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DOE OSTI2021

Demonstration of neutron radiation-induced nucleation of supercooled water

In this study, we present direct evidence for neutrons causing nucleation of supercooled water. Highly purified water (20 nm filtration) is cooled to well below freezing (as low as −20 °C) with a radioactive calibration source of neutrons/gamma-rays either present or removed during each of many control cooling runs for the same volume of water. When it is primarily neutrons irradiating the sample bulk, the non-equilibrium freezing point (also known as the “supercooling point”) is, on average, +0.7 °C warmer than the control equivalent, with a statistical significance of greater than 5 Sigma, with systematic uncertainty included. This effect is not observed with water in the presence of gamma-rays instead of neutrons. While these neutrons should have theoretically had sufficient energy to mount the energy barrier, corroborating our results, their raising of supercooling temperature has never been reported experimentally to the best of our knowledge. The potential to use deeply supercooled solutions, not only water, as metastable detectors for radiation and perhaps dark matter or neutrino physics presents now a new avenue for exploration.

Szydagis, Matthew↗

NASA NTRS1997

Large-Scale Impact Cratering and Early Earth Evolution

The surface of the Moon attests to the importance of large-scale impact in its early crustal evolution. Previous models of the effects of a massive bombardment on terrestrial crustal evolution have relied on analogies with the Moon, with allowances for the presence of water and a thinner lithosphere. It is now apparent that strict lunar-terrestrial analogies are incorrect because of the "differential scaling" of crater dimensions and melt volumes with event size and planetary gravity. Impact melt volumes and "ancient cavity dimensions for specific impacts were modeled according to previous procedures. In the terrestrial case, the melt volume (V(sub m)) exceeds that of the transient cavity (V(sub tc)) at diameters > or = 400 km. This condition is reached on the Moon only with transient cavity diameters > or = 3000 km, equivalent to whole Moon melting. The melt volumes in these large impact events are minimum estimates, since, at these sizes, the higher temperature of the target rocks at depth will increase melt production. Using the modification-scaling relation of Croft, a transient cavity diameter of about 400 km in the terrestrial environment corresponds to an expected final impact "basin" diameter of about 900 km. Such a "basin" would be comparable in dimensions to the lunar basin Orientale. This 900-km "basin" on the early Earth, however, would not have had the appearance of Orientale. It would have been essentially a melt pool, and, morphologically, would have had more in common with the palimpsests structures on Callisto and Ganymede. With the terrestrial equivalents to the large multiring basins of the Moon being manifested as muted palimpsest-like structures filled with impact melt, it is unlikely they played a role in establishing the freeboard on the early Earth. The composition of the massive impact melt sheets (> 10 (exp 7) cu km) produced in "basin-forming" events on the early Earth would have most likely ranged from basaltic to more mafic for the largest impacts, where the melt volume would have reached well into the mantle. Any contribution from adiabatic melting or shock heating of the asthenosphere would have had similar mafic compositions. The depth of the melt sheets is unknown but would have been in the multilkilometer range. Bodies of basaltic melt > or = 300 m thick differentiate in the terrestrial environment, with the degree of differentiation being a function of the thickness of the body. We therefore expect that these thick, closed-system melt pools would have differentiated into an ultramafic-mafic base and felsic top. If only 10% of the impact melt produced in a single event creating a 400-km diameter transient cavity evolved into felsic differentiates, they would be comparable in volume to the Columbia River basalts. It has been estimated that at least 200 impact events of this size or larger occurred on the early Earth during a period of heavy bombardment. We speculate that these massive differentiated melt sheets may have had a role in the formation of the initial felsic component of the Earth's crust. Additional information is contained in the original.

