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At least 55 records · Page 3

Chain Formation as a Mechanism for Mass-Independent Fractionation of Sulfur Isotopes in the Archean Atmosphere

The anomalous abundances of sulfur isotopes in ancient sediments provide the strongest evidence for an anoxic atmosphere prior to ∼2.45 Ga, but the mechanism for producing this 'mass-independent' fractionation pattern remains in question. The prevailing hypothesis has been that it is created by differences in the UV photolysis rates of different SO2 isotopologues. We investigate here a recently proposed additional source of fractionation during gas-phase formation of elemental sulfur (S4 and S8). Because two minor S isotopes rarely occur in the same chain, the longer S4 and S8 chains should be strongly, and roughly equally, depleted in all minor isotopes. This gives rise to negative ∆(sup 33) S values and positive ∆(sub 36) S values in elemental sulfur-just the opposite of (and much larger than) what is predicted from SO2 photolysis itself. Back-reactions during chain formation, specifically photolysis of S2 and S3, pass sulfur having the opposite fractionation back to atomic S, and thence to other sulfur species, causing H2S, SO2, sulfate, and short-chain elemental sulfur to have positive ∆(sup 33) S and negative ∆(sup 36) S. Positive ∆(sup 33) S values in elemental sulfur produced in laboratory SO2 photolysis experiments could be caused by the initial fractionation during photolysis, combined with rapid condensation of short-chain sulfur species on the walls of the reaction chamber, along with a scarcity of back-reactions. The simulated fractionations produced by the chain formation mechanism do not directly match fractionations from the rock record. The mismatch might be explained if the isotopic signals leaving the atmosphere were significantly modulated by life, by uncertainties in the rates of reactions of both major and minor isotopic sulfur species, or by the relatively large potential range of atmospheric parameters. Further work is needed to better constrain these uncertainties, but this novel mechanism suggests new avenues to explore in our search for a explanation for the S-MIF record.

Great Oxidation Event↗

Chain Formation as a Mechanism for Mass-Independent Fractionation of Sulfur Isotopes in the Archean Atmosphere

The anomalous abundances of sulfur isotopes in ancient sediments provide the strongest evidence for an anoxic atmosphere prior to ∼2.45 Ga, but the mechanism for producing this ‘mass-independent’ fractionation pattern remains in question. The prevailing hypothesis has been that it is created by differences in the UV photolysis rates of different SO2 isotopologues. We investigate here a recently proposed additional source of fractionation during gas-phase formation of elemental sulfur (S4 and S8). Because two minor S isotopes rarely occur in the same chain, the longer S4 and S8 chains should be strongly, and roughly equally, depleted in all minor isotopes. This gives rise to negative Δ(exp 33)S values and positive Δ(exp 33)S values in elemental sulfur—just the opposite of (and much larger than) what is predicted from SO2 photolysis itself. Back-reactions during chain formation, specifically photolysis of S2 and S3, pass sulfur having the opposite fractionation back to atomic S, and thence to other sulfur species, causing H2S, SO2, sulfate, and short-chain elemental sulfur to have positive Δ(exp 33)S and negative Δ(exp 33)S. Positive Δ(exp 33)S values in elemental sulfur produced in laboratory SO2 photolysis experiments could be caused by the initial fractionation during photolysis, combined with rapid condensation of short-chain sulfur species on the walls of the reaction chamber, along with a scarcity of back-reactions. The simulated fractionations produced by the chain formation mechanism do not directly match fractionations from the rock record. The mismatch might be explained if the isotopic signals leaving the atmosphere were significantly modulated by life, by uncertainties in the rates of reactions of both major and minor isotopic sulfur species, or by the relatively large potential range of atmospheric parameters. Further work is needed to better constrain these uncertainties, but this novel mechanism suggests new avenues to explore in our search for a explanation for the S-MIF record.

