 overpasses over the Bełchatów Power Station from July 2019 to November 2022 and found a total of 9 that were suitable for the estimation of CO2 emissions using our method. The mean uncertainty of the obtained estimates was 5.8 Mt CO2y-1 (22.0%), mainly driven by the dispersion of the cross-sectional fluxes downwind of the source, e.g. due to turbulence. This dispersion uncertainty was characterized using a semivariogram, possible thanks to the OCO-3 imaging capability over a target region in SAM mode, which provides observations containing plume information up to several tens of kilometres downwind of the source. A bottom-up emission estimate was computed based on the hourly power plant generated power and emission factors to validate the satellite-based estimates. We found that the two independent estimates agree within their 1σ uncertainty in 8 out of 9 analysed overpasses and have a high Pearson's correlation coefficient of 0.92. Our results confirm the potential for monitoring large localized CO2 emission sources from space-based observations and the usefulness of NO2 estimates for plume detection. They illustrate as well the potential to improve CO2 monitoring capabilities with the planned Copernicus Anthropogenic CO2 Monitoring (CO2M) satellite constellation, which will provide simultaneously retrieved XCO2 and NO2 maps. [ABSTRACT FROM AUTHOR]

Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly-averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN-MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tg yr-1) which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+13 %) and anthropogenic VOCs (-17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50° N, but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism. However, the top-down emissions are very sensitive to the bias correction of the observed columns. Furthermore, the use of different a priori emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. In regions with variable meteorology, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments. [ABSTRACT FROM AUTHOR]

During polar spring, ozone depletion events (ODEs) are often observed in combination with bromine explosion events (BEEs) in Ny-Ålesund. In this study, two long-term ozone data sets (2010–2021) from ozonesonde launches and in situ ozone measurements have been evaluated between March and May of each year to study ODEs in Ny-Ålesund. Ozone concentrations below 15 ppb were marked as ODEs. We applied a composite analysis to evaluate tropospheric BrO retrieved from satellite data and the prevailing meteorological conditions during these events. During ODEs, both data sets show a blocking situation with a low-pressure anomaly over the Barents Sea and anomalously high pressure in the Icelandic Low area, leading to transport of cold polar air from the north to Ny-Ålesund with negative temperature and positive BrO anomalies found around Svalbard. In addition, a higher wind speed and a higher, less stable boundary layer are noticed, supporting the assumption that ODEs often occur in combination with polar cyclones. Applying a 20 ppb ozone threshold value to tag ODEs resulted in only a slight attenuation of the BrO and meteorological anomalies compared to the 15 ppb threshold. Monthly analysis showed that BrO and meteorological anomalies are weakening from March to May. Therefore, ODEs associated with low-pressure systems, high wind speeds, and blowing snow more likely occur in early spring, while ODEs associated with low wind speed and stable boundary layer meteorological conditions seem to occur more often in late spring. Annual evaluations showed similar weather patterns for several years, matching the overall result of the composite analysis. However, some years show different meteorological patterns deviating from the results of the mean analysis. Finally, an ODE case study from the beginning of April 2020 in Ny-Ålesund is presented, where ozone was depleted for 2 consecutive days in combination with increased BrO values. The meteorological conditions are representative of the results of the composite analysis. A low-pressure system arrived from the northeast to Svalbard, resulting in high wind speeds with blowing snow and transport of cold polar air from the north. [ABSTRACT FROM AUTHOR]

Inland ships are an important source of NOx , especially for cities along busy waterways. The amount and effect of such emissions depend on the traffic density and NOx emission rates of individual vessels. Ship emission rates are typically derived using in situ land measurements in relation to NOx emission factors (e.g. the number of pollutants emitted by ships per unit of burnt fuel). In this study, a different approach is taken, and NOx emission rates are obtained (in gs-1). Within the EU LIFE project, CLean INland SHipping (CLINSH), a new approach to calculating the NOx emission rates from data of in situ measurement stations has been developed and is presented in this study. Peaks (i.e. elevated concentrations) of NOx were assigned to the corresponding source ships, using the AIS (automated identification system) signals they transmit. Each ship passage was simulated, using a Gaussian puff model, in order to derive the emission rate of the respective source ship. In total, over 32 900 ship passages have been monitored over the course of 4 years. The emission rates of NOx were investigated with respect to ship speed, ship size, and direction of travel. Comparisons of the onshore-derived emission rates and those on board for selected CLINSH ships show good agreement. The derived emission rates are of a similar magnitude to emission factors from previous studies. Most ships comply with existing limits due to grandfathering. The emission rates (in gs-1) can be directly used to investigate the effect of ship traffic on air quality, as the absolute emitted number of pollutants per unit of time is known. In contrast, for relative emission factors (in gkg-1 fuel), further knowledge about the fuel consumption of the individual ships is needed to calculate the number of pollutants emitted per unit of time. [ABSTRACT FROM AUTHOR]

Airborne imaging differential optical absorption spectroscopy (DOAS), ground-based stationary DOAS, and car DOAS measurements were conducted during the S5P-VAL-DE-Ruhr campaign in September 2020. The campaign area is located in the Rhine-Ruhr region of North Rhine-Westphalia, western Germany, which is a pollution hotspot in Europe comprising urban and large industrial sources. The DOAS measurements are used to validate spaceborne NO 2 tropospheric vertical column density (VCD) data products from the Sentinel-5 Precursor (S5P) TROPOspheric Monitoring Instrument (TROPOMI). Seven flights were performed with the airborne imaging DOAS instrument for measurements of atmospheric pollution (AirMAP), providing measurements that were used to create continuous maps of NO 2 in the layer below the aircraft. These flights cover many S5P ground pixels within an area of 30 km × 35 km and were accompanied by ground-based stationary measurements and three mobile car DOAS instruments. Stationary measurements were conducted by two Pandora, two Zenith-DOAS, and two MAX-DOAS instruments. Ground-based stationary and car DOAS measurements are used to evaluate the AirMAP tropospheric NO 2 VCDs and show high Pearson correlation coefficients of 0.88 and 0.89 and slopes of 0.90 ± 0.09 and 0.89 ± 0.02 for the stationary and car DOAS, respectively. Having a spatial resolution of about 100 m × 30 m, the AirMAP tropospheric NO 2 VCD data create a link between the ground-based and the TROPOMI measurements with a nadir resolution of 3.5 km × 5.5 km and are therefore well suited to validate the TROPOMI tropospheric NO 2 VCD. The observations on the 7 flight days show strong NO 2 variability, which is dependent on the three target areas, the day of the week, and the meteorological conditions. The AirMAP campaign data set is compared to the TROPOMI NO 2 operational offline (OFFL) V01.03.02 data product, the reprocessed NO 2 data using the V02.03.01 of the official level-2 processor provided by the Product Algorithm Laboratory (PAL), and several scientific TROPOMI NO 2 data products. The AirMAP and TROPOMI OFFL V01.03.02 data are highly correlated (r=0.87) but show an underestimation of the TROPOMI data with a slope of 0.38 ± 0.02 and a median relative difference of - 9 %. With the modifications in the NO 2 retrieval implemented in the PAL V02.03.01 product, the slope and median relative difference increased to 0.83 ± 0.06 and + 20 %. However, the modifications resulted in larger scatter and the correlation decreased significantly to r=0.72. The results can be improved by not applying a cloud correction for the TROPOMI data in conditions with high aerosol load and when cloud pressures are retrieved close to the surface. The influence of spatially more highly resolved a priori NO 2 vertical profiles and surface reflectivity are investigated using scientific TROPOMI tropospheric NO 2 VCD data products. The comparison of the AirMAP campaign data set to the scientific data products shows that the choice of surface reflectivity database has a minor impact on the tropospheric NO 2 VCD retrieval in the campaign region and season. In comparison, the replacement of the a priori NO 2 profile in combination with the improvements in the retrieval of the PAL V02.03.01 product regarding cloud heights can further increase the tropospheric NO 2 VCDs. This study demonstrates that the underestimation of the TROPOMI tropospheric NO 2 VCD product with respect to the validation data set has been and can be further significantly improved. [ABSTRACT FROM AUTHOR]