Grieve, R. A. F.↗

NASA NTRS2024

Dust Tolerance Characterization of Lunar Docking and Hatch Seals

Low-leakage seals are an enabling technology for future lunar surface systems, and they must be kept clean to ensure that crews have sufficient breathable air for extended lunar surface missions. Previous testing has shown that contamination and debris on seals can cause them to exhibit higher leak rates. However, seal performance in the presence of lunar dust has not been thoroughly characterized, and the size and concentration of dust particles that cause seal leak rates to become unacceptable have not been defined or well understood. To address this knowledge gap, researchers at the NASA Glenn Research Center have been executing a multiphase study to better understand and mitigate seal dust-exposure risks. The focus of this paper is on the first phase of that study, in which tests were conducted to develop a performance database for two representative state-of-the-art seal designs. Leak rates are presented for seals with varying levels of dust contamination, and breakthrough points are identified at which seal leak rates exceeded equivalent leak rate requirements. This phase of the study also investigated the effects of temperature on the seals’ ability to hold pressure when contaminated with dust.

Dust Mitigation↗

NASA NTRS2011

Substituted Quaternary Ammonium Salts Improve Low-Temperature Performance of Double-Layer Capacitors

Double-layer capacitors are unique energy storage devices, capable of supporting large current pulses as well as a very high number of charging and discharging cycles. The performance of doublelayer capacitors is highly dependent on the nature of the electrolyte system used. Many applications, including for electric and fuel cell vehicles, back-up diesel generators, wind generator pitch control back-up power systems, environmental and structural distributed sensors, and spacecraft avionics, can potentially benefit from the use of double-layer capacitors with lower equivalent series resistances (ESRs) over wider temperature limits. Higher ESRs result in decreased power output, which is a particular problem at lower temperatures. Commercially available cells are typically rated for operation down to only 40 C. Previous briefs [for example, Low Temperature Supercapacitors (NPO-44386), NASA Tech Briefs, Vol. 32, No. 7 (July 2008), p. 32, and Supercapacitor Electrolyte Solvents With Liquid Range Below 80 C (NPO-44855), NASA Tech Briefs, Vol. 34, No. 1 (January 2010), p. 44] discussed the use of electrolytes that employed low-melting-point co-solvents to depress the freezing point of traditional acetonitrile-based electrolytes. Using these modified electrolyte formulations can extend the low-temperature operational limit of double-layer capacitors beyond that of commercially available cells. This previous work has shown that although the measured capacitance is relatively insensitive to temperature, the ESR can rise rapidly at low temperatures, due to decreased electrolyte conductance within the pores of the high surface- area carbon electrodes. Most of these advanced electrolyte systems featured tetraethylammonium tetrafluoroborate (TEATFB) as the salt. More recent work at JPL indicates the use of the asymmetric quaternary ammonium salt triethylmethylammonium tetrafluoroborate (TEMATFB) or spiro-(l,l')-bipyrrolidium tetrafluoroborate (SBPBF4) in a 1:1 by volume solvent mixture of acetonitrile (AN) and methyl formate (MF) enables double-layer capacitor cells to operate well below -40 C with a relatively low ESR. Typically, a less than twofold increase in ESR is observed at -65 C relative to room-temperature values, when these modified electrolyte blends are used in prototype cells. Double-layer capacitor coin cells filled with these electrolytes have displayed the lowest measured ESR for an organic electrolyte to date at low temperature (based on a wide range of electrolyte screening studies at JPL). The cells featured high-surface-area (approximately equal to 2,500 m/g) carbon electrodes that were 0.50 mm thick and 1.6 cm in diameter, and coated with a thin layer of platinum to reduce cell resistance. A polyethylene separator was used to electrically isolate the electrodes.