C. E. Harman↗

Application of a coupled aerosol formation: Radiative transfer model to climatic studies of aerosols

A sophisticated one dimensional physical-chemical model of the formation and evolution of stratospheric aerosols was used to predict the size and number concentration of the stratospheric aerosols as functions of time and altitude following: a large volcanic eruption; increased addition of carbonyl sulfide (OCS) or sulfur dioxide (SO2) to the troposphere; increased supersonic aircraft (SST) flights in the stratosphere; and, large numbers of space shuttle (SS) flights through the stratosphere. A radiative-convective one dimensional climate sensitivity study, using the results of the aerosol formation model, was performed to assess the ground level climatic significance of these perturbations to the stratospheric aerosol layer. Volcanic eruptions and large OCS or SO2 increases could cause significant climatic changes. Currently projected SS launches and moderate fleets of SST's are unlikely to upset the stratospheric aerosol layer enough to significantly impact climate.

Toon, O. B.↗

Charged Particle Alterations of Surfaces in the Solar System

The surfaces of 'airless' bodies in the solar system are exposed to the ambient plasma, micrometeorites, and the solar UV. The effects of these space weathering agents on surfaces in the solar system has been studied in this project. In the last three years work was carried out on volatile depletion at Mars, on sputtering of the lunar surface, on absorption by implanted S in vapor-deposited H2O and its relevance to observations of Europa's surface in the UV, and on the spectral changes produced on irradiating SO2 and its possible relevance to Io. In addition, the role of plasma-induced charging of E-ring grains was evaluated because of its relevance to E-ring particle source and the lifetime of the E-ring. Finally, the detection of sputtered material from Dione by the CAPS instrument on CASSINI was evaluated as a tool for analysis of satellite surface composition, and the role of sputtering on the ambient OH in the vicinity of the ice satellites and the E-ring was evaluated.

Johnson, R. E.↗

Characterizing the Phyllosilicates and Amorphous Phases Found by MSL Using Laboratory XRD and EGA Measurements of Natural and Synthetic Materials

The Curiosity Rover landed on the Peace Vallis alluvial fan in Gale crater on August 5, 2012. A primary mission science objective is to search for past habitable environments, and, in particular, to assess the role of past water. Identifying the minerals and mineraloids that result from aqueous alteration at Gale crater is essential for understanding past aqueous processes at the MSL landing site and hence for interpreting the site's potential habitability. X-ray diffraction (XRD) data from the CheMin instrument and evolved gas analyses (EGA) from the SAM instrument have helped the MSL science team identify phases that resulted from aqueous processes: phyllosilicates and amorphous phases were measure in two drill samples (John Klein and Cumberland) obtained from the Sheepbed Member, Yellowknife Bay Fm., which is believed to represent a fluvial-lacustrine environment. A third set of analyses was obtained from scoop samples from the Rocknest sand shadow. Chemical data from the APXS instrument have helped constrain the chemical compositions of these secondary phases and suggest that the phyllosilicate component is Mg-enriched and the amorphous component is Fe-enriched, relatively Si-poor, and S- and H-bearing. To refine the phyllosilicate and amorphous components in the samples measured by MSL, we measured XRD and EGA data for a variety of relevant natural terrestrial phyllosilicates and synthetic mineraloids in laboratory testbeds of the CheMin and SAM instruments. Specifically, Mg-saturated smectites and vermiculites were measured with XRD at low relative humidity to understand the behavior of the 001 reflections under Mars-like conditions. Our laboratory XRD measurements suggest that interlayer cation composition affects the hydration state of swelling clays at low RH and, thus, the 001 peak positions. XRD patterns of synthetic amorphous materials, including allophane, ferrihydrite, and hisingerite were used in full-pattern fitting (FULLPAT) models to help determine the types and abundances of amorphous phases in the martian rocks and sand shadow. These models suggest that the rocks and sand shadow are composed of approx 30% amorphous phases. Sulfate-adsorbed allophane and ferrihydrite were measured by EGA to further understand the speciation of the sulfur present in the amorphous component. These data indicate that sulfate adsorbed onto the surfaces of amorphous phases could explain a portion of the SO2 evolution in the Rocknest SAM data. The additional constraints placed on the mineralogy and chemistry of the aqueous alteration phases through our laboratory measurements can help us better understand the nature of the fluids that affected the different samples and devise a history of aqueous alteration for the Sheepbed Member of the Yellowknife Bay Fm. at Gale crater.