Clouds have a strong impact on satellite measurements of tropospheric trace gases in the ultraviolet, visible, and near-infrared spectral ranges from space. Therefore, trace gas retrievals rely on information on cloud fraction, cloud albedo, and cloud height from cloud products. In this study, the cloud parameters from different cloud retrieval algorithms for the Sentinel-5 Precursor (S5P) TROPOspheric Monitoring Instrument (TROPOMI) are compared: the Optical Cloud Recognition Algorithm (OCRA) a priori cloud fraction, the Retrieval Of Cloud Information using Neural Networks (ROCINN) CAL (Clouds-As-Layers) cloud fraction and cloud top and base height, the ROCINN CRB (Clouds-as-Reflecting-Boundaries) cloud fraction and cloud height, the Fast Retrieval Scheme for Clouds from the Oxygen A-band (FRESCO) cloud fraction, the interpolated FRESCO cloud height from the TROPOMI NO 2 product, the cloud fraction from the NO 2 fitting window, the O 2 –O 2 cloud fraction and cloud height, the Mainz Iterative Cloud Retrieval Utilities (MICRU) cloud fraction, and the Visible Infrared Imaging Radiometer Suite (VIIRS) cloud fraction. Two different versions of the TROPOMI cloud products OCRA/ROCINN, FRESCO, and the TROPOMI NO 2 product are included in the comparisons (processor version 1.x and 2.x). Overall, the cloud parameters retrieved by the different algorithms show qualitative consistency in version 1.x and good agreement in version 2.x with the exception of the VIIRS cloud fraction, which cannot be directly compared to the other data. Differences between the cloud retrievals are found especially for small cloud heights with a cloud fraction threshold of 0.2, i.e. clouds that are particularly relevant for tropospheric trace gas retrievals. The cloud fractions of the different version 2 cloud products primarily differ over snow- and ice-covered pixels and scenes with sun glint, for which only MICRU includes an explicit treatment. All cloud parameters show some systematic problems related to the across-track dependence, where larger values are found at the edges of the satellite view. The consistency between the cloud parameters from different algorithms depends strongly on how the data are filtered for the comparison, for example, what quality value is used or whether snow- and ice-covered pixels are excluded from the analysis. In summary, clear differences were found between the results of various algorithms, but these differences are reduced in the most recent versions of the cloud data. [ABSTRACT FROM AUTHOR]

Airborne imaging differential optical absorption spectroscopy (DOAS), ground-based stationary and car DOAS measurements were conducted during the S5P-VAL-DE-Ruhr campaign in September 2020. The campaign area is located in the Rhine-Ruhr region of North Rhine-Westphalia,Western Germany, which is a pollution hotspot in Europe comprising urban and large industrial emitters. The measurements are used to validate space-borne NO2 tropospheric vertical column density data products from the Sentinel-5 Precursor (S5P) TROPOspheric Monitoring Instrument (TROPOMI). Seven flights were performed with the airborne imaging DOAS instrument formeasurements of atmospheric pollution (AirMAP), providing measurements which were used to create continuous maps of NO2 in the layer below the aircraft. These flights cover many S5P ground pixels within an area of 30 kmx 35 km and were accompanied by ground-based stationary measurements and three mobile car DOAS instruments. Stationary measurements were conducted by two Pandora, two zenith-sky and two MAX-DOAS instruments distributed over three target areas. Ground-based stationary and car DOAS measurements are used to evaluate the AirMAP tropospheric NO2 vertical column densities and show high Pearson correlation coefficients of 0.87 and 0.89 and slopes of 0.93±0.09 and 0.98±0.02 for the stationary and car DOAS, respectively. Having a spatial resolution of about 100mx 30m, the AirMAP tropospheric NO2 vertical column density (VCD) data creates a link between the ground-based and the TROPOMI measurements with a resolution of 3.5 kmx 5.5 km and is therefore well suited to validate the TROPOMI tropospheric NO2 VCD. The measurements on the seven flight days show strong NO2 variability, which is dependent on the different target areas, the weekday, and the meteorological conditions. The AirMAP campaign dataset is compared to the TROPOMI NO2 operational off-line (OFFL) V01.03.02 data product, the reprocessed NO2 data, using the V02.03.01 of the official L2 processor, provided by the Product Algorithm Laboratory (PAL), and several scientific TROPOMI NO2 data products. The TROPOMI data products and the AirMAP data are highly correlated with correlation coefficients between 0.72 and 0.87, and slopes of 0.38±0.02 to 1.02±0.07. On average, TROPOMI tropospheric NO2 VCDs are lower than the AirMAP NO2 results. The slope increased from 0.38±0.02 for the operational OFFL V01.03.02 product to 0.83±0.06 after the improvements in the retrieval of the PAL V02.03.01 product were implemented. Different auxiliary data, such as spatially higher resolved a priori NO2 vertical profiles, surface reflectivity and the cloud treatment, are investigated using scientific TROPOMI tropospheric NO2 VCD data products to evaluate their impact on the operational TROPOMI NO2 VCD data product. The comparison of the AirMAP campaign dataset to the scientific data products shows that the choice of surface reflectivity data base has a minor impact on the tropospheric NO2 VCD retrieval in the campaign region and season. In comparison, the replacement of the a priori NO2 profile in combination with the improvements in the retrieval of the PAL V02.03.01 product regarding cloud heights has a major impact on the tropospheric NO2 VCD retrieval and increases the slope from 0.88±0.06 to 1.00±0.07. This study demonstrates that the underestimation of the TROPOMI tropospheric NO2 VCD product with respect to the validation dataset has been and can be further significantly improved. [ABSTRACT FROM AUTHOR]

Soils in the northern high latitudes are a key component in the global carbon cycle; the northern permafrost region covers 22 % of the Northern Hemisphere land surface area and holds almost twice as much carbon as the atmosphere. Permafrost soil organic matter stocks represent an enormous long-term carbon sink which is in risk of switching to a net source in the future. Detailed knowledge about the quantity and the mechanisms controlling organic carbon storage is of utmost importance for our understanding of potential impacts of and feedbacks on climate change. Here we present a geospatial dataset of physical and chemical soil properties calculated from 651 soil pedons encompassing more than 6500 samples from 16 different study areas across the northern permafrost region. The aim of our dataset is to provide a basis to describe spatial patterns in soil properties, including quantifying carbon and nitrogen stocks. There is a particular need for spatially distributed datasets of soil properties, including vertical and horizontal distribution patterns, for modeling at local, regional, or global scales. This paper presents this dataset, describes in detail soil sampling; laboratory analysis, and derived soil geochemical parameters; calculations; and data clustering. Moreover, we use this dataset to estimate soil organic carbon and total nitrogen storage estimates in soils in the northern circumpolar permafrost region (17.9×106 km 2) using the European Space Agency's (ESA's) Climate Change Initiative (CCI) global land cover dataset at 300 m pixel resolution. We estimate organic carbon and total nitrogen stocks on a circumpolar scale (excluding Tibet) for the 0–100 and 0–300 cm soil depth to be 380 and 813 Pg for carbon, and 21 and 55 Pg for nitrogen, respectively. Our organic carbon estimates agree with previous studies, with most recent estimates of 1000 Pg (-170 to +186 Pg) to 300 cm depth. Two separate datasets are freely available on the Bolin Centre Database repository (10.17043/palmtag-2022-pedon-1, Palmtag et al., 2022a; and 10.17043/palmtag-2022-spatial-1, Palmtag et al., 2002b). [ABSTRACT FROM AUTHOR]

Inland ships are an important source of NOx, especially for cities along busy waterways. The amount and effect of these emissions depends on the traffic density and the NOx emission rates of the individual vessels. Monitoring of ship emissions is usually carried out using in situ instruments on land and often relative NOx emission factors, e.g. the amount of emitted pollutants per amount of burnt fuel is reported, but in this study, NOx emission rates in g s-1 are investigated. Within the EU Life project Clean Inland Shipping (CLINSH), a new approach to calculate NOx emission rates from data of in situ measurement stations has been developed and is presented in this study. Peaks (i.e. elevated concentrations) of NOx were assigned to the corresponding source ships and each ship passage was simulated using a Gaussian-puff-model in order to derive the emission rate. In total over 32900 ship passages have been monitored over the course of 4 years. The emission rates of NOx were investigated with respect to ship speed, ship size and direction of travel. Individual comparisons of the on-shore emission rates and those made on-board of selected CLINSH ships show good agreement. Also the emission rates are of similar magnitude as emission factors from previous studies. In contrast to relative emission factors (in grams per kilogram fuel), the emission rates (in grams per second) do not need further knowledge about the fuel consumption of the ship and can therefore be used directly to investigate the effect of ship traffic on air quality. [ABSTRACT FROM AUTHOR]

Inland ships are an important source of NO x , especially for cities along busy waterways. The amount and effect of these emissions depends on the traffic density and the NO x emission rates of the individual vessels. Monitoring of ship emissions is usually carried out using in situ instruments on land and often relative NO x emission factors, e.g. the amount of emitted pollutants per amount of burnt fuel is reported, but in this study, NO x emission rates in g s-1 are investigated. Within the EU Life project Clean Inland Shipping (CLINSH), a new approach to calculate NO x emission rates from data of in situ measurement stations has been developed and is presented in this study. Peaks (i.e. elevated concentrations) of NO x were assigned to the corresponding source ships and each ship passage was simulated using a Gaussian-puff-model in order to derive the emission rate. In total over 32900 ship passages have been monitored over the course of 4 years. The emission rates of NO x were investigated with respect to ship speed, ship size and direction of travel. Individual comparisons of the on-shore emission rates and those made on-board of selected CLINSH ships show good agreement. Also the emission rates are of similar magnitude as emission factors from previous studies. In contrast to relative emission factors (in grams per kilogram fuel), the emission rates (in grams per second) do not need further knowledge about the fuel consumption of the ship and can therefore be used directly to investigate the effect of ship traffic on air quality. [ABSTRACT FROM AUTHOR]

