Stratosphere-troposphere separation of nitrogen dioxide columns from the TEMPO geostationary satellite instrument

Separating the stratospheric and tropospheric contributions in satellite retrievals of atmospheric NO2 column abundance is a crucial step in the interpretation and application of the satellite observations. A variety of stratosphere–troposphere separation algorithms have been developed for sun-synchronous instruments in low Earth orbit (LEO) that benefit from global coverage, including broad clean regions with negligible tropospheric NO2 compared to stratospheric NO2. These global sun-synchronous algorithms need to be evaluated and refined for forthcoming geostationary instruments focused on continental regions, which lack this global context and require hourly estimates of the stratospheric column. Here we develop and assess a spatial filtering algorithm for the upcoming TEMPO geostationary instrument that will target North America. Developments include using independent satellite observations to identify likely locations of tropospheric enhancements, using independent LEO observations for spatial context, consideration of diurnally varying partial fields of regard, and a filter based on stratospheric to tropospheric air mass factor ratios. We test the algorithm with LEO observations from the OMI instrument with an afternoon overpass, and from the GOME-2 instrument with a morning overpass. We compare our TEMPO field of regard algorithm against an identical global algorithm to investigate the penalty resulting from the limited spatial coverage in geostationary orbit, and find excellent agreement in the estimated mean daily tropospheric NO2 column densities (R2=0.999, slope=1.009 for July and R2=0.998, slope=0.999 for January). The algorithm performs well even when only small parts of the continent are observed by TEMPO. The algorithm is challenged the most by east coast morning retrievals in the wintertime (e.g., R2=0.995, slope=1.038 at 14:00 UTC). We find independent global LEO observations (corrected for time of day) provide important context near the field-of-regard edges. We also test the performance of the TEMPO algorithm without these supporting global observations. Most of the continent is unaffected (R2=0.924 and slope=0.973 for July and R2=0.996 and slope=1.008 for January), with 90 % of the pixels having differences of less than ±0.2×1015 molecules cm−2 between the TEMPO tropospheric NO2 column density and the global algorithm. For near-real-time retrieval, even a climatological estimate of the stratospheric NO2 surrounding the field of regard would improve this agreement. In general, the additional penalty of a limited field of regard from TEMPO introduces no more error than normally expected in most global stratosphere–troposphere separation algorithms. Overall, we conclude that hourly near-real-time stratosphere–troposphere separation for the retrieval of NO2 tropospheric column densities by the TEMPO geostationary instrument is both feasible and robust, regardless of the diurnally varying limited field of regard.The authors are grateful to Kelly Chance, Xiong Liu, John Houck, Peter Zoogman, and other members of the TEMPO trace gas retrieval team for their input in preparation of this paper. Work at Dalhousie University was supported by Environment and Climate Change Canada. The authors also gratefully acknowledge the free use of TEMIS NO2 data from the GOME-2 sensor provided by http://www.temis.nl, last access: 12 November 2018, and the NASA Standard Product NO2 data from OMI provided by https://disc.gsfc.nasa.gov/datasets/OMNO2_V003/summary, last access: 9 November 2018. (Environment and Climate Change Canada)https://www.atmos-meas-tech.net/11/6271/2018/Published versio

Lessons Learned from OMI Observations of Point Source SO2 Pollution

The Ozone Monitoring Instrument (OMI) on NASA Aura satellite makes global daily measurements of the total column of sulfur dioxide (SO2), a short-lived trace gas produced by fossil fuel combustion, smelting, and volcanoes. Although anthropogenic SO2 signals may not be detectable in a single OMI pixel, it is possible to see the source and determine its exact location by averaging a large number of individual measurements. We describe new techniques for spatial and temporal averaging that have been applied to the OMI SO2 data to determine the spatial distributions or "fingerprints" of SO2 burdens from top 100 pollution sources in North America. The technique requires averaging of several years of OMI daily measurements to observe SO2 pollution from typical anthropogenic sources. We found that the largest point sources of SO2 in the U.S. produce elevated SO2 values over a relatively small area - within 20-30 km radius. Therefore, one needs higher than OMI spatial resolution to monitor typical SO2 sources. TROPOMI instrument on the ESA Sentinel 5 precursor mission will have improved ground resolution (approximately 7 km at nadir), but is limited to once a day measurement. A pointable geostationary UVB spectrometer with variable spatial resolution and flexible sampling frequency could potentially achieve the goal of daily monitoring of SO2 point sources and resolve downwind plumes. This concept of taking the measurements at high frequency to enhance weak signals needs to be demonstrated with a GEOCAPE precursor mission before 2020, which will help formulating GEOCAPE measurement requirements

