ALBERT

Description: The Paris megacity experiences frequent particulate matter (i.e.PM2.5, particulate matter with a diameter less than 2.5 µm) pollution episodes in spring (March–April). At this time of the year, large numbers of the particles consist of ammonium sulfate and nitrate which are formed from ammonia (NH3) released during fertilizer spreading practices and transported from the surrounding areas to Paris. There is still limited knowledge of the emission sources around Paris, their magnitude, and their seasonality. Using space-borne NH3 observation records of 10 years (2008–2017) and 5 years (2013–2017) provided by the Infrared Atmospheric Sounding Interferometer (IASI) and the Cross-Track Infrared Sounder (CrIS) instrument, regional patterns of NH3 variabilities (seasonal and interannual) are derived. Observations reveal identical high seasonal variability with three major NH3 hotspots found from March to August. The high interannual variability is discussed with respect to atmospheric total precipitation and temperature. A detailed analysis of the seasonal cycle is performed using both IASI and CrIS instrument data, together with outputs from the CHIMERE atmospheric model. For 2014 and 2015, the CHIMERE model shows coefficients of determination of 0.58 and 0.18 when compared to IASI and CrIS, respectively. With respect to spatial variability, the CHIMERE monthly NH3 concentrations in spring show a slight underrepresentation over Belgium and the United Kingdom and an overrepresentation in agricultural areas in the French Brittany–Pays de la Loire and Plateau du Jura region, as well as in northern Switzerland. In addition, PM2.5 concentrations derived from the CHIMERE model have been evaluated against surface measurements from the Airparif network over Paris, with which agreement was found (r2 = 0.56) with however an underestimation during spring pollution events. Using HYSPLIT cluster analysis of back trajectories, we show that NH3 total columns measured in spring over Paris are enhanced when air masses originate from the north-east (e.g. the Netherlands and Belgium), highlighting the importance of long-range transport in the NH3 budget over Paris. Variability in NH3 in the north-east region is likely to impact NH3 concentrations in the Parisian region since the cross-correlation function is above 0.3 (at lag = 0 and 1 d). Finally, we quantify the key meteorological parameters driving the specific conditions important for the formation of PM2.5 from NH3 in the Île-de-France region in spring. Data-driven results based on surface PM2.5 measurements from the Airparif network and IASI NH3 measurements show that a combination of the factors such as a low boundary layer of ∼500 m, a relatively low temperature of 5 ∘C, a high relative humidity of 70 %, and wind from the north-east contributes to a positive PM2.5 and NH3 correlation.

Description: Satellite remote sensing of the Earth's atmospheric composition usually samples irregularly in space and time, and many applications require spatially and temporally averaging the satellite observations (level 2) to a regular grid (level 3). When averaging level 2 data over a long period to a target level 3 grid that is significantly finer than the sizes of level 2 pixels, this process is referred to as “oversampling”. An agile, physics-based oversampling approach is developed to represent each satellite observation as a sensitivity distribution on the ground, instead of a point or a polygon as assumed in previous methods. This sensitivity distribution can be determined by the spatial response function of each satellite sensor. A generalized 2-D super Gaussian function is proposed to characterize the spatial response functions of both imaging grating spectrometers (e.g., OMI, OMPS, and TROPOMI) and scanning Fourier transform spectrometers (e.g., GOSAT, IASI, and CrIS). Synthetic OMI and IASI observations were generated to compare the errors due to simplifying satellite fields of view (FOVs) as polygons (tessellation error) and the errors due to discretizing the smooth spatial response function on a finite grid (discretization error). The balance between these two error sources depends on the target grid size, the ground size of the FOV, and the smoothness of spatial response functions. Explicit consideration of the spatial response function is favorable for fine-grid oversampling and smoother spatial response. For OMI, it is beneficial to oversample using the spatial response functions for grids finer than ∼16 km. The generalized 2-D super Gaussian function also enables smoothing of the level 3 results by decreasing the shape-determining exponents, which is useful for a high noise level or sparse satellite datasets. This physical oversampling approach is especially advantageous during smaller temporal windows and shows substantially improved visualization of trace gas distribution and local gradients when applied to OMI NO2 products and IASI NH3 products. There is no appreciable difference in the computational time when using the physical oversampling versus other oversampling methods.