Ongoing climate warming in the western Canadian Arctic is leading to thawing of permafrost soils and subsequent mobilization of its organic matter pool. Part of this mobilized terrestrial organic matter enters the aquatic system as dissolved organic matter (DOM) and is laterally transported from land to sea. Mobilized organic matter is an important source of nutrients for ecosystems, as it is available for microbial breakdown, and thus a source of greenhouse gases. We are beginning to understand spatial controls on the release of DOM as well as the quantities and fate of this material in large Arctic rivers. Yet, these processes remain systematically understudied in small, high-Arctic watersheds, despite the fact that these watersheds experience the strongest warming rates in comparison. Here, we sampled soil (active layer and permafrost) and water (porewater and stream water) from a small ice wedge polygon (IWP) catchment along the Yukon coast, Canada, during the summer of 2018. We assessed the organic carbon (OC) quantity (using dissolved (DOC) and particulate OC (POC) concentrations and soil OC content), quality (δ13C DOC, optical properties and source apportionment) and bioavailability (incubations; optical indices such as slope ratio, Sr ; and humification index, HIX) along with stream water properties (temperature, T ; pH; electrical conductivity, EC; and water isotopes). We classify and compare different landscape units and their soil horizons that differ in microtopography and hydrological connectivity, giving rise to differences in drainage capacity. Our results show that porewater DOC concentrations and yield reflect drainage patterns and waterlogged conditions in the watershed. DOC yield (in mgDOCg-1soilOC) generally increases with depth but shows a large variability near the transition zone (around the permafrost table). Active-layer porewater DOC generally is more labile than permafrost DOC, due to various reasons (heterogeneity, presence of a paleo-active-layer and sampling strategies). Despite these differences, the very long transport times of porewater DOC indicate that substantial processing occurs in soils prior to release into streams. Within the stream, DOC strongly dominates over POC, illustrated by DOC/POC ratios around 50, yet storm events decrease that ratio to around 5. Source apportionment of stream DOC suggests a contribution of around 50 % from permafrost/deep-active-layer OC, which contrasts with patterns observed in large Arctic rivers (12 ± 8 %; Wild et al., 2019). Our 10 d monitoring period demonstrated temporal DOC patterns on multiple scales (i.e., diurnal patterns, storm events and longer-term trends), underlining the need for high-resolution long-term monitoring. First estimates of Black Creek annual DOC (8.2 ± 6.4 tDOCyr-1) and POC (0.21 ± 0.20 tyr-1) export allowed us to make a rough upscaling towards the entire Yukon Coastal Plain (34.51 ± 2.7 ktDOCyr-1 and 8.93 ± 8.5 ktPOCyr-1). Rising Arctic temperatures, increases in runoff, soil organic matter (OM) leaching, permafrost thawing and primary production are likely to increase the net lateral OC flux. Consequently, altered lateral fluxes may have strong impacts on Arctic aquatic ecosystems and Arctic carbon cycling. [ABSTRACT FROM AUTHOR]

Satellite observations of the high-resolution TROPOspheric Monitoring Instrument (TROPOMI) on Sentinel-5 Precursor can be used to observe nitrogen dioxide (NO 2) at city scales to quantify short time variability of nitrogen oxide (NO x) emissions and lifetimes on a daily and seasonal basis. In this study, 2 years of TROPOMI tropospheric NO 2 columns, having a spatial resolution of up to 3.5 km × 5.5 km , have been analyzed together with wind and ozone data. NO x lifetimes and emission fluxes are estimated for 50 different NO x sources comprising cities, isolated power plants, industrial regions, oil fields, and regions with a mix of sources distributed around the world. The retrieved NO x emissions are in agreement with other TROPOMI-based estimates and reproduce the variability seen in power plant stack measurements but are in general lower than the analyzed stack measurements and emission inventory results. Separation into seasons shows a clear seasonal dependence of NO x emissions with in general the highest emissions during winter, except for isolated power plants and especially sources in hot desert climates, where the opposite is found. The NO x lifetime shows a systematic latitudinal dependence with an increase in lifetime from 2 to 8 h with latitude but only a weak seasonal dependence. For most of the 50 sources including the city of Wuhan in China, a clear weekly pattern of NO x emissions is found, with weekend-to-weekday ratios of up to 0.5 but with a high variability for the different locations. During the Covid-19 lockdown period in 2020, strong reductions in the NO x emissions were observed for New Delhi, Buenos Aires, and Madrid. [ABSTRACT FROM AUTHOR]

Ongoing climate warming in the western Canadian Arctic is leading to thawing of permafrost soils and subsequent mobilization of its organic matter pool. Part of this mobilized terrestrial organic matter enters the aquatic system as dissolved organic matter (DOM) and is laterally transported from land to sea. Mobilized organic matter is an important source of nutrients for ecosystems as it is available for microbial breakdown, and thus a source of greenhouse gases. We are beginning to understand spatial controls on the release of DOM as well as the quantities and fate of this material in large arctic rivers. Yet, these processes remain systematically understudied in small, high-arctic watersheds, despite the fact that these watersheds experience the strongest warming rates in comparison. Here, we sampled soil (active layer and permafrost) and water (porewater and stream water) from a small catchment along the Yukon coast, Canada, during the summer of 2018. We assessed the organic carbon (OC) quantity (using dissolved (DOC) and particulate OC (POC) concentrations and soil OC content), quality δ13C-DOC, optical properties, source-apportionment), and bioavailability (incubations, optical indices such as slope ratio (Sr) and humification index (HIX)) along with stream water properties (T, pH, EC, water isotopes). We classify and compare different landscape units and their soil horizons that differ in microtopography and hydrological connectivity, giving rise to differences in drainage capacity. Our results show that porewater DOC concentrations and yield reflect drainage patterns and waterlogged conditions in the watershed. DOC yield (in mg DOC g soil OC-1) generally increases with depth but shows a large variability near the transition zone (around the permafrost table). Active layer porewater DOC generally is more labile than permafrost DOC, due to various reasons (heterogeneity, presence of a paleo-active layer, and sampling strategies). Despite these differences, the very long transport times of porewater DOC indicate that substantial processing occurs in soils prior to release into streams. Within the stream, DOC strongly dominates over POC, illustrated by DOC/POC ratios around 50, yet storm events decrease that ratio to around 5. Source-apportionment of stream DOC suggests a contribution of around 50 % from permafrost/deep-active layer OC, which contrasts to patterns observed in large arctic rivers (12 ±8 % Wild et al., 2019). Our 10-day monitoring period demonstrated temporal DOC patterns on multiple scales (i.e. diurnal patterns, storm-events, and longer-term trend) underlining the need for high-resolution long-term monitoring. First estimates of Black Creek annual DOC (8.2 ±6.4 t DOC yr-1) and POC (0.21 ±0.20 t yr-1) export allowed us to make a rough up-scaling towards the entire Yukon Coastal Plain (34.51 ±2.7 kt DOC yr-1 and 8.93 ±8.5 kt POC yr-1). With raising arctic temperatures, increases in runoff, soil OM leaching, permafrost thawing and primary production are likely to increase the net lateral OC flux. Consequently, altered lateral fluxes may have strong impacts on the arctic aquatic ecosystems and arctic carbon cycling. [ABSTRACT FROM AUTHOR]

We present the first global glyoxal (CHOCHO) tropospheric column product derived from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite. Atmospheric glyoxal results from the oxidation of other non-methane volatile organic compounds (NMVOCs) and from direct emissions caused by combustion processes. Therefore, this product is a useful indicator of VOC emissions. It is generated with an improved version of the BIRA-IASB scientific retrieval algorithm relying on the differential optical absorption spectroscopy (DOAS) approach. Among the algorithmic updates, the DOAS fit now includes corrections to mitigate the impact of spectral misfits caused by scene brightness inhomogeneity and strong NO 2 absorption. The product comes along with a full error characterization, which allows for providing random and systematic error estimates for every observation. Systematic errors are typically in the range of 1 ×1014 –3 ×1014 molec. cm -2 (∼30% – 70% in emission regimes) and originate mostly from a priori data uncertainties and spectral interferences with other absorbing species. The latter may be at the origin, at least partly, of an enhanced glyoxal signal over equatorial oceans, and further investigation is needed to mitigate them. Random errors are large (>6×1014 molec. cm -2) but can be reduced by averaging observations in space and/or time. Benefiting from a high signal-to-noise ratio and a large number of small-size observations, TROPOMI provides glyoxal tropospheric column fields with an unprecedented level of detail. Using the same retrieval algorithmic baseline, glyoxal column data sets are also generated from the Ozone Monitoring Instrument (OMI) on Aura and from the Global Ozone Monitoring Experiment-2 (GOME-2) on board Metop-A and Metop-B. Those four data sets are intercompared over large-scale regions worldwide and show a high level of consistency. The satellite glyoxal columns are also compared to glyoxal columns retrieved from ground-based Multi-AXis DOAS (MAX-DOAS) instruments at nine stations in Asia and Europe. In general, the satellite and MAX-DOAS instruments provide consistent glyoxal columns both in terms of absolute values and vari ability. Correlation coefficients between TROPOMI and MAX-DOAS glyoxal columns range between 0.61 and 0.87. The correlation is only poorer at one mid-latitude station, where satellite data appear to be biased low during wintertime. The mean absolute glyoxal columns from satellite and MAX-DOAS generally agree well for low/moderate columns with differences of less than 1×1014 molec. cm -2. A larger bias is identified at two sites where the MAX-DOAS columns are very large. Despite this systematic bias, the consistency of the satellite and MAX-DOAS glyoxal seasonal variability is high. [ABSTRACT FROM AUTHOR]