Assessing Snow Extent Data Sets over North America to Inform and Improve Trace Gas Retrievals from Solar Backscatter

Accurate representation of surface reflectivity is essential to tropospheric trace gas retrievals from solar backscatter observations. Surface snow cover presents a significant challenge due to its variability and thus snow-covered scenes are often omitted from retrieval data sets; however, the high reflectance of snow is potentially advantageous for trace gas retrievals. We first examine the implications of surface snow on retrievals from the upcoming TEMPO geostationary instrument for North America. We use a radiative transfer model to examine how an increase in surface reflectivity due to snow cover changes the sensitivity of satellite retrievals to NO2 in the lower troposphere. We find that a substantial fraction (>50%) of the TEMPO field of regard can be snow covered in January, and that the average sensitivity to the tropospheric NO2 column substantially increases (doubles) when the surface is snow covered. We then evaluate seven existing satellite-derived or reanalysis snow extent products against ground station observations over North America to assess their capability of informing surface conditions for TEMPO retrievals. The Interactive Multisensor Snow and Ice Mapping System (IMS) had the best agreement with ground observations (accuracy of 93%, precision of 87%, recall of 83%). Multiangle Implementation of Atmospheric Correction (MAIAC) retrievals of MODIS-observed radiances had high precision (90% for Aqua and Terra), but underestimated the presence of snow (recall of 74% for Aqua, 75% for Terra). MAIAC generally outperforms the standard MODIS products (precision of 51%, recall of 43% for Aqua; precision of 69%, recall of 45% for Terra). The Near-real-time Ice and Snow Extent (NISE) product had good precision (83%) but missed a significant number of snow-covered pixels (recall of 45%). The Canadian Meteorological Centre (CMC) Daily Snow Depth Analysis Data set had strong performance metrics (accuracy of 91%, precision of 79%, recall of 82%). We use the F score, which balances precision and recall, to determine overall product performance (F = 85%, 82(82)%, 81%, 58%, 46(54)% for IMS, MAIAC Aqua(Terra), CMC, NISE, MODIS Aqua(Terra) respectively) for providing snow cover information for TEMPO retrievals from solar backscatter observations. We find that using IMS to identify snow cover and enable inclusion of snow-covered scenes in clear-sky conditions across North America in January can increase both the number of observations by a factor of 2.1 and the average sensitivity to the tropospheric NO2 column by a factor of 2.7

Effect of volcanic aerosol on stratospheric NO₂ and N₂O₅ from 2002-2014 as measured by Odin-OSIRIS and Envisat-MIPAS

Following the large volcanic eruptions of Pinatubo in 1991 and El Chichón in 1982, decreases in stratospheric NO₂ associated with enhanced aerosol were observed. The Optical Spectrograph and Infrared Imaging Spectrometer (OSIRIS) measured the widespread enhancements of stratospheric aerosol following seven volcanic eruptions between 2002 and 2014, although the magnitudes of these eruptions were all much smaller than the Pinatubo and El Chichón eruptions. In order to isolate and quantify the relationship between volcanic aerosol and NO₂, NO₂ anomalies were calculated using measurements from OSIRIS and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). In the tropics, variability due to the quasi-biennial oscillation was subtracted from the time series. OSIRIS profile measurements indicate that the strongest anticorrelations between NO₂ and volcanic aerosol extinction were for the 5 km layer starting  ∼  3 km above the climatological mean tropopause at the given latitude. OSIRIS stratospheric NO₂ partial columns in this layer were found to be smaller than background NO₂ levels during these aerosol enhancements by up to  ∼  60 % with typical Pearson correlation coefficients of R ∼ −0. 7. MIPAS also observed decreases in NO₂ partial columns during periods affected by volcanic aerosol, with percent differences of up to  ∼  25 % relative to background levels. An even stronger anticorrelation was observed between OSIRIS aerosol optical depth and MIPAS N₂O₅ partial columns, with R ∼ −0. 9, although no link with MIPAS HNO3 was observed. The variation in OSIRIS NO₂ with increasing aerosol was found to be consistent with simulations from a photochemical box model within the estimated model uncertainty

Estimation of anthropogenic and volcanic SO2 emissions from satellite data in the presence of snow/ice on the ground