Brandon, Erik J.↗

NASA NTRS2012

Satellite Remote Sensing of Snow/Ice Albedo over the Himalayas

The Himalayan glaciers and snowpacks play an important role in the hydrological cycle over Asia. The seasonal snow melt from the Himalayan glaciers and snowpacks is one of the key elements to the livelihood of the downstream densely populated regions of South Asia. During the pre-monsoon season (April-May-June), South Asia not only experiences the reversal of the regional meridional tropospheric temperature gradient (i.e., the onset of the summer monsoon), but also is being bombarded by dry westerly airmass that transports mineral dust from various Southwest Asian desert and arid regions into the Indo-Gangetic Plains in northern India. Mixed with heavy anthropogenic pollution, mineral dust constitutes the bulk of regional aerosol loading and forms an extensive and vertically extended brown haze lapping against the southern slopes of the Himalayas. Episodic dust plumes are advected over the Himalayas, and are discernible in satellite imagery, resulting in dust-capped snow surface. Motivated by the potential implications of accelerated snowmelt, we examine the changes in radiative energetics induced by aerosol transport over the Himalayan snow cover by utilizing space borne observations. Our objective lies in the investigation of potential impacts of aerosol solar absorption on the Top-of-Atmosphere (TOA) spectral reflectivity and the broadband albedo, and hence the accelerated snowmelt, particularly in the western Himalayas. Lambertian Equivalent Reflectivity (LER) in the visible and near-infrared wavelengths, derived from Moderate Resolution Imaging Spectroradiometer radiances, is used to generate statistics for determining perturbation caused due to dust layer over snow surface in over ten years of continuous observations. Case studies indicate significant reduction of LER ranging from 5 to 8% in the 412-860nm spectra. Broadband flux observations, from the Clouds and the Earth's Radiant Energy System, are also used to investigate changes in shortwave TOA flux over dust-laden and dust-free snow covered regions. Additionally, spatio-temporal and intra-seasonal variations of LER, along with snow cover information, are used to characterize the seasonal melt pattern and thus to distinguish the outstanding aerosol-induced snowmelt signal. Results from this observational work are expected to provide better understanding of the radiative impact of aerosols over snow surface, especially its role in the Himalayan hydro-glacialogical variability.

Hsu, N. Christina↗

DOE OSTI2022

A Meteorology and Snow Data Set From Adjacent Forested and Meadow Sites at Crested Butte, CO, USA

We present meteorology and snow observation data collected at sites in the southwestern Colorado Rocky Mountains (USA) over three consecutive water years with different amounts of snow water equivalent (SWE) accumulation: A year with above average SWE (2019), a year with average SWE (2020), and a year with below average SWE (2021). This data set is distinguished by its emphasis on paired open-forest sites in a continental snow climate. Approximately once a month during February–May, we collected data from 15 to 20 snow pits and took 8 to 19 snow depth transects. Our sampling sites were in open and adjacent forested areas at 3,100 m and in a lower elevation aspen (3,035 m) and higher elevation conifer stand (3,395 m). In total, we recorded 270 individual snow pit density and temperature profiles and over 4,000 snow depth measurements. These data are complimented by continuous meteorological measurements from two weather stations: One in the open and one in the adjacent forest. Meteorology data—including incoming shortwave and longwave radiation, outgoing shortwave radiation, relative humidity, wind speed, snow depth, and air and infrared surface temperature—were quality controlled and the forcing data were gap-filled. These data are available to download from Bonner, Smyth, et al. at three levels of processing, including a level with downscaled, adjusted precipitation based on data assimilation using observed snow depth and a process-based snow model. We demonstrate the utility of these data with a modeling experiment that explores open-forest differences and identifies opportunities for improvements in model representation.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1998

The Atmospheric Structure of Triton and Pluto

The goal of this research was to better determine the atmospheric structures of Triton and Pluto through further analysis of three occultation data sets obtained with the Kuiper Airborne Observatory (KAO.) As the research progressed, we concentrated our efforts on the Triton data, as this appeared to be the most fruitful. Three papers have been prepared as a result of this research. The first paper presents new results about Triton's atmospheric structure from the analysis of all ground-based stellar occultation data recorded to date, including one single-chord occultation recorded on 1993 July 10 and nine occultation lightcurves from the double-star event on 1995 August 14. These stellar occultation observations made both in the visible and in the infrared have good spatial coverage of Triton, including the first Triton central-flash observations, and are the first data to probe the altitude level 20-100 km on Triton. The small-planet lightcurve model of J. L. Elliot and L. A. Young was generalized to include stellar flux refracted by the far limb, and then fitted to the data. Values of the pressure, derived from separate immersion and emersion chords, show no significant trends with latitude, indicating that Triton's atmosphere is spherically symmetric at approximately 50 km altitude to within the error of the measurements; however, asymmetry observed in the central flash indicates the atmosphere is not homogenous at the lowest levels probed (approximately 20 km altitude). From the average of the 1995 occultation data, the equivalent isothermal temperature of the atmosphere is 47 plus or minus 1 K and the atmospheric pressure at 1400 km radius (approximately 50 km altitude) is 1.4 plus or minus 0.1 microbar. Both of these are not consistent with a model based on Voyager UVS and RSS observations in 1989. The atmospheric temperature from the occultation is 5 K colder than that predicted by the model and the observed pressure is a factor of 1.8 greater than the model. In our opinion, the disagreement in temperature and pressure is probably due to modeling problems at the microbar level, since measurements at this level have not previously been made. Alternatively, the difference could be due to seasonal change in Triton's atmospheric structure. The second paper reports observations of a recent stellar occultation by Triton which, when combined with earlier results, show that Triton has undergone a period of global warming since 1989. The most conservative estimates of the rate of temperature and surface-pressure increase during this period imply that the atmosphere is doubling in bulk every 10 years -- significantly faster than predicted by published frost model for Triton. Our results suggests that permanent polar caps on Triton play a dominant role in regulating seasonal atmospheric changes. Similar processes should also be active on Pluto. A third paper 'Global Warming on Triton' will appear in a the January 1999 issue of Sky and Telescope.