Here we present a new retrieval algorithm of the slant column densities (SCDs) of chlorine dioxide (OClO) by differential optical absorption spectroscopy (DOAS) from measurements performed by TROPOspheric Monitoring Instrument (TROPOMI) on board of Sentinel-5P satellite. To achieve a substantially improved accuracy, which is especially important for OClO observations, accounting for absorber and pseudo absorber structures in optical depth even of the order of 10-4 is important. Therefore, in comparison to existing retrievals, we include several additional fit parameters by accounting for spectral effects like the temperature dependency of the Ring effect and Ring absorption effects, a higher-order term for the OClO SCD dependency on wavelength and accounting for the BrO absorption. We investigate the performance of different retrieval settings by an error analysis with respect to random variations, large-scale systematic variations as a function of solar zenith angle and also more localized systematic variations by a novel application of an autocorrelation analysis. The retrieved TROPOMI OClO SCDs show a very good agreement with ground-based zenith sky measurements and are correlated well with preliminary data of the operational TROPOMI OClO retrieval algorithm currently being developed as part of ESA's Sentinel-5P+ Innovation project. [ABSTRACT FROM AUTHOR]

This paper reports on ground-based validation of the atmospheric OClO data record produced in the framework of EUMETSAT's Satellite Application Facility on Atmospheric Chemistry Monitoring (AC SAF) using the GOME2-A and -B instruments over the 2007-2016 and 2013-2016 periods, respectively. OClO slant column densities are compared to correlative measurements collected from 9 NDACC Zenith-Scattered-Light DOAS (ZSL-DOAS) instruments distributed in both the Arctic and Antarctic. Sensitivity tests are performed on the ground-based data to estimate the impact of the different OClO DOAS analysis settings. On this basis, we infer systematic uncertainties of about 25 % between the different ground-based data analysis, reaching total uncertainties ranging from about 26 % to 33 % for the different stations. Time-series at the different sites show good agreement between satellite and ground-based data, both for the inter-annual variability and the overall OClO seasonal behavior. GOME-2A results are found to be nosier than those of GOME-2B, especially after 2011, probably due to instrumental degradation effects. Daily linear regression analysis for OClO activated periods yield correlation coefficients of 0.8 for GOME-2A and 0.87 for GOME-2B, with slopes of 0.64 and 0.72, respectively. Biases are within 8 x 1013 molec/cm2 with some differences between GOME-2A and GOME- 2B, depending on the station. Overall, considering all the stations, a median bias of about -2.2 x 1013 molec/cm2 is found for both GOME-2 instruments. [ABSTRACT FROM AUTHOR]

Ships are an important source of SO 2 and NO x , which are key parameters of air quality. Monitoring of ship emissions is usually carried out using in situ instruments on land, which depend on favourable wind conditions to transport the emitted substances to the measurement site. Remote sensing techniques such as long-path differential optical absorption spectroscopy (LP-DOAS) measurements can supplement those measurements, especially in unfavourable meteorological conditions. In this study 1 year of LP-DOAS measurements made across the river Elbe close to Hamburg (Germany) have been evaluated. Peaks (i.e. elevated concentrations) in the NO 2 and SO 2 time series were assigned to passing ships, and a method to derive emission rates of SO 2 , NO 2 and NO x from those measurements using a Gaussian plume model is presented. A total of 7402 individual ship passages have been monitored, and their respective NO x , SO 2 and NO 2 emission rates have been derived. The emission rates, coupled with the knowledge of the ship type, ship size and ship speed, have been analysed. Emission rates are compared to emission factors from previous studies and show good agreement. In contrast to emission factors (in grams per kilogram fuel), the derived emission rates (in grams per second) do not need further knowledge about the fuel consumption of the ship. To our knowledge this is the first time emission rates of air pollutants from individual ships have been derived from LP-DOAS measurements. [ABSTRACT FROM AUTHOR]

Since May 2017 and August 2018, two ground-based MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments have been continuously recording daytime spectral UV–visible measurements in the northwest (University of Natural Resources and Life Sciences (BOKU) site) and south (Arsenal site), respectively, of the Vienna city center (Austria). In this study, vertical aerosol extinction (AE) profiles, aerosol optical depth (AOD), and near-surface AE are retrieved from MAX-DOAS measurements recorded on cloud-free days applying the Bremen Optimal estimation REtrieval for Aerosols and trace gaseS (BOREAS) algorithm. Measurements of atmospheric profiles of pressure and temperature obtained from routinely performed sonde ascents are used to calculate box-air-mass factors and weighting functions for different seasons. The performance of BOREAS was evaluated against co-located ceilometer, sun photometer, and in situ instrument observations covering all four seasons. The results show that the vertical AE profiles retrieved from the BOKU UV–visible MAX-DOAS observations are in very good agreement with data from the co-located ceilometer, reaching correlation coefficients (R) of 0.936–0.996 (UV) and 0.918–0.999 (visible) during the fall, winter, and spring seasons. Moreover, AE extracted using the lowest part of MAX-DOAS vertical profiles (up to 100 m above ground) is highly consistent with near-surface ceilometer AE (R>0.865 and linear regression slopes of 0.815–1.21) during the fall, winter, and spring seasons. A strong correlation is also found for the BOREAS-based AODs when compared to the AERONET ones. Notably, the highest correlation coefficients (R=0.953 and R=0.939 for UV and visible, respectively) were identified for the fall season. While high correlation coefficients are generally found for the fall, winter, and spring seasons, the results are less reliable for measurements taken during summer. For the first time, the spatial variability of AOD and near-surface AE over the urban environment of Vienna is assessed by analyzing the retrieved and evaluated BOREAS aerosol profiling products in terms of different azimuth angles of the two MAX-DOAS instruments and for different seasons. We found that the relative differences of averaged AOD between different azimuth angles are 7–13 % , depending on the season. Larger relative differences of up to 32 % are found for near-surface AE in the different azimuthal directions. This study revealed the strong capability of BOREAS to retrieve AE profiles, AOD, and near-surface AE over urban environments and demonstrated its use for identifying the spatial variability of aerosols in addition to the temporal variation. [ABSTRACT FROM AUTHOR]

Satellite observations of the high-resolution instrument TROPOMI on Sentinel-5 Precursor can be used to observe nitrogen dioxide (NO2) at city scales, to quantify short time variability of NOx emissions and lifetime on a seasonal and daily basis. In this study, two years of TROPOMI NO2data, having a spatial resolution of 3.5km x 5.5km, together with ECMWF ERA5 wind data have been analyzed. NOx lifetimes and emission fluxes are calculated for 45 different NOx sources comprising cities and power plants, distributed around the world. The retrieved emissions are lower than the bottom-up emission inventories from EDGAR v5.0 but are in good agreement with other TROPOMI based estimates. Separation into seasons shows a clear seasonal dependence of emissions with in general the highest emissions during winter, except for cities in hot dessert climates, where the opposite is found. The NOx lifetime shows a systematic latitudinal dependence with an increase in lifetime from two to eight hours with latitude but only a weak seasonal dependence. For most of the 45 sources, a clear weekly pattern of emissions is found with weekend-to-week day ratios of up to 0.5, but with a high variability for the different locations. During the Covid-19 lockdown period in 2020 strong reductions in the NOx emissions were observed for New Delhi, Buenos Aires and Madrid. [ABSTRACT FROM AUTHOR]

