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NASA NTRS2021

Measuring Atmospheric CO2 Enhancements from the 2017 British Columbia 1 Wildfires Using a Lidar

During the summer 2017 ASCENDS/ABoVE airborne science campaign, the NASA Goddard CO2 Sounder lidar overflew smoke plumes from wildfires in the British Columbia, Canada. In the flight path over Vancouver Island on 8 August 2017, the column XCO2 retrievals from the lidar measurements at flight altitudes around 9 km showed an average enhancement of 4 ppm from the wildfires. A comparison of these enhancements with those from the Goddard Global Chemistry Transport model suggested that the modeled CO2 emissions from wildfires were underestimated by more than a factor of 2. A spiral-down validation performed at Moses Lake airport, Washington showed a bias of 0.1 ppm relative to in situ measurements and a standard deviation of 1 ppm in lidar XCO2 retrievals. The results show that future airborne campaigns and spaceborne missions with this type of lidar can improve estimates of CO2 emissions from wildfires and estimates of carbon fluxes globally.

Jianping Mao↗
NASA NTRS1997

Energy, volatile production, and climatic effects of the Chicxulub Cretaceous/Tertiary impact

A comprehensive analysis of volatiles in the Chicxulub impact strongly supports the hypothesis that impact-generated sulfate aerosols caused over a decade of global cooling, acid rain, and disruption of ocean circulation, which contributed to the mass extinction at the Cretaceous/Tertiary (K/T) boundary. The crater size, meteoritic content of the K/T boundary clay, and impact models indicate that the Chicxulub crater was formed by a short period comet or an asteroid impact that released 0.7-3.4 x 10(31) ergs of energy. Impact models and experiments combined with estimates of volatiles in the projectile and target rocks predict that over 200 gigatons (Gt) each of SO2 and water vapor, and over 500 Gt of CO2, were globally distributed in the stratosphere by the impact. Additional volatiles may have been produced on a global or regional scale that formed sulfate aerosols rapidly in cooler parts of the vapor plume, causing an early, intense pulse of sulfuric acid rain. Estimates of the conversion rate of stratospheric SO2 and water vapor to sulfate aerosol, based on volcanic production of sulfate aerosols, coupled with calculations of diffusion, coagulation, and sedimentation, demonstrate that the 200 Gt stratospheric SO2 and water vapor reservoir would produce sulfate aerosols for 12 years. These sulfate aerosols caused a second pulse of acid rain that was global. Radiative transfer modeling of the aerosol clouds demonstrates (1) that if the initial rapid pulse of sulfate aerosols was global, photosynthesis may have been shut down for 6 months and (2) that for the second prolonged aerosol cloud, solar transmission dropped 80% by the end of first year and remained 50% below normal for 9 years. As a result, global average surface temperatures probably dropped between 5 degrees and 31 degrees K, suggesting that global near-freezing conditions may have been reached. Impact-generated CO2 caused less than 1 degree K greenhouse warming and therefore was insignificant compare to the sulfate cooling. The magnitude of sulfate cooling depends largely upon the rate of ocean mixing as surface waters cool, sink, and are replaced by upwelling of deep ocean water. This upwelling apparently drastically altered ocean stratification and circulation, which may explain the global collapse of the delta 13C gradient between surface and deep ocean waters at the K/T boundary.

NASA Center JPL↗
NASA NTRS1995

In situ observations in aircraft exhaust plumes in the lower stratosphere at midlatitudes

Instrumentation on the NASA ER-2 high-altitude aircraft has been used to observe engine exhaust from the same aircraft while operating in the lower stratosphere. Encounters with the exhaust plume occurred approximately 10 min after emission with spatial scales near 2 km and durations of up to 10 s. Measurements include total reactive nitrogen, NO(y), the component species NO and NO2, CO2, H2O, CO, N2O, condensation nuclei, and meteorological parameters. The integrated amounts of CO2 and H2O during the encounters are consistent with the stoichiometry of fuel combustion (1:1 molar). Emission indices (EI) for NO(x) (= NO + NO2), CO, and N2O are calculated using simultaneous measurements of CO2. EI values for NO(x) near 4 g/(kg fuel) are in good agreement with values scaled from limited ground-based tests of the ER-2 engine. Non-NO(x) species comprise less than about 20% of emitted reactive nitrogen, consistent with model evaluations. In addition to demonstrating the feasibility of aircraft plume detection, these results increase confidence in the projection of emissions from current and proposed supersonic aircraft fleets and hence in the assessment of potential long-term changes in the atmosphere.