Elliot, James L.↗

DOE OSTI2022

Boron Nitride Solid-State Neutron Detectors

The goal of this project is to build upon the work performed under the Texas Tech IDEAS project (DE-AR0000964 monitored by Dr. Isik Kizilyalli) to bring the developed B-10 enriched hexagonal boron nitride (h- 10 BN or 10 BN or BN) semiconductor neutron detector technology to the next level of maturity. In comparison to He-3 ( 3 He) gas detectors, BN neutron detectors possess all the intrinsic advantages of semiconductor devices: light weight, compact size, fast response speed, high spatial resolution, high temperature and low voltage operation capability, ease of mass production via existing semiconductor infrastructures, low cost of operation and maintenance, flexible form factors, and durability. The project will develop a prototype h- 10 BN neutron detector as a potential replacement for the 3 He gas neutron detectors (LND 25185 or equivalent) used in various neutron survey meters currently produced and commercialized by Ludlum Measurements, Inc. (LMI). To increase the overall detection efficiency, it is essential to maximize the collection efficiency of charge carriers (electrons and holes) generated by the nuclear reaction, which demands a further push to achieve 10 BN epilayers with improved material quality. The material growth processes will be guided by characterization of structural, optical, and electrical properties of h-BN. Selective devices will be calibrated at LMI. During ARPA-E supporting period, the key material parameters of h-BN produced by metal organic chemical vapor deposition (MOCVD), including the layer thickness, mobility-lifetime product, surface recombination field and detector size for maintaining a high charge collection efficiency all have been improved by several orders of magnitude. These improvements have enabled the realization of high-performance h 10BN semiconductor thermal neutron detectors. Presently, h- 10 BN thermal neutron detectors developed under ARPA-E’s support hold the record high detection efficiency among all solid-state detectors at 59%. With further development in manufacturing, there is no question that h-BN detectors will replace the traditional He-3 gas detectors in certain application areas by offering obvious advantages of semiconductor technologies over gas detectors and opportunities for users to dedicate the scarce and expensive supply of He-3 gas to other application areas where substitutes of He-3 gas are not possible.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Influence of Ink Formulation and Drying Conditions on Ionomer Distribution in High-Performance Roll-to-Roll-Coated Gas-Diffusion Electrodes