Rampe, Elizabeth B.↗

Kinetic studies of the reaction of the SO radical with NO2 and ClO from 210 to 363 K

The rates of the reactions of the SO radical with NO2 and ClO (significant in the upper atmosphere of earth and Venus) were determined in a discharge flow system near 1 torr pressure with detection of radical and molecular species using collision-free sampling mass spectrometry. The rate constants were obtained from the decay of SO radicals in the presence of an excess of NO2 and ClO. The NO2 reaction was examined between 210 and 363 K and found to be temperature invariant: SO + NO2 yields SO2 + NO; k1 = (1.37 + or - 0.10) x 10 to the -11th cu cm/s. In addition, the ClO reaction was observed to be independent of temperature between 248 and 363 K: SO + ClO yields SO2 + Cl; k2 = (3.22 + or - 0.48) x 10 to the -11th cu cm/s. A comparison was made with previous investigations of these reactions at room temperature and with other radical-radical reactions involving SO or ClO.

Brunning, J.↗

Satellite measurements of the backscattered ultraviolet to determine ozone trends, volcanic SO2, and nitric oxide

Measurements of the atmospheric backscattered UV albedo have been used from satellites for more than 20 years to measure ozone. The longest continuous record has been from the Solar Backscattered Ultraviolet instrument (SBUV) and TOMS on the Nimbus 7 satellite, which have been in operation since November of 1978. Because of degradation in space of the diffuser plate used to measure extraterrestrial solar flux, it has been necessary to develop new techniques to maintain the calibration of these instruments. Calibration is maintained by requiring that ozone measured by different wavelength pairs be consistent, and by requiring that ozone measured at different solar zenith angles be consistent. This technique of using a geophysical quantity, ozone, as a transfer standard for wavelength calibration is very powerful. The recalibrated data have been used to measure total ozone trends to an accuracy of +/- 1.3 percent 2(sigma) error over ten years. No significant trends are found near the equator, but significant trends larger than predicted by homogeneous chemistry are found at middle to high latitudes in both hemispheres. In addition, UV albedo data have been used to measure SO2 using band structure in the 300-310 nm range, and to measure nitric oxide in the upper stratosphere and mesosphere using the (10) and (02) NO gamma band fluorescence features.

Mcpeters, Richard↗

Perturbations in Stratospheric Aerosol Evolution Due to the Water-Rich Plume of the 2022 Hunga-Tonga Eruption

The January 2022 Hunga Tonga-Hunga Ha'apai (HTHH) volcanic eruption injected a relatively small amount of SO2, but significantly more water into the stratosphere than previously seen in the modern satellite record. Here we show that the large amount of water resulted in large perturbations to stratospheric aerosol evolution. Our Community Earth System Model simulation reproduces the enhanced water vapor observed by the Microwave Limb Sounder at pressure levels between 10 and 50 hPa for three months. Compared with a simulation without a water injection, this additional source of water vapor increases OH, which halves the SO2 lifetime. Subsequent coagulation creates larger sulfate particles that double the stratospheric aerosol optical depth. A seasonal forecast of volcanic plume transport in the southern hemisphere indicates this eruption will greatly enhance the aerosol surface area and water vapor near the polar vortex until at least October 2022, suggesting that there will continue to be an impact of the HTHH eruption on the climate system.

Atmospheric science↗

Profiling the SO2 Plume from Volcan Turrialba: Ticosonde Balloon Measurements Compared with OMI and OMPS Retrievals