Fahey, D. W.↗
NASA NTRSDate not supplied

Enabling more routine monitoring of volcanic CO2 degassing from space

“Volcanic aerosol impacts on satellite trace gas retrievals: enabling volcanic emission plume composition measurements to track evolving sub-surface magmatic conditions” ROSES 2019 IDS (Interdisciplinary Science), 2020-2023 (S. Broccardo, PI) Main hypothesis: Space-based observations of the CO2, SO2, and H2O emissions of passively degassing volcanoes, and the derived mass fluxes and their ratios, can be used to constrain a physical model of the pre-eruptive conditions of magmatic reservoirs and thereby improve our understanding of sub-surface processes.

Enabling↗
NASA NTRSDate not supplied

PyroCbs from Australia Fires and its Impact Using Satellite Observations from CrIS and TROPOMI and Reanalysis Data

Pyrocumulonimbus (pyroCb) clouds are thunder clouds created by intense heat from the Earth’s surface. They are formed similarly to cumulonimbus clouds, but the intense heat that results in the vigorous updraft comes from fire, either large wildfires or volcanic eruptions. Australia’s unprecedented fire disasters at the end of 2019 to early 2020 emitted huge amounts of carbon monoxide (CO) and fire aerosol particles to the atmosphere, particularly during the pyroCb outbreak that occurred in southeast Australia between 29 December 2019 and 4 January 2020. It was estimated that at least 18 pyroCbs were generated during this episode, and some of them injected ice, smoke, and biomass burning gases above the local tropopause. An unprecedented abundance of H2O and CO in the stratosphere, and the displacement of background ozone (O3) and N2O from rapid ascent of air from the troposphere and lower stratosphere were found from satellite observations. Some other studies also found that the fire emissions and their long-range transport resulted in stratospheric aerosol, temperature, and O3 anomalies after the 2020 Australian bushfires and altered the Antarctic ozone and vortex, posing great impact to local air quality and climate change. Further study on the atmospheric thermodynamic status of atmosphere associated with these pyroCbs, and the change of the cloud properties and trace gases during this unprecedented Australia fires will be made using a new single Field of View (SFOV) Sounder Atmospheric Products (SiFSAP). SiFSAP was developed by NASA using the Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) onboard SNPP and JPSS-1, and will soon be available to the public at NASA DAAC. Since this product has a spatial resolution of 15 km at nadir, which is better than most global weather and climate models and other current operational sounding products, a process-oriented analysis of the dynamic transport of CO and fire plumes during this unprecedented fire disasters will be made in this study. Based on a Principal Component Radiative Transfer Model (PCRTM) and an optimized estimation retrieval algorithm, a simultaneously retrieval is made using the whole spectral information measured by CrIS, and the derived SiFSAP include temperature, water vapor, trace gases (such as O3, CO2, CO, CH4 and N2O), cloud properties and surface properties. Use of ATMS together with CrIS allows SiFSAP to get accurate retrieval products under thick pyroCb conditions, and an algorithm to detect pyroCb based on the hyperspectral infrared sounder spectrum from CrIS will be developed and verified. In addition to SiFSAP sounding products, other products like CO, O3, NO2 from TROPOMI, O3 from OMPS will be used for retrospective analysis. The wind fields from the NASA’s Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) and ERA5 will be used to characterize the transport, and the SiFSAP temperature and water vapor profiles within and around pyroCbs will be compared with MERRA-2 and ERA5 products.

Xiaozhen (Shawn) Xiong↗
NASA NTRS2004

Spatial Distributions of Metal Atoms During Carbon SWNTs Formation: Measurements and Modelling

Experiments and modelling have been undertaken to clarify the role of metal catalysts during single-wall carbon nanotube formation. For instance, we wonder whether the metal catalyst is active as an atom, a cluster, a liquid or solid nanoparticle [1]. A reactor has been developed for synthesis by continuous CO2-laser vaporisation of a carbon-nickel-cobalt target in laminar helium flow. The laser induced fluorescence technique [2] is applied for local probing of gaseous Ni, Co and CZ species throughout the hot carbon flow of the target heated up to 3500 K. A rapid depletion of C2 in contrast to the spatial extent of metal atoms is observed in the plume (Fig. 1). This asserts that C2 condenses earlier than Ni and Co atoms.[3, 4]. The depletion is even faster when catalysts are present. It may indicate that an interaction between metal atoms and carbon dimers takes place in the gas as soon as they are expelled from the target surface. Two methods of modelling are used: a spatially I-D calculation developed originally for the arc process [5], and a zero-D time dependent calculation, solving the chemical kinetics along the streamlines [6]. The latter includes Ni cluster formation. The peak of C2 density is calculated close to the target surface where the temperature is the highest. In the hot region, C; is dominant. As the carbon products move away from the target and mix with the ambient helium, they recombine into larger clusters, as demonstrated by the peak of C5 density around 1 mm. The profile of Ni-atom density compares fairly well with the measured one (Fig. 2). The early increase is due to the drop of temperature, and the final decrease beyond 6 mm results from Ni cluster formation at the eutectic temperature (approx.1600 K).