To enable mass production of fuel cell membrane electrode assemblies (MEAs) catalyst layers production will require continuous roll-to-roll (R2R) coating processes. Gas diffusion electrodes (GDEs) are advantageous for mass production because the catalyst layer can be directely coated on the microporous layer of the gas diffusion media without the need for a decal-transfer process. It is known that the water-to-alcohol ratio in the catalyst ink influences the interactions of the ionomer with the catalyst leading to different distributions of ionomer in spray-coated catalyst layers. It is also known that during drying of colloidal mixtures, like fuel cell inks, factors such as drying rate, particle size, and agglomeration influence how the materials distribute themselves throughout the thickness of the dired film. Thus far there have only been limited studies to understand how process conditions such as ink formulation and drying temperature influence the distribution of ionomer and catalyst coated using scalable methods. This understanding is especially important for GDEs since it is known that having a sufficient amount of ionomer at the catalyst layer-membrane interface is critical for high performance. In this study we have focused on determining how the ratio of water to 1-propanol in the catalyst ink ink and drying temperature influence the distribution of ionomer throughout the thickness of the catalyst layer. Using a combination of Kelvin probe and x-ray photoelectron spectroscopy we show that an ionomer-rich surface is promoted by a higher drying rate and a water-rich catalyst ink. In contrast, a 1-propanol catalyst ink leads to a lower concentration of ionomer on the top surface. Using x-ray computed tomography, we are able to characterize the ionomer distribution throughout the thickness of the layer. We find that, in addition to promoting an ionomer-rich top surface, water-rich inks lead to a more homogenous distribution of ionomer, whereas a 1-propanol-rich ink leads to a more irregular distribution. It is found that MEA performance is improved by selecting conditions and ink formulations that promote ionomer enrichment at the top surface to facilitate a good interface with the membrane. MEAs prepared with a 75 wt% water catalyst ink with a 0.9 I/C have equivalent performance to spray-coated GDEs. Critically, these R2R-coated GDEs do not need an additional ionomer overlayer like the spray-coated GDEs do, reducing the number of processing steps in a manufacturing setting. This work shows that with the appropriate selection of materials, ink formulation, and processing conditions gas-diffusion electrodes are a viable pathway for fuel cell manufacturing.

ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION↗

DOE OSTI2023

Mastering the synergy between Na 3 V 2 (PO 4 ) 2 F 3 electrode and electrolyte: A must for Na-ion cells

Sodium-ion batteries are emerging as suitable energy storage devices for special applications such as high-power devices with the advantages of being cheaper and more sustainable than the Li-ion equivalents. The sodium ion cells consisting of polyanionic Na 3 V 2 (PO 4 ) 2 F 3 - hard carbon electrodes exhibit high power rate capabilities but limited cycle life, especially at high temperatures. To circumvent this drawback we herein conducted in-depth analyses of the origins of structural degradations occurring in Na 3 V 2 (PO 4 ) 2 F 3 electrodes upon long cycling. Vanadium dissolution with associated parasitic reactions is identified as one of the major reasons for cell failure. Its amount varies depending on the electrolyte, with NaTFSI-based electrolyte showing the least vanadium dissolution as the TFSI - anion decomposes without producing acidic impurities, in contrast to the NaPF 6 -based electrolyte. The dissolved vanadium species undergoes oxidation and reduction processes at the Na 3 V 2 (PO 4 ) 2 F 3 and HC electrodes, respectively, with the electrochemical signature of these processes being used as a fingerprint to identify state of health of the 18650 cells. Here, having found that surface reactivity is the primary cause of vanadium dissolution we provide methods to mitigate it by combining surface coating and optimized electrolyte formulation.

25 ENERGY STORAGE↗

DOE OSTI2021

Groundwater Inflows to the Columbia River Along the Hanford Reach and Associated Nitrate Concentrations

Healthy river ecosystems require the interaction of many physical and biological processes to maintain their status. One physical process supporting biogeochemical cycling is hydrologic exchange (i.e., hydrologic exchange flows, HEFs) between relatively fast-flowing channel waters and slower-flowing surface and subsurface waters (lateral and vertical). Land uses adjacent to rivers have the potential to alter the water quality of off-channel surface and subsurface waters, and HEFs therefore have the potential to deliver solutes associated with river-adjacent land uses to rivers. HEFs can be nonpoint, diffuse sources of pollution, making the ultimate pollution source difficult to identify, especially in large rivers. Here, we seek to identify HEFs in the Columbia River near Richland, WA by looking for anomalies in temperature and electrical conductivity (EC) along the bed of the river in February, June, July, August, and November 2018. These are ultimately the “ends” of HEFs as they are locations of subsurface inflow to the river. We found these anomalies to be a combination of warmer or colder and higher (but not lower) EC than river water. We identified a majority of warm anomalies in February and July 2018, and majority cold anomalies in June, August, and November 2018. High-EC anomalies were found mostly in February, August, and November. Combined, we observe a shift from warm, high EC anomalies dominating in February to equivalent EC, warm anomalies in June, to equivalent EC, cool anomalies dominating July. In August, we also measured dissolved nitrate ($NO^-_3$) in-situ to determine whether anomalies were associated with increased $NO^-_3$ loading to the river, especially along the eastern shoreline, which is dominated by agricultural land use. Inflows along the eastern shoreline have greater concentrations of nitrate than river water (up to 10 mg $N–NO^-_3$/L). This research demonstrates that HEFs are temporally and spatially dynamic transferring heat and solutes to rivers.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1998