The summit of Volcan Turrialba (elev. 3340 m) lies less than 50 km upstream in the prevailing easterlies from the Ticosonde balloon launch site at San Jose, Costa Rica, where ECC ozone sondes have been launched regularly since 2005. In 2006 we began to see telltale notches in the ozone profiles in the altitude range between 2 and 6 km. Given the proximity of Turrialba, it seemed likely that SO2 in the volcano's plume was interfering in the chemical reaction in the ECC ozone sonde used to detect ozone. In early 2010, fumarolic activity in the Turrialba crater increased strongly, and the profile notches in our soundings increased in frequency as well, consistent with this hypothesis. In February 2012 we tested a dual ECC sonde system, where an additional sonde is flown on the same payload using a selective SO2 filter. The difference of the measurements in the dual sonde is a direct measure of the amount of SO2 encountered. This first dual sonde passed through the plume, and the data indicated a tropospheric SO2 column of 1.4 DU, comparing favorably with a total column of 1.7 DU in the OMI 3-km linear fit (LF) product at the sonde profile location and at nearly the same time. We are now launching dual sondes on a regular basis with 18 launches in the first 12 months through July 2014; 11 of these have detectable SO2 signals. These soundings have great potential for validation of the Aura OMI and the Suomi-NPP OMPS retrievals of SO2. Here we present the sonde measurements and compare them with two satellite datasets: the Aura OMI Linear Fit (LF) product and the Suomi-NPP OMPS Principal Components Analysis (PCA) boundary layer product. The PCA algorithm reduces retrieval noise and artifacts by more accurately accounting for various interferences in SO2 retrievals such as O3 absorption and rotational Raman scattering. The comparisons with the in situ observations indicate a significant improvement of the PCA algorithm in capturing relatively weak volcanic SO2 signals.

sondes↗

Formation and Stability of Radiation Products in Europa's Icy Shell

Spectra of Europa reveal a surface dominated by water-ice along with hydrated materials and minor amounts of SO2, CO2, and H2O2. Jovian magnetospheric ions (protons, sulfur, and oxygen) and electrons produce significant chemical modifications of the surface on time scales of a few years at micrometer depths. Our laboratory studies examine the formation and stability of radiation products in H2O-rich ices relevant to Europa. Infrared (IR) spectra of ices before and after irradiation reveal the radiation destruction of molecules and the formation of products at 86 - 132 K. In addition, spectra of ices during warming track thermal evolution due to chemical changes and sublimation processes. IR-identified radiation products in 86 - 132 K irradiated H2O + SO2 ices are the bisulfate ion, HSO4(-), sulfate ion, SO4(2-) and the hydronium ion, H3O(+). Warming results in the formation of a residual spectrum similar to liquid sulfuric acid, H2SO4, for H2O:SO2 ratios of 30:1, whereas hydrated sulfuric acid, H2SO4 4 H2O, forms for ratios of 30:1. Radiation products identified for irradiated H2O + H2S ices at 86 K are H2S2 and SO2. When irradiated at 110 and 132 K, ices with H2O:H2S ratios if either 3:1 or 30:1 show the formation of H2SO4 4 H2O on warming to 175 K. We have also examined the radiation stability of H2SO4. Addition of CO2 to H2O + SO2 ices results in the formation of CO3 at 2046 cm (sup -1) (4.89 m). This is the strongest band from a carbon-containing product in the mid-IR spectral region, and it is also seen when either pure CO2 or H2O + CO2 ice is irradiated. Experiments with CH4 added to H2O + SO2 + CO2 ices addressed the question of methane's use as a marker of methanogens in an irradiated ice environment. New results on the near-IR spectrum of pure H2O2 will be included in this presentation. Interpretations of near-IR water bands, with H2O2 present, will be discussed. Irradiations of H2O2 and H2O + H2O2 mixtures, to examine the possibility of O2 and O3 formation, are currently under investigation and new results will be discussed.

Moore, M. H.↗

An ultraviolet video technique for visualization of stack plumes and for measuring sulfur dioxide concentration and effluent velocity

Absorption spectroscopy utilizing a video sensing technique was investigated as a means of visualizing SO2 in power plant stack plumes and for measuring SO2 concentration and effluent velocity in these plumes. The absorption of SO2 is measured in the ultraviolet region by using the sky as a background source. An additional spectral channel is used to correct for particulate scattering encountered in coal fired power plant plumes. The video system also tracks fluctuations in the SO2 concentration which leads to the determination of an eddy convection velocity. Field measurements were performed to show that the eddy convection velocity is proportional to the average in-stack velocity and to empirically determine their relationship. It was concluded that the video absorption technique is an attractive method for remotely determining both SO2 concentration and plume velocity with the same instrument.