Description: Recently, Whitburn et al.(2016) presented a neural-network-based algorithm for retrieving atmospheric ammonia (NH3) columns from Infrared Atmospheric Sounding Interferometer (IASI) satellite observations. In the past year, several improvements have been introduced, and the resulting new baseline version, Artificial Neural Network for IASI (ANNI)-NH3-v2.1, is documented here. One of the main changes to the algorithm is that separate neural networks were trained for land and sea observations, resulting in a better training performance for both groups. By reducing and transforming the input parameter space, performance is now also better for observations associated with favourable sounding conditions (i.e. enhanced thermal contrasts). Other changes relate to the introduction of a bias correction over land and sea and the treatment of the satellite zenith angle. In addition to these algorithmic changes, new recommendations for post-filtering the data and for averaging data in time or space are formulated. We also introduce a second dataset (ANNI-NH3-v2.1R-I) which relies on ERA-Interim ECMWF meteorological input data, along with surface temperature retrieved from a dedicated network, rather than the operationally provided Eumetsat IASI Level 2 (L2) data used for the standard near-real-time version. The need for such a dataset emerged after a series of sharp discontinuities were identified in the NH3 time series, which could be traced back to incremental changes in the IASI L2 algorithms for temperature and clouds. The reanalysed dataset is coherent in time and can therefore be used to study trends. Furthermore, both datasets agree reasonably well in the mean on recent data, after the date when the IASI meteorological L2 version 6 became operational (30 September 2014).

Description: Vegetation fires are a major source of ammonia (NH3) in the atmosphere. Their emissions are mainly estimated using bottom-up approaches that rely on uncertain emission factors. In this study, we derive new biome-specific NH3 enhancement ratios relative to carbon monoxide (CO), ERNH3 ∕ CO (directly related to the emission factors), from the measurements of the IASI sounder onboard the Metop-A satellite. This is achieved for large tropical regions and for an 8-year period (2008–2015). We find substantial differences in the ERNH3 ∕ CO ratios between the biomes studied, with calculated values ranging from 7  ×  10−3 to 23  ×  10−3. For evergreen broadleaf forest these are typically 50–75 % higher than for woody savanna and savanna biomes. This variability is attributed to differences in fuel types and size and is in line with previous studies. The analysis of the spatial and temporal distribution of the ERNH3 ∕ CO ratio also reveals a (sometimes large) within-biome variability. On a regional level, woody savanna shows, for example, a mean ERNH3 ∕ CO ratio for the region of Africa south of the Equator that is 40–75 % lower than in the other five regions studied, probably reflecting regional differences in fuel type and burning conditions. The same variability is also observed on a yearly basis, with a peak in the ERNH3 ∕ CO ratio observed for the year 2010 for all biomes. These results highlight the need for the development of dynamic emission factors that take into better account local variations in fuel type and fire conditions. We also compare the IASI-derived ERNH3 ∕ CO ratio with values reported in the literature, usually calculated from ground-based or airborne measurements. We find general good agreement in the referenced ERNH3 ∕ CO ratio except for cropland, for which the ERNH3 ∕ CO ratio shows an underestimation of about 2–2.5 times.

Description: Volcanic eruptions impact climate through the injection of sulfur dioxide (SO2), which is oxidized to form sulfuric acid aerosol particles that can enhance the stratospheric aerosol optical depth (SAOD). Besides large-magnitude eruptions, moderate-magnitude eruptions such as Kasatochi in 2008 and Sarychev Peak in 2009 can have a significant impact on stratospheric aerosol and hence climate. However, uncertainties remain in quantifying the atmospheric and climatic impacts of the 2009 Sarychev Peak eruption due to limitations in previous model representations of volcanic aerosol microphysics and particle size, whilst biases have been identified in satellite estimates of post-eruption SAOD. In addition, the 2009 Sarychev Peak eruption co-injected hydrogen chloride (HCl) alongside SO2, whose potential stratospheric chemistry impacts have not been investigated to date. We present a study of the stratospheric SO2–particle–HCl processing and impacts following Sarychev Peak eruption, using the Community Earth System Model version 1.0 (CESM1) Whole Atmosphere Community Climate Model (WACCM) – Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics model (with no a priori assumption on particle size). The Sarychev Peak 2009 eruption injected 0.9 Tg of SO2 into the upper troposphere and lower stratosphere (UTLS), enhancing the aerosol load in the Northern Hemisphere. The post-eruption evolution of the volcanic SO2 in space and time are well reproduced by the model when compared to Infrared Atmospheric Sounding Interferometer (IASI) satellite data. Co-injection of 27 Gg HCl causes a lengthening of the SO2 lifetime and a slight delay in the formation of aerosols, and acts to enhance the destruction of stratospheric ozone and mono-nitrogen oxides (NOx) compared to the simulation with volcanic SO2 only. We therefore highlight the need to account for volcanic halogen chemistry when simulating the impact of eruptions such as Sarychev on stratospheric chemistry. The model-simulated evolution of effective radius (reff) reflects new particle formation followed by particle growth that enhances reff to reach up to 0.2 µm on zonal average. Comparisons of the model-simulated particle number and size distributions to balloon-borne in situ stratospheric observations over Kiruna, Sweden, in August and September 2009, and over Laramie, USA, in June and November 2009 show good agreement and quantitatively confirm the post-eruption particle enhancement. We show that the model-simulated SAOD is consistent with that derived from the Optical Spectrograph and InfraRed Imager System (OSIRIS) when both the saturation bias of OSIRIS and the fact that extinction profiles may terminate well above the tropopause are taken into account. Previous modelling studies (involving assumptions on particle size) that reported agreement with (biased) post-eruption estimates of SAOD derived from OSIRIS likely underestimated the climate impact of the 2009 Sarychev Peak eruption.