The evaluation of chemical transport models, CTMs, is essential for the assessment of their performance regarding the physical and chemical parameterizations used. While regional CTMs have been widely used and evaluated over Europe, their validation over Greece is limited. In this study, we investigate the performance of the Long Term Ozone Simulation European Operational Smog (LOTOS-EUROS) v2.2.001 regional chemical transport model in simulating nitrogen dioxide, NO 2 , over Greece from June to December 2018. In situ NO 2 measurements obtained from 14 stations of the National Air Pollution Monitoring Network are compared with surface simulations over the two major cities of Greece, Athens and Thessaloniki. Overall the LOTOS-EUROS NO 2 surface simulations compare very well to the in situ measurements showing a mild underestimation of the measurements with a mean relative bias of ∼-10 %, a high spatial correlation coefficient of 0.86 and an average temporal correlation of 0.52. The CTM underestimates the NO 2 surface concentrations during daytime by ∼-50 ± 15 %, while it slightly overestimates during night-time ∼ 10 ± 35 %. Furthermore, the LOTOS-EUROS tropospheric NO 2 columns are evaluated against ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) NO 2 measurements in Athens and Thessaloniki. We report that the CTM tropospheric NO 2 column simulations over both urban and rural locations represent the diurnal patterns and hourly levels for both summer and winter seasons satisfactorily. The relative biases range between ∼ - 2 % and - 35 %, depending on season and relative NO 2 load observed. Finally, the CTM was assessed also against space-borne Sentinel-5 Precursor (S5P) carrying the Tropospheric Monitoring Instrument (TROPOMI) tropospheric NO 2 observations. We conclude that LOTOS-EUROS simulates extremely well the tropospheric NO 2 patterns over the region with very high spatial correlation of 0.82 on average, ranging between 0.66 and 0.95, with negative biases in the summer and positive in the winter. Updated emissions for the simulations and model improvements when extreme values of boundary layer height are encountered are further suggested. [ABSTRACT FROM AUTHOR]

In this study, we report on the retrieval of aerosol extinction profiles from ground-based scattered sunlight multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, carried out at Athens, Greece. It is the first time that aerosol profiles are retrieved from MAX-DOAS measurements in Athens. The reported aerosol vertical distributions at 477 nm are derived from the oxygen dimer (O4) differential-slant-column-density observations at different elevation angles by applying the BRemen Optimal estimation REtrieval for Aerosol and trace gaseS (BOREAS) retrieval algorithm. Four case studies have been selected for validation purposes; the retrieved aerosol profiles and the corresponding aerosol optical depths (AODs) from the MAX-DOAS are compared with lidar extinction profiles and with sun-photometric measurements (Aerosol Robotic Network, AERONET, observations), respectively. Despite the different approach of each method regarding the retrieval of the aerosol information, the comparison with the lidar measurements at 532 nm reveals a very good agreement in terms of vertical distribution, with r>0.90 in all cases. The AODs from the MAX-DOAS and the sun photometer (the latter at 500 nm) show a satisfactory correlation (with 0.45 < r < 0.7 in three out of the four cases). The comparison indicates that the MAX-DOAS systematically underestimates the AOD in the cases of large particles (small Ångström exponent) and for measurements at small relative azimuthal angles between the viewing direction and the sun. Better agreement is achieved in the morning, at large relative azimuthal angles. Overall, the aerosol profiles retrieved from MAX-DOAS measurements are of good quality; thus, new perspectives are opened up for assessing urban aerosol pollution on a long-term basis in Athens from continuous and uninterrupted MAX-DOAS measurements. [ABSTRACT FROM AUTHOR]

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites – Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish realm) – and ozone-sonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models – a global chemistry transport model (parallelised-Tropospheric Offline Model of Chemistry and Transport, p-TOMCAT) and a global chemistry climate model (United Kingdom Chemistry and Aerosol, UKCA) – are used for model data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at Eureka, Canada, are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs; defined as ozone volume mixing ratios, VMRs, < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry. Modelled total inorganic bromine (Br Y) over the Arctic sea ice is sensitive to model configuration; e.g. under the same bromine loading, Br Y in the Arctic spring boundary layer in the p-TOMCAT control run (i.e. with all bromine emissions) can be 2 times that in the UKCA control run. Despite the model differences, both model control runs can successfully reproduce large bromine explosion events (BEEs) and ODEs in polar spring. Model-integrated tropospheric-column BrO generally matches GOME-2 tropospheric columns within ∼ 50 % in UKCA and a factor of 2 in p-TOMCAT. The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA production and bromide release on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. Note that this work dose not necessary rule out other possibilities that may act as a source of reactive bromine from the sea ice zone. [ABSTRACT FROM AUTHOR]

The evaluation of chemical transport models, CTMs, is essential for the assessment of their performance regarding the physical and chemical parameterizations used. While regional CTMs have been widely used and evaluated over Europe, their validation over Greece is limited. In this study, we investigate the performance of the LOTOS-EUROS v2.2.001 regional chemical transport model in simulating nitrogen dioxide, NO2, over Greece from June to December 2018. In-situ NO2 measurements obtained from the National Air Pollution Monitoring Network are compared with surface simulations over the two major cities of Greece, Athens and Thessaloniki. The model reproduces well the spatial variability of the measured NO2 with a spatial correlation coefficient of 0.85 for the period between June and December 2018. About half of the 14 air quality monitoring stations show a good temporal correlation to the simulations, higher than 0.6, during daytime (12–15 p.m. local time), while the corresponding biases are negative. Most stations show stronger negative biases during winter than in summer. Furthermore, the simulated tropospheric NO2 columns are evaluated against ground-based MAX-DOAS NO2 measurements and space-borne Sentinel 5-Precursor TROPOMI tropospheric NO2 observations in July and December 2018. LOTOS-EUROS captures better the NO2 temporal variability in December (0.61 and 0.81) than in July (0.50 and 0.21) when compared to the corresponding measurements of the MAX-DOAS instruments in Thessaloniki and the rural azimuth viewing direction in Athens respectively. The urban azimuth viewing direction in Athens region however shows a better correlation in July than in December (0.41 and 0.19, respectively). LOTOS-EUROS NO2 columns over Athens and Thessaloniki agree well with the TROPOMI observations showing higher spatial correlation in July (0.95 and 0.82, respectively) than in December (0.82 and 0.66, respectively) while the relative temporal correlations are higher during winter. Overall, the comparison of the simulations with the TROPOMI observations shows a model underestimation in summer and an overestimation in winter both in Athens and Thessaloniki. Updated emissions for the simulations and model improvements when extreme values of boundary layer height are encountered are further suggested. [ABSTRACT FROM AUTHOR]

Satellite observations have shown large areas of elevated bromine monoxide (BrO) covering several thousand square kilometres over the Arctic and Antarctic sea ice regions in polar spring. These enhancements of total BrO columns result from increases in stratospheric or tropospheric bromine amounts or both, and their occurrence may be related to local meteorological conditions. In this study, the spatial distribution of the occurrence of total BrO column enhancements and the associated changes in meteorological parameters are investigated in both the Arctic and Antarctic regions using 10 years of Global Ozone Monitoring Experiment-2 (GOME-2) measurements and meteorological model data. Statistical analysis of the data presents clear differences in the meteorological conditions between the 10-year mean and episodes of enhanced total BrO columns in both polar sea ice regions. These differences show pronounced spatial patterns. In general, atmospheric low pressure, cold surface air temperature, high surface-level wind speed, and low tropopause heights were found during periods of enhanced total BrO columns. In addition, spatial patterns of prevailing wind directions related to the BrO enhancements are identified in both the Arctic and Antarctic sea ice regions. The relevance of the different meteorological parameters on the total BrO column is evaluated based on a Spearman rank correlation analysis, finding that tropopause height and surface air temperature have the largest correlations with the total BrO vertical column density. Our results demonstrate that specific meteorological parameters can have a major impact on the BrO enhancement in some areas, but in general, multiple meteorological parameters interact with each other in their influence on BrO columns. [ABSTRACT FROM AUTHOR]

Every polar spring, phenomena called bromine explosions occur over sea ice. These bromine explosions comprise photochemical heterogeneous chain reactions that release bromine molecules, Br2 , to the troposphere and lead to tropospheric plumes of bromine monoxide, BrO. This autocatalytic mechanism depletes ozone, O3 , in the boundary layer and troposphere and thereby changes the oxidizing capacity of the atmosphere. The phenomenon also leads to accelerated deposition of metals (e.g., Hg). In this study, we present a 22-year (1996 to 2017) consolidated and consistent tropospheric BrO dataset north of 70 ∘ N, derived from four different ultraviolet–visible (UV–VIS) satellite instruments (GOME, SCIAMACHY, GOME-2A and GOME-2B). The retrieval data products from the different sensors are compared during periods of overlap and show good agreement (correlations of 0.82–0.98 between the sensors). From our merged time series of tropospheric BrO vertical column densities (VCDs), we infer changes in the bromine explosions and thus an increase in the extent and magnitude of tropospheric BrO plumes during the period of Arctic warming. We determined an increasing trend of about 1.5 % of the tropospheric BrO VCDs per year during polar springs, while the size of the areas where enhanced tropospheric BrO VCDs can be found has increased about 896 km 2 yr -1. We infer from comparisons and correlations with sea ice age data that the reported changes in the extent and magnitude of tropospheric BrO VCDs are moderately related to the increase in first-year ice extent in the Arctic north of 70 ∘ N, both temporally and spatially, with a correlation coefficient of 0.32. However, the BrO plumes and thus bromine explosions show significant variability, which also depends, apart from sea ice, on meteorological conditions. [ABSTRACT FROM AUTHOR]