Exton, R. J.↗

Continuation of Long-Term Global SO2 Pollution Monitoring from OMI to OMPS

Over the past 20 years, advances in satellite remote sensing of pollution-relevant species have made space-borne observations an increasingly important part of atmospheric chemistry research and air quality management. This progress has been facilitated by advanced UV-vis spectrometers, such as the Ozone Monitoring Instrument (OMI) on board the NASA Earth Observing System (EOS) Aura satellite, and continues with new instruments, such as the Ozone Mapping and Profiler Suite (OMPS) on board the NASA-NOAA Suomi National Polar-orbiting Partnership (SNPP) satellite. In this study, we demonstrate that it is possible, using our state-of-the-art principal component analysis (PCA) retrieval technique, to continue the long-term global SO2 pollution monitoring started by OMI with the current and future OMPS instruments that will fly on the NOAA Joint Polar Satellite System (JPSS) 1, 2, 3, and 4 satellites in addition to SNPP, with a very good consistency of retrievals from these instruments. Since OMI SO2 data have been primarily used for (1) providing regional context on air pollution and long-range transport on a daily basis and (2) providing information on point emission sources on an annual basis after data averaging, we focused on these two aspects in our OMI-OMPS comparisons. Four years of retrievals (2012-2015) have been compared for three regions: eastern China, Mexico, and South Africa. In general, the comparisons show relatively high correlations (r = 0. 79-0.96) of daily regional averaged SO2 mass between the two instruments and near-unity regression slopes (0.76-0.97). The annual averaged SO2 loading differences between OMI and OMPS are small (< 0.03 Dobson unit (DU) over South Africa and up to 0.1 DU over eastern China). We also found a very good correlation (r = 0. 92-0.97) in the spatial distribution of annual averaged SO2 between OMI and OMPS over the three regions during 2012-2015. The emissions from ∼ 400 SO2 sources calculated with the two instruments also show a very good correlation (r = ∼ 0.9) in each year during 2012-2015. OMPS-detected SO2 point source emissions are slightly lower than those from OMI, but OMI-OMPS differences decrease with increasing strength of source. The OMI-OMPS SO2 mass differences on a pixel by pixel (daily) basis in each region can show substantial differences. The two instruments have a spatial correlation coefficient of 0.7 or better on < ∼ 50 % of the days. It is worth noting that consistent SO2 retrievals were achieved without any explicit adjustments to OMI or OMPS radiance data and that the retrieval agreement may be further improved by introducing a more comprehensive Jacobian lookup table than is currently used.

satellite remote sensing of pollution↗

The composition of the Martian atmosphere - Minor constituents.

The Mariner 6 and 7 infrared spectrometers provided data which, in principle, determine upper limits on the possible atmospheric abundance of every gaseous substance that was undetected but which has recognized absorptions in the accessible spectral region, 1.9 to 14.4 microns. Through supporting laboratory determinations of curves of growth under pressure-broadening conditions appropriate to Mars, upper limits can be specified (expressed first in cm-atm, STP, for a vertical column and then in parts per million) for NO2, NH3, C3O2, SO2, OCS, NO, O3, CH4, N2O, HCL, HBr, and H2S. In addition, considerations of band contours, moments of inertia, and experimental absorption coefficients make it possible to place useful upper limits on 27 additional substances that were not detected and for which curves of growth have not been measured.