Recent Advances in Visualizing 3D Flow with LIC

Line Integral Convolution (LIC), introduced by Cabral and Leedom in 1993, is an elegant and versatile technique for representing directional information via patterns of correlation in a texture. Although most commonly used to depict 2D flow, or flow over a surface in 3D, LIC methods can equivalently be used to portray 3D flow through a volume. However, the popularity of LIC as a device for illustrating 3D flow has historically been limited both by the computational expense of generating and rendering such a 3D texture and by the difficulties inherent in clearly and effectively conveying the directional information embodied in the volumetric output textures that are produced. In an earlier paper, we briefly discussed some of the factors that may underlie the perceptual difficulties that we can encounter with dense 3D displays and outlined several strategies for more effectively visualizing 3D flow with volume LIC. In this article, we review in more detail techniques for selectively emphasizing critical regions of interest in a flow and for facilitating the accurate perception of the 3D depth and orientation of overlapping streamlines, and we demonstrate new methods for efficiently incorporating an indication of orientation into a flow representation and for conveying additional information about related scalar quantities such as temperature or vorticity over a flow via subtle, continuous line width and color variations.

Interrante, Victoria↗

DOE OSTI2026

Ammonolysis with N 2 -diluted NH 3 suppresses Ta( IV ) defects in BaTaO 2 N and enhances photocatalytic water oxidation

BaTaO 2 N stands out among oxynitride photocatalysts because of its ability to capture visible light and to drive the photoelectrochemical water oxidation reaction. However, its solar energy conversion performance is limited by electron–hole recombination at Ta( IV ) defects in the material. These defects are formed by overreduction of the Ta(v) oxide precursor by excess ammonia under the high temperature conditions during ammonolysis. Here we show for the first time that Ta( IV ) defect concentrations can be lowered by conducting the ammonolysis reaction in mixed NH 3 /N 2 gas. The obtained BaTaO 2 N samples crystallize in the cubic CaTiO 3 structure type and form 200–300 nm faceted nanocrystals, based on X-ray diffraction, scanning electron microscopy, and HRTEM. Electron paramagnetic resonance spectra observe the Ta( IV ) defects at g = 1.999 and confirm an 11-fold reduction for the product synthesized in mixed (0.13 : 1.0 vol) NH 3 /N 2 gas, equivalent to 1.14 × 10 16 cm −3 Ta( IV ) ions. This optimized BaTaO 2 N has nearly twice the photocatalytic oxygen evolution activity (AQE of 6.78% at 400 nm) of a reference material made with 1.0 atm ammonia and 78% higher photoelectrochemical water oxidation photocurrent (0.9 mA cm −2 at 1.23 V vs. RHE) under simulated sunlight. According to X-ray photoelectron spectroscopy, remaining Ta( IV ) defects are concentrated in the surface region of the BaTaO 2 N particles, where >50% of all Ta ions are found in the +4 oxidation state. This surface Ta( IV ) population can be directly observed in Vibrating Kelvin Probe Surface Photovoltage Spectra (VK-SPV) via its 1.2–1.4 eV photovoltage onset. Here, it suggests that the surface Ta( IV ) ions contribute empty d-states 0.5–0.7 eV below the BaTaO 2 N conduction band edge. These findings highlight how the energetics and concentrations of Ta( IV ) defects influence the photoelectrochemical water oxidation ability of BaTaO 2 N. Additionally, the work establishes ammonolysis with diluted NH 3 as a new tool to minimize defects in BaTaO 2 N and to raise its solar energy conversion efficiency toward its theoretical limit. Because of its simplicity, the reduced ammonia pressure strategy will likely be applicable to other oxynitrides, which generally suffer from overreduction problems during ammonolysis.