The Airborne ROmanian Measurements of Aerosols and Trace gases (AROMAT) campaigns took place in Romania in September 2014 and August 2015. They focused on two sites: the Bucharest urban area and large power plants in the Jiu Valley. The main objectives of the campaigns were to test recently developed airborne observation systems dedicated to air quality studies and to verify their applicability for the validation of space-borne atmospheric missions such as the TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P). We present the AROMAT campaigns from the perspective of findings related to the validation of tropospheric NO2 , SO2 , and H2CO. We also quantify the emissions of NOx and SO2 at both measurement sites. We show that tropospheric NO2 vertical column density (VCD) measurements using airborne mapping instruments are well suited for satellite validation in principle. The signal-to-noise ratio of the airborne NO2 measurements is an order of magnitude higher than its space-borne counterpart when the airborne measurements are averaged at the TROPOMI pixel scale. However, we show that the temporal variation of the NO2 VCDs during a flight might be a significant source of comparison error. Considering the random error of the TROPOMI tropospheric NO2 VCD (σ), the dynamic range of the NO2 VCDs field extends from detection limit up to 37 σ (2.6×1016 molec. cm -2) and 29 σ (2 ×1016 molec. cm -2) for Bucharest and the Jiu Valley, respectively. For both areas, we simulate validation exercises applied to the TROPOMI tropospheric NO2 product. These simulations indicate that a comparison error budget closely matching the TROPOMI optimal target accuracy of 25 % can be obtained by adding NO2 and aerosol profile information to the airborne mapping observations, which constrains the investigated accuracy to within 28 %. In addition to NO2 , our study also addresses the measurements of SO2 emissions from power plants in the Jiu Valley and an urban hotspot of H2CO in the centre of Bucharest. For these two species, we conclude that the best validation strategy would consist of deploying ground-based measurement systems at well-identified locations. [ABSTRACT FROM AUTHOR]

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97 ∘ N, 4.93 ∘ E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques. [ABSTRACT FROM AUTHOR]

In this study, we report on the retrieval of aerosol extinction profiles from ground-based scattered sunlight multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, carried out at Athens, Greece. It is the first time that aerosol profiles are retrieved from MAX-DOAS measurements in Athens. The reported aerosol vertical distributions at 477 nm are derived from the oxygen dimer (O4) differential slant column density observations at different elevation angles by applying the BOREAS retrieval algorithm. Four case studies have been selected for validation purposes; the retrieved aerosol profiles and the corresponding aerosol optical depths (AODs) from the MAX-DOAS are compared with lidar extinction profiles and with sun photometric measurements (AERONET observations), respectively. Despite the different approach of each method regarding the retrieval of the aerosol information, the comparison with the lidar measurements at 532 nm reveals a very good agreement in terms of vertical distribution, with r > 0.85 in all cases. The AODs from the MAX-DOAS and the sun-photometer (the latter at 500 nm) show a satisfactory correlation (with r ≈ 0.6 in three out of the four cases). The comparison indicates that the MAX-DOAS systematically underestimates the AOD in the cases of large particles (small Ångström exponent) and for measurements at small relative azimuthal angles between the viewing direction and the Sun. Better agreement is achieved in the morning, at large relative azimuthal angles. Overall, the aerosol profiles retrieved from MAX-DOAS measurements are of good quality; thus, new perspectives are opened up for assessing urban aerosol pollution on a long term-basis in Athens from continuous and uninterrupted MAX-DOAS measurements. [ABSTRACT FROM AUTHOR]

Multi-axis differential optical absorption spectroscopy (MAX-DOAS) tropospheric NO2 column retrievals from four European measurement stations are compared to simulations from five regional air quality models which contribute to the European regional ensemble forecasts and reanalyses of the operational Copernicus Atmosphere Monitoring Service (CAMS). Compared to other observational data usually applied for regional model evaluation, MAX-DOAS data are closer to the regional model data in terms of horizontal and vertical resolution, and multiple measurements are available during daylight, so that, for example, diurnal cycles of trace gases can be investigated. In general, there is good agreement between simulated and retrieved NO2 column values for individual MAX-DOAS measurements with correlations between 35 % and 70 % for individual models and 45 % to 75 % for the ensemble median for tropospheric NO2 vertical column densities (VCDs), indicating that emissions, transport and tropospheric chemistry of NOx are on average well simulated. However, large differences are found for individual pollution plumes observed by MAX-DOAS. Most of the models overestimate seasonal cycles for the majority of MAX-DOAS sites investigated. At the urban stations, weekly cycles are reproduced well, but the decrease towards the weekend is underestimated and diurnal cycles are overall not well represented. In particular, simulated morning rush hour peaks are not confirmed by MAX-DOAS retrievals, and models fail to reproduce observed changes in diurnal cycles for weekdays versus weekends. The results of this study show that future model development needs to concentrate on improving representation of diurnal cycles and associated temporal scalings. [ABSTRACT FROM AUTHOR]

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites: Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish Realm), and ozonesonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models: a global chemistry transport model (p-TOMCAT) and a global chemistry climate model (UKCA), are used for model-data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based Multi-axis Differential Optical Absorption Spectroscopy (MAX-DOAS) at Eureka, Canada are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs) (defined as ozone volume mixing ratios VMRs < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry. Model bromine is sensitive to model configuration, e.g., under the same bromine loading, the total inorganic bromine (BrY) in the Arctic spring boundary layer in the p-TOMCAT base run (i.e., with all bromine emissions) can be 2 times larger than that in the UKCA base run. Despite the model differences, both model base runs can successfully reproduce large bromine explosion events (BEEs) in polar spring. Model-integrated tropospheric column BrO generally matches GOME-2 tropospheric columns within ~50 % (in the UKCA base run) and factors of 2–3 (in the p-TOMCAT base run). The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA and bromine production from blowing snow on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. [ABSTRACT FROM AUTHOR]

Glyoxal (CHOCHO) and formaldehyde (HCHO) are intermediate products in the tropospheric oxidation of the majority of volatile organic compounds (VOCs). CHOCHO is also a precursor of secondary organic aerosol (SOA) in the atmosphere. CHOCHO and HCHO are released from biogenic, anthropogenic, and pyrogenic sources. CHOCHO and HCHO tropospheric lifetimes are typically considered to be short during the daytime at mid-latitudes (e.g. several hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles or deposition. At night and at high latitudes, tropospheric lifetimes increase to many hours or even days. Previous studies demonstrated that CHOCHO and HCHO vertical column densities (VCDs) are well retrieved from space-borne observations using differential optical absorption spectroscopy (DOAS). In this study, we present CHOCHO and HCHO VCDs retrieved from measurements by TROPOMI (TROPOspheric Monitoring Instrument), launched on the Sentinel-5 Precursor (S5P) platform in October 2017. We observe strongly elevated amounts of CHOCHO and HCHO during the 2018 fire season in British Columbia, Canada, where a large number of fires occurred in August. CHOCHO and HCHO plumes from individual fire hot spots are observed in air masses travelling over distances of up to 1500 km , i.e. much longer than expected for the relatively short tropospheric lifetime expected for CHOCHO and HCHO. Comparison with simulations by the particle dispersion model FLEXPART (FLEXible PARTicle dispersion model) indicates that effective lifetimes of 20 h and more are needed to explain the observations of CHOCHO and HCHO if they decay in an effective first-order process. FLEXPART used in the study calculates accurately the transport. In addition an exponential decay, in our case assumed to be photochemical, of a species along the trajectory is added. We have used this simple approach to test our assumption that CHOCHO and HCHO are created in the fires and then decay at a constant rate in the plume as it is transported. This is clearly not the case and we infer that CHOCHO and HCHO are either efficiently recycled during transport or continuously formed from the oxidation of longer-lived precursors present in the plume, or possibly a mixture of both. We consider the best explanation of the observed CHOCHO and HCHO VCD in the plumes of the fire is that they are produced by oxidation of longer-lived precursors, which were also released by the fire and present in the plume. [ABSTRACT FROM AUTHOR]

The Airborne ROmanian Measurements of Aerosols and Trace gases (AROMAT) campaigns took place in Romania in September 2014 and August 2015. They focused on two sites: the Bucharest urban area and the power plants in the Jiu Valley. Their main objectives were to test recently developed airborne observation systems dedicated to air quality studies and to verify the concept of such campaigns in support of the validation of spaceborne atmospheric missions such as TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P). We show that tropospheric NO2 vertical column density (VCD) measurements using airborne mapping instruments are valuable for satellite validation. The signal to noise ratio of the airborne NO2 measurements is one order of magnitude higher than its spaceborne counterpart when the airborne measurements are averaged at the TROPOMI pixel scale. A significant source of comparison error appears to be the time variation of the NO2 VCDs during a flight, which we estimated at about 4 x 1015 molec cm-2 in the AROMAT conditions. Considering the random error of the TROPOMI tropospheric NO2 VCD (σ), the dynamic range of the NO2 VCDs field extends from detection limit up to 37σ (2.6 x 1016 molec cm-2) or 29σ (2 x 1016 molec cm-2) for Bucharest and the Jiu Valley, respectively. For the two areas, we simulate validation exercises of the TROPOMI tropospheric NO2 product using airborne measurements. These simulations indicate that we can closely approach the TROPOMI optimal target accuracy of 25 % by adding NO2 and aerosol profile information to the mapping data, which constrains the investigated accuracy within 28 %. In addition to NO2, we also measured significant amounts of SO² in the Jiu Valley, as well as a hotspot of H2CO in the center of Bucharest. For these two species, we conclude that the best validation strategy would consist in deploying ground-based measurement systems at key locations which the AROMAT observations help identify. [ABSTRACT FROM AUTHOR]