Cau, M.↗
NASA NTRS1982

The satellite power system - Assessment of the environmental impact on middle atmosphere composition and on climate

Numerical models were developed to calculate the total deposition of watervapor, hydrogen, CO2, CO, SO2, and NO in the middle atmosphere from operation of heavy lift launch vehicles (HLLV) used to build a satellite solar power system (SPS). The effects of the contaminants were examined for their effects on the upper atmosphere. One- and two-dimensional models were formulated for the photochemistry of the upper atmosphere and for rocket plumes and reentry. An SPS scenario of 400 launches per year for 10 yr was considered. The build-up of the contaminants in the atmosphere was projected to have no significant effects, even at the launch latitude. Neither would there by any dangerous ozone depletion. It was found that H, OH, and HO2 species would double in the thermosphere. No measurable changes in climate were foreseen.

Whitten, R. C.↗
NASA NTRS1975

Parametric studies with an atmospheric diffusion model that assesses toxic fuel hazards due to the ground clouds generated by rocket launches

Parametric studies were made with a multilayer atmospheric diffusion model to place quantitative limits on the uncertainty of predicting ground-level toxic rocket-fuel concentrations. Exhaust distributions in the ground cloud, cloud stabilized geometry, atmospheric coefficients, the effects of exhaust plume afterburning of carbon monoxide CO, assumed surface mixing-layer division in the model, and model sensitivity to different meteorological regimes were studied. Large-scale differences in ground-level predictions are quantitatively described. Cloud alongwind growth for several meteorological conditions is shown to be in error because of incorrect application of previous diffusion theory. In addition, rocket-plume calculations indicate that almost all of the rocket-motor carbon monoxide is afterburned to carbon dioxide CO2, thus reducing toxic hazards due to CO. The afterburning is also shown to have a significant effect on cloud stabilization height and on ground-level concentrations of exhaust products.

Stewart, R. B.↗
NASA NTRS2020

Constraining Fossil Fuel CO2 Emissions from Urban Area Using OCO-2 Observations of Total Column CO2

Satellite observations of the total column dry-air CO2(XCO2) are expected to support the quantification and monitoring of fossil fuel CO2 (ffCO2) emissions from urban areas. We evaluate the utility of the Orbiting Carbon Observatory 2 (OCO-2) XCO2 retrievals to optimize whole-city emissions, using a Bayesian inversion system and high-resolution transport modeling. The uncertainties of constrained emissions related to transport model, satellite measurements, and local biospheric fluxes are quantified. For the first two uncertainty sources, we examine cities of different landscapes: “plume city” located in relatively flat terrain, represented by Riyadh and Cairo; “basin city” located in basin terrain, represented by Los Angeles (LA). The retrieved scaling factors of emissions and their uncertainties show prominent variabilities from track to track, due to the varying meteorological conditions and relative locations of the tracks transecting plumes. To explore the performance of multiple tracks in retrieving emissions, pseudo data experiments are carried out. The estimated least number of tracks required to constrain the total emissions for Riyadh (<10% uncertainty), Cairo (<10%), and LA (<5%) are 5, 8, and 7, respectively. Additionally, to evaluate the impact of biospheric fluxes on derivation of the ffXCO2 enhancements, we conduct simulations for Pearl River Delta metropolitan area. Significant fractions of local XCO2 enhancements associated with local biospheric XCO2 variations are shown, which potentially lead to biased estimates of ffCO2 emissions. We demonstrate that satellite measurements can be used to improve urban ffCO2 emissions with a sufficient amount of measurements and appropriate representations of the uncertainty components.

Xinxin Ye↗
NASA NTRS1997

Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific

During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.