Early versions of satellite nadir-viewing UV SO2 data products did not explicitly account for the effects of snow/ice on retrievals. Snow-covered terrain, with its high reflectance in the UV, typically enhances satellite sensitivity to boundary layer pollution. However, a significant fraction of high-quality cloud-free measurements over snow is currently excluded from analyses. This leads to increased uncertainties of satellite emission estimates and potential seasonal biases due to the lack of data in winter months for some high-latitudinal sources. In this study, we investigated how Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) satellite SO2 measurements over snow-covered surfaces can be used to improve the annual emissions reported in our SO2 emissions catalogue (version 2; Fioletov et al., 2023). Only 100 out of 759 sources listed in the catalogue have 10 % or more of the observations over snow. However, for 40 high-latitude sources, more than 30 % of measurements suitable for emission calculations were made over snow-covered surfaces. For example, in the case of Norilsk, the world's largest SO2 point-source, annual emission estimates in the SO2 catalogue were based only on 3–4 summer months, while the addition of data for snow conditions extends that period to 7 months. Emissions in the SO2 catalogue were based on satellite measurements of SO2 slant column densities (SCDs) that were converted to vertical column densities (VCDs) using site-specific clear-sky air mass factors (AMFs), calculated for snow-free conditions. The same approach was applied to measurements with snow on the ground whereby a new set of constant, site-specific, clear sky with snow AMFs was created, and these were applied to the measured SCDs. Annual emissions were then estimated for each source considering (i) only clear-sky and snow-free days, (ii) only clear-sky with snow days, and (iii) a merged dataset (snow and snow-free conditions). For individual sources, the difference between emissions estimated for snow and snow-free conditions is within ±20 % for three-quarters of smelters and oil and gas sources and with practically no systematic bias. This is excellent consistency given that there is typically a factor of 3–5 difference between AMFs for snow and snow-free conditions. For coal-fired power plants, however, emissions estimated for snow conditions are on average 25 % higher than for snow-free conditions; this difference is likely real and due to larger production (consumption of coal) and emissions in wintertime.</p

Validation of ACE-FTS Version 3.5 NOy Species Profiles Using Correlative Satellite Measurements

The ACE-FTS (Atmospheric Chemistry Experiment - Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NOy (N + NO + NO2 + NO3 + 2 x N2O5 + HNO3 + HNO4 + ClONO2 + BrONO2) species. Version 2.2 of ACE-FTS NO, NO2, HNO3, N2O5, and ClONO2 has previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments - GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NOy species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25-50 km, ACE-FTS typically agrees with correlative data to within -10%. Instrument-averaged mean relative differences are approximately -10% at 30-40 km for NO2, within ± 7% at 8-30km for HNO3, better than -7 % at 21-34 km for local morning N205, and better than -8% at 21-34 km for ClONO2. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed

Version 2 of the global catalogue of large anthropogenic and volcanic SO2 sources and emissions derived from satellite measurements

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI), Ozone Mapping and Profiler Suite (OMPS), and TROPOspheric Monitoring Instrument (TROPOMI) satellite spectrometers were used to update and extend the previously developed global catalogue of large SO2 emission sources. This version 2 of the global catalogue covers the period of 2005-2021 and includes a total of 759 continuously emitting point sources releasing from about 10 ktyr-1 to more than 4000 ktyr-1 of SO2, that have been identified and grouped by country and primary source origin: volcanoes (106 sources); power plants (477); smelters (74); and sources related to the oil and gas industry (102). There are several major improvements compared to the original catalogue: it combines emissions estimates from three satellite instruments instead of just OMI, uses a new version 2 of the OMI and OMPS SO2 dataset, and updated consistent site-specific air mass factors (AMFs) are used to calculate SO2 vertical column densities (VCDs). The newest TROPOMI SO2 data processed with the Covariance-Based Retrieval Algorithm (COBRA), used in the catalogue, can detect sources with emissions as low as 8 ktyr-1 (in 2018-2021) compared to the 30 ktyr-1 limit for OMI. In general, there is an overall agreement within ±12 % in total emissions estimated from the three satellite instruments for large regions. For individual emission sources, the spread is larger: the annual emissions estimated from OMI and TROPOMI agree within ±13 % in 50 % of cases and within ±28 % in 90 % of cases. The version 2 catalogue emissions were calculated as a weighted average of emission estimates from the three satellite instruments using an inverse-variance weighting method. OMI, OMPS, and TROPOMI data contribute 7 %, 5 %, and 88 % to the average, respectively, for small (\u3c30 \u3ektyr-1) sources and 33 %, 20 %, and 47 %, respectively, for large (\u3e300 ktyr-1) sources. The catalogue data show an approximate 50 % decline in global SO2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years. The version 2 of the global catalogue has been posted at the NASA global SO2 monitoring website (10.5067/MEASURES/SO2/DATA406, Fioletov et al., 2022)