The large stocks of soil organic carbon (SOC) in soils and deposits of the northern permafrost region are sensitive to global warming and permafrost thawing. The potential release of this carbon (C) as greenhouse gases to the atmosphere does not only depend on the total quantity of soil organic matter (SOM) affected by warming and thawing, but it also depends on its lability (i.e., the rate at which it will decay). In this study we develop a simple and robust classification scheme of SOM lability for the main types of soils and deposits in the northern permafrost region. The classification is based on widely available soil geochemical parameters and landscape unit classes, which makes it useful for upscaling to the entire northern permafrost region. We have analyzed the relationship between C content and C- CO2 production rates of soil samples in two different types of laboratory incubation experiments. In one experiment, ca. 240 soil samples from four study areas were incubated using the same protocol (at 5 ∘ C, aerobically) over a period of 1 year. Here we present C release rates measured on day 343 of incubation. These long-term results are compared to those obtained from short-term incubations of ca. 1000 samples (at 12 ∘ C, aerobically) from an additional three study areas. In these experiments, C- CO2 production rates were measured over the first 4 d of incubation. We have focused our analyses on the relationship between C- CO2 production per gram dry weight per day (µ gC- CO2 gdw -1 d -1) and C content (%C of dry weight) in the samples, but we show that relationships are consistent when using C/N ratios or different production units such as µ gC per gram soil C per day (µ gC- CO2 gC -1 d -1) or per cm 3 of soil per day (µ gC- CO2 cm -3 d -1). C content of the samples is positively correlated to C- CO2 production rates but explains less than 50 % of the observed variability when the full datasets are considered. A partitioning of the data into landscape units greatly reduces variance and provides consistent results between incubation experiments. These results indicate that relative SOM lability decreases in the order of Late Holocene eolian deposits to alluvial deposits and mineral soils (including peaty wetlands) to Pleistocene yedoma deposits to C-enriched pockets in cryoturbated soils to peat deposits. Thus, three of the most important SOC storage classes in the northern permafrost region (yedoma, cryoturbated soils and peatlands) show low relative SOM lability. Previous research has suggested that SOM in these pools is relatively undecomposed, and the reasons for the observed low rates of decomposition in our experiments need urgent attention if we want to better constrain the magnitude of the thawing permafrost carbon feedback on global warming. [ABSTRACT FROM AUTHOR]

Satellite observations have shown large areas of elevated BrO covering several thousand km² over the Arctic and Antarctic sea ice region in polar spring. These enhancements of total BrO columns result from increases in stratospheric or tropospheric bromine amounts or both, and their occurrence may be related to local meteorological conditions. In this study, the spatial distribution of the occurrence of total BrO column enhancements and the associated changes in meteorological parameters are investigated in both the Arctic and Antarctic regions using 10 years of GOME-2 measurements in combination with meteorological model data. Statistical analysis of the data presents clear differences in the meteorological conditions between the 10 year mean and episodes of enhanced total BrO columns in both polar sea ice regions. These differences show pronounced spatial patterns. In general, atmospheric low pressure, cold surface air temperature, high surface-level wind speed and low tropopause heights were found during periods of enhanced total BrO columns. In addition, spatial patterns of prevailing wind directions related to the BrO enhancements are identified in both the Arctic and Antarctic sea ice region. The relevance of the different meteorological parameters for the total BrO column is evaluated based on a Spearman rank correlation analysis, finding that tropopause height and surface air temperature have the largest correlations with the total BrO vertical column density. Our results demonstrate that specific meteorological parameters can have a major impact on the BrO enhancement in some areas, but in general, multiple meteorological parameters interact with each other in their influence on BrO columns. [ABSTRACT FROM AUTHOR]

This study describes a novel application of an "onion-peeling" approach to multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of shipping emissions aiming at investigating the strong horizontal inhomogeneities in NO2 over a shipping lane. To monitor ship emissions on the main shipping route towards the port of Hamburg, a two-channel (UV and visible) MAX-DOAS instrument was deployed on the island Neuwerk in the German Bight, 6–7 km south of the main shipping lane. Utilizing the fact that the effective light path length in the atmosphere depends systematically on wavelength, simultaneous measurements and DOAS retrievals in the UV and visible spectral ranges are used to probe air masses at different horizontal distances to the instrument to estimate two-dimensional pollutant distributions. Two case studies have been selected to demonstrate the ability to derive the approximate plume positions in the observed area. A situation with northerly wind shows high NO2 concentrations close to the measurement site and low values in the north of the shipping lane. The opposite situation with southerly wind, unfavorable for the on-site in situ instrumentation, demonstrates the ability to detect enhanced NO2 concentrations several kilometers away from the instrument. Using a Gaussian plume model, in-plume NO2 volume mixing ratios can be derived from the MAX-DOAS measurements. For validation, a comparison to airborne imaging DOAS measurements during the NOSE campaign in July 2013 is performed, showing good agreement between the approximate plume position derived from the onion-peeling MAX-DOAS and the airborne measurements as well as between the derived in-plume NO2 volume mixing ratios (VMRs). [ABSTRACT FROM AUTHOR]

A novel imaging-DOAS (differential optical absorption spectroscopy) instrument IMPACT (Imaging MaPper for AtmospheriC observaTions) is presented combining full-azimuthal pointing (360 ∘) with a large vertical coverage (∼41 ∘). Complete panoramic scans are acquired at a temporal resolution of ∼15 min, enabling the retrieval of NO2 vertical profiles over the entire panorama around the measurement site. IMPACT showed excellent agreement (correlation >99 %) with coincident multiaxis DOAS (MAX-DOAS) measurements during the Second Cabauw Intercomparison of Nitrogen Dioxide measuring Instruments (CINDI-2) campaign. The temporal variability of NO2 slant columns within a typical MAX-DOAS vertical scanning sequence could be resolved and was as large as 20 % in a case study under good viewing conditions. The variation of corresponding profiles and surface concentrations was even larger (40 %). This variability is missed when retrieving trace gas profiles based on standard MAX-DOAS measurements. The azimuthal distribution of NO2 around the measurement site showed inhomogeneities (relative differences) up to 120 % (on average 35 %) on short timescales (individual panoramic scans). This is more than expected for the semirural location. We explain this behavior by the transport of pollution. Exploiting the instrument's advantages, the plume's trajectory during a prominent transport event could be reconstructed. Finally, the potential for retrieving information about the aerosol phase function from O4 slant columns along multiple almucantar scans of IMPACT is demonstrated, with promising results for future studies. [ABSTRACT FROM AUTHOR]

Glyoxal (CHO.CHO) and formaldehyde (HCHO) are intermediate products in the oxidation of the majority of volatile organic compounds (VOC). CHO.CHO is also a precursor of secondary organic aerosol (SOA) formation in the atmosphere. These VOCs are released from biogenic, anthropogenic, and pyrogenic sources. CHO.CHO and HCHO tropospheric lifetimes are short during the daytime and at mid-latitudes (few hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles/deposition. During nighttime or at high latitudes, lifetime can be prolonged to many hours or even days. Previous studies demonstrated that CHO.CHO and HCHO can be retrieved from space-borne observations using the DOAS method. In this study, we present CHO.CHO and HCHO columns retrieved from measurements of the TROPOMI instrument, launched recently on the Sentinel-5 Precursor (S5P) platform in October 2017. Strongly elevated amounts of CHO.CHO and HCHO are observed during the fire season in British Columbia Canada, where a large number of fires occurred in August 2018. CHO.CHO and HCHO plumes from individual fire hot-spots are observed in air masses travelling over distances of up to 1500 km, i.e. much longer than expected for the short atmospheric lifetime of CHO.CHO and HCHO. However, the temporal evolution of the plume differs for both species. Comparison with Lagrangian-based FLEXPART simulations for particles with different lifetimes shows that effective lifetimes of 20 hours and more are needed to explain the observations, indicating that CHO.CHO and HCHO are either efficiently recycled during transport or, continuously formed from the oxidation of longer-lived precursors present in the plume. [ABSTRACT FROM AUTHOR]