Horn, D.↗

Instrumentation Working Group Summary

The Instrumentation Working Group compiled a summary of measurement techniques applicable to gas turbine engine aerosol precursors and particulates. An assessment was made of the limits, accuracy, applicability, and technology readiness of the various techniques. Despite advances made in emissions characterization of aircraft engines, uncertainties still exist in the mechanisms by which aerosols and particulates are produced in the near-field engine exhaust. To adequately assess current understanding of the formation of sulfuric acid aerosols in the exhaust plumes of gas turbine engines, measurements are required to determine the degree and importance of sulfur oxidation in the turbine and at the engine exit. Ideally, concentrations of all sulfur species would be acquired, with emphasis on SO2 and SO3. Numerous options exist for extractive and non-extractive measurement of SO2 at the engine exit, most of which are well developed. SO2 measurements should be performed first to place an upper bound on the percentage of SO2 oxidation. If extractive and non-extractive techniques indicate that a large amount of the fuel sulfur is not detected as SO2, then efforts are needed to improve techniques for SO3 measurements. Additional work will be required to account for the fuel sulfur in the engine exhaust. Chemical Ionization Mass Spectrometry (CI-MS) measurements need to be pursued, although a careful assessment needs to be made of the sampling line impact on the extracted sample composition. Efforts should also be placed on implementing non-intrusive techniques and extending their capabilities by maximizing exhaust coverage for line-of-sight measurements, as well as development of 2-D techniques, where feasible. Recommendations were made to continue engine exit and combustor measurements of particulates. Particulate measurements should include particle size distribution, mass fraction, hydration properties, and volatile fraction. However, methods to ensure that unaltered samples are obtained need to be developed. Particulate speciation was also assigned a high priority for quantifying the fractions of carbon soot, PAH, refractory materials, metals, sulfates, and nitrates. High priority was also placed on performing a comparison of particle sizing instruments. Concern was expressed by the workshop attendees who routinely make particulate measurements about the variation in number density measured during in-flight tests by different instruments. In some cases, measurements performed by different groups of researchers during the same flight tests showed an order of magnitude variation. Second priority was assigned to measuring concentrations of odd hydrogen and oxidizing species. Since OH, HO2, H2O2, and O are extremely reactive, non-extractive measurements are recommended. A combination of absorption and fluorescence is anticipated to be effective for OH measurements in the combustor and at the engine exit. Extractive measurements of HO2 have been made in the stratosphere, where the ambient level of OH is relatively low. Use of techniques that convert HO2 to OH for combustor and engine exit measurements needs to be evaluated, since the ratio of HO2/OH may be 1% or less at both the combustor and engine exit. CI-MS might be a viable option for H2O2, subject to sampling line conversion issues. However, H2O2 is a low priority oxidizing species in the combustor and at the engine exit. Two candidates for atomic oxygen measurements are Resonance Enhanced Multi-Photon Ionization (REMPI) and Laser-Induced Fluorescence (LIF). Particulate measurement by simultaneous extractive and non-extractive techniques was given equal priority to the oxidizer measurements. Concern was expressed over the ability of typical ground test sampling lines to deliver an unaltered sample to a remotely located instrument. It was suggested that the sampling probe and line losses be checked out by attempting measurements using an optical or non-extractive technique immediately upstream of the sampling probe. This is a possible application for Laser Induced Incandescence (LII) as a check on the volume fraction of soot. Optical measurements of size distribution are not well developed for ultrafine particles less than about 20 nm in diameter, so a non-extractive technique for particulate size distribution cannot be recommended without further development. Carbon dioxide measurements need to be made to complement other extractive measurement techniques. CO2 measurements enable conversion of other species concentrations to emission indices. Carbon monoxide, which acts as a sink for oxidizing species, should be measured using non-extractive techniques. CO can be rapidly converted to CO2 in extractive probes, and a comparison between extractive and non-extractive measurements should be performed. Development of non-extractive techniques would help to assess the degree of CO conversion, and might be needed to improve the concentration measurement accuracy. Measurements of NO(x) will continue to be critical due to the role of NO and NO2 in atmospheric chemistry, and their influence on atmospheric ozone. Time-resolved measurements of temperature, velocity, and species concentrations were included on the list of desired measurement. Thermocouples are typically adequate for engine exit measurements. PIV and LDV are well established for obtaining velocity profiles. The techniques are listed in the accompanying table; are divided into extractive and non-extractive techniques. Efforts were made to include a measurement uncertainty for each technique. An assessment of the technology readiness was included.

Zaller, Michelle↗

Recent Results from Galileo PPR at Io: Orbits I31 and I32

Recent Galileo PPR (Photo-Polarimeter Radiometer) results will be shown, including global day and nighttime maps, high latitude regional maps, and high-resolution scans across hotspots and from pole to pole. SO2 vapor pressure, global heatflow, and hotspot power outputs are estimated. Additional information is contained in the original extended abstract.