Description: This paper presents decadal simulations of stratospheric and tropospheric aerosol and its radiative effects by the chemistry general circulation model EMAC constrained with satellite observations in the framework of the ESA Aerosol CCI project such as GOMOS (Global Ozone Monitoring by Occultation of Stars) and (A)ATSR ((Advanced) Along Track Scanning Radiometer) on the ENVISAT (European Environmental Satellite), IASI (Infrared Atmospheric Sounding Interferometer) on MetOp (Meteorological Operational Satellite), and, additionally, OSIRIS (Optical Spectrograph and InfraRed Imaging System). In contrast to most other studies, the extinctions and optical depths from the model are compared to the observations at the original wavelengths of the satellite instruments covering the range from the UV (ultraviolet) to terrestrial IR (infrared). This avoids conversion artifacts and provides additional constraints for model aerosol and interpretation of the observations. MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) SO2 limb measurements are used to identify plumes of more than 200 volcanic eruptions. These three-dimensional SO2 plumes are added to the model SO2 at the eruption times. The interannual variability in aerosol extinction in the lower stratosphere, and of stratospheric aerosol radiative forcing at the tropopause, is dominated by the volcanoes. To explain the seasonal cycle of the GOMOS and OSIRIS observations, desert dust simulated by a new approach and transported to the lowermost stratosphere by the Asian summer monsoon and tropical convection turns out to be essential. This also applies to the radiative heating by aerosol in the lowermost stratosphere. The existence of wet dust aerosol in the lowermost stratosphere is indicated by the patterns of the wavelength dependence of extinction in observations and simulations. Additional comparison with (A)ATSR total aerosol optical depth at different wavelengths and IASI dust optical depth demonstrates that the model is able to represent stratospheric as well as tropospheric aerosol consistently.

Description: After 43 years of inactivity, the Calbuco volcano, which is located in the southern part of Chile, erupted on 22 April 2015. The space–time evolutions (distribution and transport) of its aerosol plume are investigated by combining satellite (CALIOP, IASI, OMPS), in situ aerosol counting (LOAC OPC) and lidar observations, and the MIMOSA advection model. The Calbuco aerosol plume reached the Indian Ocean 1 week after the eruption. Over the Reunion Island site (21° S, 55.5° E), the aerosol signal was unambiguously enhanced in comparison with background conditions, with a volcanic aerosol layer extending from 18 to 21 km during the May–July period. All the data reveal an increase by a factor of  ∼  2 in the SAOD (stratospheric aerosol optical depth) with respect to values observed before the eruption. The aerosol mass e-folding time is approximately 90 days, which is rather close to the value ( ∼  80 days) reported for the Sarychev eruption. Microphysical measurements obtained before, during, and after the eruption reflecting the impact of the Calbuco eruption on the lower stratospheric aerosol content have been analyzed over the Reunion Island site. During the passage of the plume, the volcanic aerosol was characterized by an effective radius of 0.16 ± 0.02 µm with a unimodal size distribution for particles above 0.2 µm in diameter. Particle concentrations for sizes larger than 1 µm are too low to be properly detected by the LOAC OPC. The aerosol number concentration was  ∼  20 times higher that observed before and 1 year after the eruption. According to OMPS and lidar observations, a tendency toward conditions before the eruption was observed by April 2016. The volcanic aerosol plume is advected eastward in the Southern Hemisphere and its latitudinal extent is clearly bounded by the subtropical barrier and the polar vortex. The transient behavior of the aerosol layers observed above Reunion Island between May and July 2015 reflects an inhomogeneous spatio-temporal distribution of the plume, which is controlled by the localization of these dynamical barriers.