Multiscale computational analysis of Xenopus laevis morphogenesis reveals key insights of systems-level behavior

<p>Abstract</p> <p>Background</p> <p>Tissue morphogenesis is a complex process whereby tissue structures self-assemble by the aggregate behaviors of independently acting cells responding to both intracellular and extracellular cues in their environment. During embryonic development, morphogenesis is particularly important for organizing cells into tissues, and although key regulatory events of this process are well studied in isolation, a number of important systems-level questions remain unanswered. This is due, in part, to a lack of integrative tools that enable the coupling of biological phenomena across spatial and temporal scales. Here, we present a new computational framework that integrates intracellular signaling information with multi-cell behaviors in the context of a spatially heterogeneous tissue environment.</p> <p>Results</p> <p>We have developed a computational simulation of mesendoderm migration in the <it>Xenopus laevis </it>explant model, which is a well studied biological model of tissue morphogenesis that recapitulates many features of this process during development in humans. The simulation couples, via a JAVA interface, an ordinary differential equation-based mass action kinetics model to compute intracellular Wnt/β-catenin signaling with an agent-based model of mesendoderm migration across a fibronectin extracellular matrix substrate. The emergent cell behaviors in the simulation suggest the following properties of the system: maintaining the integrity of cell-to-cell contact signals is necessary for preventing fractionation of cells as they move, contact with the Fn substrate and the existence of a Fn gradient provides an extracellular feedback loop that governs migration speed, the incorporation of polarity signals is required for cells to migrate in the same direction, and a delicate balance of integrin and cadherin interactions is needed to reproduce experimentally observed migratory behaviors.</p> <p>Conclusion</p> <p>Our computational framework couples two different spatial scales in biology: intracellular with multicellular. In our simulation, events at one scale have quantitative and dynamic impact on events at the other scale. This integration enables the testing and identification of key systems-level hypotheses regarding how signaling proteins affect overall tissue-level behavior during morphogenesis in an experimentally verifiable system. Applications of this approach extend to the study of tissue patterning processes that occur during adulthood and disease, such as tumorgenesis and atherogenesis.</p

A New Global Anthropogenic SO2 Emission Inventory for the Last Decade: A Mosaic of Satellite-Derived and Bottom-Up Emissions

Sulfur dioxide (SO2) measurements from the Ozone Monitoring Instrument (OMI) satellite sensor have been used to detect emissions from large point sources. Emissions from over 400 sources have been quantified individually based on OMI observations, accounting for about a half of total reported anthropogenic SO2 emissions. Here we report a newly developed emission inventory, OMI-HTAP, by combining these OMI-based emission estimates and the conventional bottom-up inventory, HTAP, for smaller sources that OMI is not able to detect. OMI-HTAP includes emissions from OMI-detected sources that are not captured in previous leading bottom-up inventories, enabling more accurate emission estimates for regions with such missing sources. In addition, our approach offers the possibility of rapid updates to emissions from large point sources that can be detected by satellites. Our methodology applied to OMI-HTAP can also be used to merge improved satellite-derived estimates with other multi-year bottom-up inventories, which may further improve the accuracy of the emission trends. OMI-HTAP SO2 emissions estimates for Persian Gulf, Mexico, and Russia are 59%, 65%, and 56% larger than HTAP estimates, respectively, in year 2010. We have evaluated the OMI-HTAP inventory by performing simulations with the Goddard Earth Observing System version 5 (GEOS-5) model. The GEOS-5 simulated SO2 concentrations driven by both HTAP and OMI-HTAP were compared against in situ measurements. We focus for the validation on year 2010 for which HTAP is most valid and for which a relatively large number of in situ measurements are available. Results show that the OMI-HTAP inventory improves the agreement between the model and observations, in particular over the US, with the normalized mean bias decreasing from 0.41 (HTAP) to -0.03 (OMI-HTAP) for year 2010. Simulations with the OMI-HTAP inventory capture the worldwide major trends of large anthropogenic SO2 emissions that are observed with OMI. Correlation coefficients of the observed and modelled surface SO2 in 2014 increase from 0.16 (HTAP) to 0.59 (OMI-HTAP) and the normalized mean bias dropped from 0.29 (HTAP) to 0.05 (OMI-HTAP), when we updated 2010 HTAP emissions with 2014 OMI-HTAP emissions in the model