Rathbun, J. A.↗

EOS-Aura's Ozone Monitoring Instrument (OMI): Validation Requirements

OMI is an advanced hyperspectral instrument that measures backscattered radiation in the UV and visible. It will be flown as part of the EOS Aura mission and provide data on atmospheric chemistry that is highly synergistic with other Aura instruments HIRDLS, MLS, and TES. OMI is designed to measure total ozone, aerosols, cloud information, and UV irradiances, continuing the TOMS series of global mapped products but with higher spatial resolution. In addition its hyperspectral capability enables measurements of trace gases such as SO2, NO2, HCHO, BrO, and OClO. A plan for validation of the various OM1 products is now being formulated. Validation of the total column and UVB products will rely heavily on existing networks of instruments, like NDSC. NASA and its European partners are planning aircraft missions for the validation of Aura instruments. New instruments and techniques (DOAS systems for example) will need to be developed, both ground and aircraft based. Lidar systems are needed for validation of the vertical distributions of ozone, aerosols, NO2 and possibly SO2. The validation emphasis will be on the retrieval of these products under polluted conditions. This is challenging because they often depend on the tropospheric profiles of the product in question, and because of large spatial variations in the troposphere. Most existing ground stations are located in, and equipped for, pristine environments. This is also true for almost all NDSC stations. OMI validation will need ground based sites in polluted environments and specially developed instruments, complementing the existing instrumentation.

Brinksma, E. J.↗

Cropland and Land-Clearing Emission Factors From Firex-AQ

The Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign is a NOAA/NASA interagency intensive study of North American fires that took place from July to September 2019. Agricultural fires were sampled on 7 flights from August 21st to September 3rd, 2019. We present emission factors for gas-phase and aerosol-phase species for the different fuel types identified during the campaign. We discuss the dependence of these emission factors on both fuel type and burning characteristics such as modified combustion efficiency (MCE). We analyze 73 fires encompassing four different agricultural fuels (corn, rice, soybean, wheat) and four different types of land-clearing fuels (grass, slash, pile, shrub). Approximately half of all sampled fires were burning corn agricultural residue. We report emission factors for 118 VOCs, where two thirds of emissions are made up of species with lifetimes against oxidation by OH of less than 12 hours (near-field impacts) and the remainder have longer-lifetimes (far-field impacts). We also include an additional 9 aerosol species, 12 halogenated species, 5 sulfur-containing species, and 22 nitrogen-containing species, including NH3 and NOx. There is a statistically significant difference in MCE between agricultural and land-clearing fires that accounts for some of the differences in emission factors across these fuels. VOCs generally have a strong negative correlation with MCE but with different slopes across fuel types. There is a significant positive relationship between MCE and three gas-phase (NO, NO2, SO2) and two aerosol-phase (pCl, pNH4) species. Many emission factors show additional dependence factors beyond MCE that could be related to fuel composition, fire temperature, soil moisture, or other possible differences in burning conditions. Therefore, important differences in emission factors may result when averaging together different types of agricultural and land-clearing fuels in compilations for use in modeling efforts.

biomass burning↗

Application of OMI, SCIAMACHY and GOME-2 Satellite SO2 Retrievals for Detection of Large Emission Sources

Retrievals of sulfur dioxide (SO2) from space-based spectrometers are in a relatively early stage of development. Factors such as interference between ozone and SO2 in the retrieval algorithms often lead to errors in the retrieved values. Measurements from the Ozone Monitoring Instrument (OMI), Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY), and Global Ozone Monitoring Experiment-2 (GOME-2) satellite sensors, averaged over a period of several years, were used to identify locations with elevated SO2 values and estimate their emission levels. About 30 such locations, detectable by all three sensors and linked to volcanic and anthropogenic sources, were found after applying low and high spatial frequency filtration designed to reduce noise and bias and to enhance weak signals to SO2 data from each instrument. Quantitatively, the mean amount of SO2 in the vicinity of the sources, estimated from the three instruments, is in general agreement. However, its better spatial resolution makes it possible for OMI to detect smaller sources and with additional detail as compared to the other two instruments. Over some regions of China, SCIAMACHY and GOME-2 data show mean SO2 values that are almost 1.5 times higher than those from OMI, but the suggested spatial filtration technique largely reconciles these differences.

SO2 retrievals↗