Salmanion, Mahya [University of California, Davis,↗

NASA NTRS1994

Computations of diabatic descent in the stratospheric polar vortex

A radiation model, together with National Meteorological Center temperature observations, was used to compute daily net heating rates in the northern hemisphere (NH) for the Arctic late fall and winter periods of both 1988-1989 and 1991-1992 and in the southern hemisphere (SH) for the Antarctic fall and winters of 1987 and 1992. The heating rates were interpolated to potential temperature (theta) surfaces between 400 K and 2000 K and averaged within the polar vortex, the boundary of which was determined by the maximum gradient in potential vorticity. The averaged heating rates were used in a one-dimensional vortex interior descent model to compute the change in potential temperature with time of air parcels initialized at various theta values, as well as to compute the descent in log pressure coodinates. In the NH vortex, air parcels which were initialized at 18 km on November 1, descended about 6 km by March 21, while air initially at 25 km descended 9 km in the same time period. this represents an average descent rate in the lower stratosphere of 1.3 to 2 km per month. Air initialized at 50 km descended 27 km between November 1 and March 21. In the SH vortex, parcels initialized at 18 km on March 1, descended 3 km, while air at 25 km descended 5-7 km by the end of October. This is equivalent to an average descent in the lower stratosphere of 0.4 to 0.9 km per month during this 8-month period. Air initialized at 52 km descended 26-29 km between March 1 and October 31. In both the NH and the SH, computed descent rates increased markedly with height. The descent for the NH winter of 1992-1993 and the SH winter of 1992 computed with a three-dimensional trajectory model using the same radiation code was within 1 to 2 km of that calculated by the one-dimensional model, thus validating the vortex averaging procedure. The computed descent rates generally agree well with observations of long-lived tracers, thus validating the radiative transfer model.

Rosenfield, Joan E.↗

NASA NTRSDate not supplied

Constraining Venus Cloud Habitability: Earth's Aerobiosphere as an Analogue Environment

The potential habitability of Venus's cloud and haze layers has been debated for decades, with interest fueled by observations including disequilibria in atmospheric chemistry, strongly UV-absorbing particles, and (most recently) a controversial phosphine detection. Venus cloud temperature and pressure are clement by Earth standards; however, the calculated high acid activity and low water activity may exceed the limits of Earth biochemistry, based on observed life in extreme environments. A significant challenge in understanding Venus's habitability is the lack of an appropriate terrestrial analogue environment. Life has not been found in hydrothermal systems approaching Venus aerosol acidities, but these systems also contain high levels of other harsh solutes. Earth's stratospheric sulfate layer is a partial match in terms of acidity, desiccation, size, and isolation from the surface, but the few samples returned from these altitudes have yielded only sparse, inactive cells. Earth's tropospheric cloud droplets have an active microbial presence, but are larger and far more water-rich than Venus aerosols; tropospheric times aloft are also similar to microbial generation times, making Earth's aerobiosphere dependent on continuous surface replenishment. Direct detection of potential biosignatures from a single transect is challenging; Earth's cloud microbiota yields 102 - 108 viable cells per mL, equivalent to one per 103 - 109 particles, with highly dynamic and heterogeneous distribution. The most important in situ measurement for Venus cloud habitability is detailed aerosol composition: confirmation of acid and water activity, presence of potentially bioavailable nutrients and energy, and potential presence of organic matter. Modeling Venus cloud aerosol residence time in comparison to periodic influxes of water and photochemical energy, and thus the ability of an ecosystem to maintain itself over time, would also address a significant habitability constraint particular to aerobiospheres.