Description: Air pollution reaching hazardous levels in many Chinese cities has been a major concern in China over the past decades. New policies have been applied to regulate anthropogenic pollutant emissions, leading to changes in atmospheric composition and in particulate matter (PM) production. Increasing levels of atmospheric ammonia columns have been observed by satellite during recent years. In particular, observations from the Infrared Atmospheric Sounding Interferometer (IASI) reveal an increase of these columns by 15 % and 65 % from 2011 to 2013 and 2015, respectively, over eastern China. In this paper we performed model simulations for 2011, 2013 and 2015 in order to understand the origin of this increase and to quantify the link between ammonia and the inorganic components of particles: NH4(p)+/SO4(p)2-/NO3(p)-. Interannual change of meteorology can be excluded as a reason: year 2015 meteorology leads to enhanced sulfate production over eastern China, which increases the ammonium and decreases the ammonia content, which is contrary to satellite observations. Reductions in SO2 and NOx emissions from 2011 to 2015 of 37.5 % and 21 % respectively, as constrained from satellite data, lead to decreased inorganic matter (by 14 % for NH4(p)++SO4(p)2-+NO3(p)-). This in turn leads to increased gaseous NH3(g) tropospheric columns by as much as 24 % and 49 % (sampled corresponding to IASI data availability) from 2011 to 2013 and 2015 respectively and thus can explain most of the observed increase.

Description: Concentrated agricultural activities and animal feeding operations in the northeastern plains of Colorado represent an important source of atmospheric ammonia (NH3). The NH3 from these sources contributes to regional fine particle formation and to nitrogen deposition to sensitive ecosystems in Rocky Mountain National Park (RMNP), located  ∼  80 km to the west. In order to better understand temporal and spatial differences in NH3 concentrations in this source region, weekly concentrations of NH3 were measured at 14 locations during the summers of 2010 to 2015 using Radiello passive NH3 samplers. Weekly (biweekly in 2015) average NH3 concentrations ranged from 2.66 to 42.7 µg m−3, with the highest concentrations near large concentrated animal feeding operations (CAFOs). The annual summertime mean NH3 concentrations were stable in this region from 2010 to 2015, providing a baseline against which concentration changes associated with future changes in regional NH3 emissions can be assessed. Vertical profiles of NH3 were also measured on the 300 m Boulder Atmospheric Observatory (BAO) tower throughout 2012. The highest NH3 concentration along the vertical profile was always observed at the 10 m height (annual average concentration of 4.63 µg m−3), decreasing toward the surface (4.35 µg m−3) and toward higher altitudes (1.93 µg m−3). The NH3 spatial distributions measured using the passive samplers are compared with NH3 columns retrieved by the Infrared Atmospheric Sounding Interferometer (IASI) satellite and concentrations simulated by the Comprehensive Air Quality Model with Extensions (CAMx). The satellite comparison adds to a growing body of evidence that IASI column retrievals of NH3 provide very useful insight into regional variability in atmospheric NH3, in this case even in a region with strong local sources and sharp spatial gradients. The CAMx comparison indicates that the model does a reasonable job simulating NH3 concentrations near sources but tends to underpredict concentrations at locations farther downwind. Excess NH3 deposition by the model is hypothesized as a possible explanation for this trend.

Description: As a precursor of atmospheric aerosols, ammonia (NH3) is one of the primary gaseous air pollutants. Given its short atmospheric lifetime, ambient NH3 concentrations are dominated by local sources. In a recent study, Van Damme et al. (2018) have highlighted the importance of NH3 point sources, especially those associated with feedlots and industrial ammonia production. Their emissions were shown to be largely underestimated in bottom-up emission inventories. The discovery was made possible thanks to the use of oversampling techniques applied to 9 years of global daily IASI NH3 satellite measurements. Oversampling allows one to increase the spatial resolution of averaged satellite data beyond what the satellites natively offer. Here we apply for the first time superresolution techniques, which are commonplace in many fields that rely on imaging, to measurements of an atmospheric sounder, whose images consist of just single pixels. We demonstrate the principle on synthetic data and on IASI measurements of a surface parameter. Superresolution is a priori less suitable to be applied on measurements of variable atmospheric constituents, in particular those affected by transport. However, by first applying the wind-rotation technique, which was introduced in the study of other primary pollutants, superresolution becomes highly effective in mapping NH3 at a very high spatial resolution. We show that plume transport can be revealed in greater detail than what was previously thought to be possible. Next, using this wind-adjusted superresolution technique, we introduce a new type of NH3 map that allows tracking down point sources more easily than the regular oversampled average. On a subset of known emitters, the source could be located within a median distance of 1.5 km. We subsequently present a new global point-source catalog consisting of more than 500 localized and categorized point sources. Compared to our previous catalog, the number of identified sources more than doubled. In addition, we refined the classification of industries into five categories – fertilizer, coking, soda ash, geothermal and explosives industries – and introduced a new urban category for isolated NH3 hotspots over cities. The latter mainly consists of African megacities, as clear isolation of such urban hotspots is almost never possible elsewhere due to the presence of a diffuse background with higher concentrations. The techniques presented in this paper can most likely be exploited in the study of point sources of other short-lived atmospheric pollutants such as SO2 and NO2.