Srivastava, Vandana↗
NASA NTRS1986

Development of a global model for atmospheric backscatter at CO2 wavelengths

The variation of the aerosol backscattering at 10.6 micrometers within the free troposphere was investigated and a model to describe this variation was developed. The analysis combines theoretical modeling with the results contained within three independent data sets. The data sets used were obtained by the SAGE I/SAM II satellite experiments, the GAMETAG flight series, and by direct backscatter measurements. The theoretical work includes use of a bimodal, two component aerosol model, and the study of the microphysical and associated optical changes occurring within an aerosol plume. A consistent picture is obtained that describes the variation of the aerosol backscattering function in the free troposphere with altitude, latitude, and season.

Kent, G. S.↗
NASA NTRS1985

Development of global model for atmospheric backscatter at CO2 wavelengths

The improvement of an understanding of the variation of the aerosol backscattering at 10.6 micron within the free troposphere and the development model to describe this was undertaken. The analysis combines theoretical modeling with the results contained within three independent data sets. The data sets are obtained by the SAGE I/SAM II satellite experiments, the GAMETAG flight series and by direct backscatter measurements. The theoretical work includes use of a bimodal, two component aerosol model, and the study of the microphysical and associated optical changes occurring within an aerosol plume. A consistent picture is obtained, which describes the variation of the aerosol backscattering function in the free troposphere with altitude, latitude, and season. Most data are available and greatest consistency is found inside the Northern Hemisphere.

Kent, G. S.↗
NASA NTRSDate not supplied

UAS Payload Design for In-Situ Smoke Plume Sensing

To aid in the detection of harmful aerosols and trace gases emitted in wildfires and prescribed burns, we are designing a smoke-specific payload which can be flown on the Black Swift S2™ Uncrewed Aerial System (UAS) platform. The payload will be custom and mounted within the nosecone, equipped with a trace gas sensor suite and particle spectrometer for characterization of wildfire and prescribed burn emissions. This data will aid in the improvement of HYSPLIT3 modeling to make more informed decisions regarding prescribed burns, particularly for mountain valleys in the Pacific Northwest. The trace gas suite will be composed of 8 low-cost trace gas sensors (CH4, CO2, CO, HCN, NO2, NO, O3, and Volatile Organic Compounds (VOCs)). Portable Optical Particle Spectrometer (POPS) measures particle size range between 0.14 to 3 µm, which is crucial for assessing public health impact, air quality, and visibility.

Henry Miller↗
NASA NTRS2014

Afterbody Heat Flux Measurements in the NASA Ames HFFAF Ballistic Range

In order to measure afterbody heat fluxes over a model in the ballistic range, the required modifications to a proven technique for measuring forebody heat fluxes are described. This involves the use of an extended helium gas plume to remove the glowing wake and the use of special high conductivity, high temperature capable graphite-filled plastic for the afterbody. The models and test conditions are described. Data in the form of plots of the surface temperature of the models are presented. Finally, experimental and computational fluid dynamic (CFD) heat flux data for forebody and afterbody heat fluxes are presented and compared. Data are presented for a 45 degree sphere-cone (with a projecting rear stud) at 2.70 km/s and for a sphere at 4.76 km/s. Both models were launched into 76 Torr of CO2 gas. The experimental forebody heat fluxes were within 1.5% of the CFD values. The experimental afterbody heat fluxes were within 1% of the CFD values for the sphere, but only 51% of the CFD values for the sphere-cone.

Bogdanoff, David W.↗
NASA NTRS2011

Primordial Synthesis of Amines and Amino Acids in a 1958 Miller H2S-Rich Spark Discharge Experiment

Archived samples from a previously unreported 1958 Stanley Miller electric discharge experiment containing hydrogen sulfide (H2S) were recently discovered and analyzed using high-performance liquid chromatography and time-of-flight mass spectrometry. We report here the detection and quantification of primary amine-containing compounds in the original sample residues, which were produced via spark discharge using a gaseous mixture of H2S, CH4, NH3, and CO2. A total of 23 amino acids and 4 amines, including 7 organosulfur compounds, were detected in these samples. The major amino acids with chiral centers are racemic within the accuracy of the measurements, indicating that they are not contaminants introduced during sample storage. This experiment marks the first synthesis of sulfur amino acids from spark discharge experiments designed to imitate primordia! environments. The relative yield of some amino acids, in particular the isomers of aminobutyric acid, are the highest ever found in a spark discharge experiment. The simulated primordial conditions used by Miller may serve as a model for early volcanic plume chemistry and provide insight to the possible roles such plumes may have played in abiotic organic synthesis. Additionally, the overall abundances of the synthesized amino acids in the presence of H2S are very similar to the abundances found in some carbonaceous meteorites, suggesting that H2S may have played an important role in prebiotic reactions in early solar system environments.