Venus↗

NASA NTRS1995

Comparison between global latent heat flux computed from multisensor (SSM/I and AVHRR) and from in situ data

Comprehensive Ocean-Atmosphere Data Set (COADS) and satellite-derived parameters are input to a similarity theory-based model and treated in completely equivalent ways to compute global latent heat flux (LHF). In order to compute LHF exclusively from satellite measurements, an empirical relationship (Q-W relationship) is used to compute the air mixing ratio from Special Sensor Microwave/Imager (SSM/I) precipitable water W and a new one is derived to compute the air temperature also from retrieved W(T-W relationship). First analyses indicate that in situ and satellite LHF computations compare within 40%, but systematic errors increase the differences up to 100% in some regions. By investigating more closely the origin of the discrepancies, the spatial sampling of ship reports has been found to be an important source of error in the observed differences. When the number of in situ data records increases (more than 20 per month), the agreement is about 50 W/sq m rms (40 W/sq m rms for multiyear averages). Limitations of both empirical relationships and W retrieval errors strongly affect the LHF computation. Systematic LHF overestimation occurs in strong subsidence regions and LHF underestimation occurs within surface convergence zones and over oceanic upwelling areas. The analysis of time series of the different parameters in these regions confirms that systematic LHF discrepancies are negatively correlated with the differences between COADS and satellite-derived values of the air mixing ratio and air temperature. To reduce the systematic differences in satellite-derived LHF, a preliminary ship-satellite blending procedure has been developed for the air mixing ratio and air temperature.

Jourdan, Didier↗

DOE OSTI2021

Experimental Soil Warming and Permafrost Thaw Increase CH 4 Emissions in an Upland Tundra Ecosystem

Rapid Arctic warming is causing permafrost to thaw and exposing large quantities of soil organic carbon (C) to potential decomposition. In dry upland tundra systems, subsidence from thawing permafrost can increase surface soil moisture resulting in higher methane (CH 4 ) emissions from newly waterlogged soils. The proportion of C released as carbon dioxide (CO 2 ) and CH 4 remains uncertain as previously dry landscapes transition to a thawed state, resulting in both wetter and drier microsites. To address how thaw and moisture interact to affect total C emissions, here we measured CH 4 and CO 2 emissions from paired chambers across thaw and moisture gradients created by nine years of experimental soil warming in interior Alaska. Cumulative growing season (May–September) CH 4 emissions were elevated at both wetter (216.1–1,099.4 mg CH 4 -C m –2 ) and drier (129.7–392.3 mg CH 4 -C m –2 ) deeply thawed microsites relative to shallow thaw (55.6–215.7 mg CH 4 -C m –2 ) and increased with higher deep soil temperatures and permafrost thaw depth. Interannual variability in CH4 emissions was driven by wet conditions in graminoid-dominated plots that generated >70% of emissions in a wet year. Shoulder season emissions were equivalent to growing season CH 4 emissions rates in the deeply thawed, warmed soils, highlighting the importance of non-growing season CH 4 emissions. Net C sink potential was reduced in deeply thawed wet plots by 4%–42%, and by 3.5%–8% in deeply thawed drier plots due to anaerobic respiration, suggesting that some dry upland tundra landscapes may transition into stronger CH 4 sources in a warming Arctic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Metal-Catalyzed Thermo-Catalytic Decomposition and Continuous Catalyst Generation

In this study, metal dusting is utilized to initiate a two-stage thermo-catalytic decomposition (TCD) process. Stage 1 starts with metal-catalyzed TCD, and in stage 2 the metal-catalyzed carbon catalyzes additional TCD. TEM is presented of the early- versus late-stage TCD to qualitatively illustrate the second-stage TCD by the metal-catalyzed carbons. Corresponding SEM illustrates differences in growth type and surface density between early versus late reaction times, with backscattered imaging differentiating the first- versus second-stage TCD. TGA supports the microscopic inference of a second carbon phase by the presence of an early (low-temperature) reaction peak, characteristic of low-structure or disordered carbon as the second-stage TCD carbon. Raman analysis confirms that the second-stage carbon deposit is more disordered and unstructured, especially at 1000 °C, supported by the ID/IG and La value changes from 0.068 to 0.936 and 65 nm to 4.7 nm, respectively. To further confirm second-stage TCD occurrence upon pre-catalyzed carbons, two carbon blacks are tested. Exposing a combination of edge and basal or exclusively basal sites for the graphitized form, they afford a direct comparison of TCD carbon nanostructure dependence upon the initial carbon catalyst nanostructure. Pre-oxidation of the stainless-steel wool (SSW) prior to TCD is advantageous, accelerating TCD rates and increasing carbon yield relative to the nascent SSW for an equivalent reaction duration.

Chemistry↗