Trace gas maps retrieved from satellite measurements show enhanced levels of the atmospheric volatile organic compounds formaldehyde (HCHO) and glyoxal (CHOCHO) over the Atlantic Ocean. To validate the spatial distribution of this continental outflow, ship-based measurements were taken during the Continental Outflow of Pollutants towards the MArine tRoposphere (COPMAR) project. A Multi-AXis Differential Optical Absorption Spectrometer (MAX-DOAS) was operated aboard the research vessel (RV) Maria S. Merian during cruise MSM58/2. This cruise was conducted in October 2016 from Ponta Delgada (Azores) to Cape Town (South Africa), crossing between Cabo Verde and the African continent. The instrument was continuously scanning the horizon, looking towards the African continent. Enhanced levels of HCHO and CHOCHO were found in the area of expected outflow during this cruise. The observed spatial gradients of HCHO and CHOCHO along the cruise track agree with the spatial distributions from satellite measurements and the Model for OZone and Related chemical Tracers version 4 (MOZART-4) model simulations. The continental outflow from the African continent is observed in an elevated layer, higher than 1000 m, and probably originates from biogenic emissions or biomass burning according to FLEXible PARTicle dispersion model (FLEXPART) emission sensitivities. [ABSTRACT FROM AUTHOR]

Despite its key role in climate change, large uncertainties persist in our knowledge of the anthropogenic emissions of carbon dioxide (CO2) and no global observing system exists that allows us to monitor emissions from localized CO2 sources with sufficient accuracy. The Orbiting Carbon Observatory-2 (OCO-2) satellite allows retrievals of the column-average dry-air mole fractions of CO2 (XCO2). However, regional column-average enhancements of individual point sources are usually small, compared to the background concentration and its natural variability, and often not much larger than the satellite's measurement noise. This makes the unambiguous identification and quantification of anthropogenic emission plume signals challenging. NO2 is co-emitted with CO2 when fossil fuels are combusted at high temperatures. It has a short lifetime on the order of hours so that NO2 columns often greatly exceed background and noise levels of modern satellite sensors near sources, which makes it a suitable tracer of recently emitted CO2. Based on six case studies (Moscow, Russia; Lipetsk, Russia; Baghdad, Iraq; Medupi and Matimba power plants, South Africa; Australian wildfires; and Nanjing, China), we demonstrate the usefulness of simultaneous satellite observations of NO2 and XCO2. For this purpose, we analyze co-located regional enhancements of XCO2 observed by OCO-2 and NO2 from the Sentinel-5 Precursor (S5P) satellite and estimate the CO2 plume's cross-sectional fluxes. We take advantage of the nearly simultaneous NO2 measurements with S5P's wide swath and small measurement noise by identifying the source of the observed XCO2 enhancements, excluding interference with remote upwind sources, allowing us to adjust the wind direction, and by constraining the shape of the CO2 plumes. We compare the inferred cross-sectional fluxes with the Emissions Database for Global Atmospheric Research (EDGAR), the Open-Data Inventory for Anthropogenic Carbon dioxide (ODIAC), and, in the case of the Australian wildfires, with the Global Fire Emissions Database (GFED). The inferred cross-sectional fluxes range from 31 Mt CO2 a -1 to 153 Mt CO2 a -1 with uncertainties (1 σ) between 23 % and 72 %. For the majority of analyzed emission sources, the estimated cross-sectional fluxes agree, within their uncertainty, with either EDGAR or ODIAC or lie somewhere between them. We assess the contribution of multiple sources of uncertainty and find that the dominating contributions are related to the computation of the effective wind speed normal to the plume's cross section. The flux uncertainties are expected to be reduced by the planned European Copernicus anthropogenic CO2 monitoring mission (CO2M), which will provide not only precise measurements with high spatial resolution but also imaging capabilities with a wider swath of simultaneous XCO2 and NO2 observations. Such a mission, particularly if performed by a constellation of satellites, will deliver CO2 emission estimates from localized sources at an unprecedented frequency and level of accuracy. [ABSTRACT FROM AUTHOR]

We present different methods for in-field elevation calibration of MAX-DOAS (Multi AXis Differential Optical Absorption Spectroscopy) instruments that were applied and inter-compared during the second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2). One necessary prerequisite of consistent MAX-DOAS retrievals is a precise and accurate calibration of the elevation angles of the different measuring systems. Therefore, different methods for this calibration were applied to 12 instruments from 11 groups during the campaign and the results were inter-compared. This work first introduces and explains the different methods, namely far and near lamp measurements, white/bright stripe scans and horizon scans, using data and results for only one (mainly the MPIC) instrument. In the second part, the far lamp measurements and the horizon scans are examined for all participating groups. Here, the results for both methods are first inter-compared for the different instruments and secondly, the two methods are compared amongst each other. All methods turned out to be well-suited for the calibration of the elevation angles of MAX-DOAS systems, with each of them having individual advantages and drawbacks. Considering the results of this study, the uncertainties of the methods can be estimated as ± 0.05° for the far lamp measurements, ± 0.1° to ± 0.3° for the horizon scans, and around ± 0.1° for the white stripe and near lamp measurements. When comparing the results of far lamp and horizon scan measurements, a spread of around 1° in the elevation calibrations is found between the participating instruments for both methods. This spread is on the order of a typical field of view (FOV) of a MAX-DOAS instrument and therefore, affecting the retrieval results. Further, a consistent (wavelength dependent) offset of 0.31° and 0.40° between far lamp measurements and horizon scans is found, which can be explained by the fact that, despite the flat topography around the measurement site, obstacles such as trees might mark the visible horizon during daytime. The observed wavelength dependence can be explained by surface albedo effects. Lastly, the results are discussed and recommendations for future campaigns are given. [ABSTRACT FROM AUTHOR]

For more than 2 decades, satellite observations from instruments such as GOME, SCIAMACHY, GOME-2, and OMI have been used for the monitoring of bromine monoxide (BrO) distributions on global and regional scales. In October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) was launched on board the Copernicus Sentinel-5 Precursor platform with the goal of continuous daily global trace gas observations with unprecedented spatial resolution. In this study, sensitivity tests were performed to find an optimal wavelength range for TROPOMI BrO retrievals under various measurement conditions. From these sensitivity tests, a wavelength range for TROPOMI BrO retrievals was determined and global data for April 2018 as well as for several case studies were retrieved. Comparison with GOME-2 and OMI BrO retrievals shows good consistency and low scatter of the columns. The examples of individual TROPOMI overpasses show that due to the better signal-to-noise ratio and finer spatial resolution of 3.5×7 km2 , TROPOMI BrO retrievals provide good data quality with low fitting errors and unique information on small-scale variabilities in various BrO source regions such as Arctic sea ice, salt marshes, and volcanoes. [ABSTRACT FROM AUTHOR]

The large stocks of soil organic carbon (SOC) in soils and deposits of the northern permafrost region are sensitive to global warming and permafrost thawing. The potential release of this carbon (C) as greenhouse gases to the atmosphere does not only depend on the total quantity of soil organic matter (SOM) affected by warming and thawing, but also on its lability (i.e. the rate at which it will decay). In this study we develop a simple and robust classification scheme of SOM lability for the main types of soils and deposits of the northern permafrost region. The classification is based on widely available soil geochemical parameters and landscape unit classes, which makes it useful for upscaling to the entire northern permafrost region. We have analyzed the relationship between C content and C-CO2 production rates of soil samples in two different types of laboratory incubation experiment. In one experiment, c. 240 soil samples from four study areas were incubated using the same protocol (at 5°C, aerobically) over a period of one year. Here we present C release rates measured on day 343 of incubation. These long-term results are compared to those obtained from short-term incubations of c. 1000 samples (at 12°C, aerobically) from an additional three study areas. In these experiments, C-CO2 production rates were measured over the first four days of incubation. We have focused our analyses on the relationship between C-CO2 production per gram dry weight per day (µgC-CO2gdw-1d-1) and C content (%C of dry weight) in the samples, but show that relationships are consistent when using C/N ratios or different production units such as µgC per gram soil C per day (µgC-CO2gC-1d-1) or per cm of soil per day (µgC-CO2cm3-1d-1). C content of the samples is positively correlated to C-CO2 production rates but explains less than 50% of the observed variability when the full datasets are considered. A partitioning of the data into landscape units greatly reduces variance and provides consistent results between incubation experiments. These results indicate that relative SOM lability decreases in the order: Late Holocene eolian deposits > alluvial deposits and mineral upland soils (including peaty wetlands) > Pleistocene Yedoma deposits > C-enriched pockets in cryoturbated soils > peat deposits. Thus, three of the most important SOC storage classes in the northern permafrost region (Yedoma, cryoturbated soils and peatlands) show low relative SOM lability. Previous research has suggested that SOM in these pools is relatively undecomposed and the reasons for the observed resistance to decomposition in our experiments needs urgent attention if we want to better constrain the magnitude of the thawing permafrost carbon feedback on global warming. [ABSTRACT FROM AUTHOR]

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 days during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, The Netherlands (51.97° N, 4.93° E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were to characterise and better understand the differences between a large number of Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, to discuss the performance of the various types of instruments and to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen dimer (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region and NO2 in an additional (smaller) wavelength range in the visible. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in an unprecedented set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the reference, and the RMS error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the measurement performance of all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques. [ABSTRACT FROM AUTHOR]