Parker, Eric T.↗
NASA NTRS2016

Emissions Relationships Among Western Forest Fire Plumes: II. Plume Typing for Sources of Ozone and Aerosol Absorption

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAs SEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing Cburn Ctot added to the fire plume, where Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individualspecies i, xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

ozone↗
NASA NTRS2020

The Effect of Europa and Enceladus Analog Seawater Composition on Isotopic Measurements of Volatile CO2

Science goals for icy ocean worlds missions include characterizing the chemical compositionof the surface and interior using remote sensing and in situ techniques. The next class of flightmass spectrometers for these missions will obtain compositional identifications and isotope ratiomeasurements of volatiles evolved from the ice surface (exosphere) and plumes. These massspectra will be combined with data from other flight instruments to infer the composition of theinterior from volatiles. To ensure accurate interpretation of these measurements, it is critical toverify whether the fundamental assumption that volatiles observed in icy ocean world exospheresor plumes will be a direct reflection of the sub-ice ocean. The present study evaluates whether isotopologues from an initial CO2 gas fractionate by interacting with seawater (brine) of varyingsalt composition and concentration. δ13CCO2 are affected by the pH of the brine and subsequentspeciation of {CO2}, where {CO2} represents the combination of CO2, H2CO3, HCO3-, and CO32-.{CO2} for low pH brines hypothesized for Europa will preferentially speciate as CO2. Analyzedδ13CCO2 for low pH brines are within error of the original δ13CCO2, demonstrating that volatile CO2in a low pH system will be a direct reflection of the original CO2. However, Europa’s radiativeenvironment and rapid depressurization due to plume ejection may impose fractionation effects.In contrast, high pH systems relevant to Enceladus or a more alkaline Europa are expected toform all carbonate species, while favoring speciation as HCO3-. High pH brines in theseexperiments include both an original CO2 gas and an isotopically distinct HCO3- (from NaHCO3salt). These alkaline experiments demonstrate that δ13CCO2 values are highly variable, and dependon the concentration of the dominant carbonate species, (Na)HCO3-. Mass balance estimatesindicate that measured δ13CCO2 is a thermodynamically predictable mixture of both carbonsources, suggesting that measurements of δ13C at Enceladus would directly reflect of the sourcesof CO2 and carbonate buffering in the ocean. δ18O measurements for CO2 interacting with KCland MgCl2 follow established models for δ18O-ionic strength. CO2 interacting with MgSO4,Na2SO4, and NaCl demonstrate an offset from established δ18O-ionic strength models dependingon the concentration of initial CO2. These results suggest that current predictive models for δ18Oin brines need to be resolved for changing concentrations of CO2

Ocean Worlds↗
NASA NTRSDate not supplied

Interpretable Machine Learning Models for Autonomous Characterization of Analogue Ocean World Seawater Chemistry and Biosignature Potential Using Isotope Ratio Data

Background: Future missions to ocean worlds, such as Enceladus and Europa, will attempt to characterize the subsurface seawater chemistry and assess the potential for life. Such missions will be equipped with capabilities to precisely measure volatile isotopes in plumes, atmospheres, and exospheres. Motivation: While large isotopic fractionations can indicate a biological source, there are signatures resulting from abiotic geochemical processes that mimic isotopic biosignatures. While machine learning (ML) has the potential to disentangle competing effects and biotic mimicry, high-dimensional isotope ratio mass spectrometry (IRMS) data is likely to contain noise/irrelevant features and involve complex statistical interactions that make human inference and interpretation difficult. Further, ML predictions with as far-reaching implications as an extraterrestrial biosignature on an ocean world requires the use of interpretable models (i.e., not “black box” models) with physically and mathematically meaningful feature spaces along with false positive diagnostics. Methods: We use volatile CO2 IRMS data of analogue ocean world seawaters to validate an ML approach to provide biogeochemical context for biosignature detection. We employ a feature selection method called nearest-neighbor projected distance regression (NPDR) that detects statistical interactions and helps elucidate the mechanisms of the Random Forest classification models. Results: We train and validate predictive ML models on volatile CO2 IRMS data of analogue ocean world seawaters to predict major salt components (e.g., MgSO4, NaHCO3), pH, ionic strength, and the presence of biosignatures. Features derived from IRMS measurements are augmented with extracted time-series features. Our results show high test accuracy and interpretability, which is increased by interaction network visualization, sample-wise variable importance scores, and single-sample class probability estimates. We demonstrate an ML mission software solution that triggers autonomous data transmission and biogeochemical sample prediction.

geochemistry↗