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NASA NTRS2001

Investigating Type I Polar Stratospheric Cloud Formation Mechanisms with POAM Satellite Observations

Type Ia PSCs are believed to be composed of nitric acid hydrate particles. Recent results from the SOLVE/THESEO 2000 campaign showed evidence that this type of PSC was composed of a small number of very large particles capable of sedimentary denitrification of regions of the stratosphere. It is unknown whether homogeneous or heterogeneous nucleation is responsible for the formation of these PSCs. Arctic winters are tending to be colder in response to global tropospheric warming. The degree to which this influences ozone depletion will depend on the freezing mechanism of nitric acid hydrate particles. If nucleation is homogeneous it implies that the freezing process is an inherent property of the particle, while heterogeneous freezing means that the extent of PSCs will depend in part on the number of nuclei available. The Polar Ozone and Aerosol Measurement (POAM)II and III satellites have been making observations of stratospheric aerosols and Polar Stratospheric Clouds (PSCs) since 1994. Recently, we have developed a technique that can discriminate between Type Ia and Ib PSCs using these observations. A statistical approach is employed to demonstrate the robustness of this approach and results are compared with lidar measurements. The technique is used to analyze observations from POAM II and II during Northern Hemisphere winters where significant PSC formation occurred with the objective of exploring Type I PSC formation mechanisms. The different PSCs identified using this method exhibit different growth curve as expressed as extinction versus temperature.

Strawa, Anthony W.↗

NASA NTRS1993

A model for heterogeneous chemical processes on the surfaces of ice and nitric acid trihydrate particles

The study presents a model that incorporates the physics and physical chemistry of ice surfaces relevant to polar stratospheric clouds. Surface concentrations of H2O, HCl, HOCl, ClONO2, and N2O5 on ice and nitric acid trihydrate (NAT) crystals are computed, and surface reaction rates and reaction probabilities (sticking coefficients) are determined. For gas pressures of about 10 exp -7 torr and temperatures in the range of 180-200 K, HCl completely coats ice and water-rich NAT surfaces, while HOCl, ClOHO2, and N2O5 may cover 0.01-1 percent of these surfaces. The energy parameters are used to calculate surface temperatures such as adsorption and desorption constants, surface coverages, reaction rate coefficients, surface diffusion coefficients, and reaction probabilities for various species and chemical interactions on ice and NAT surfaces. Implications for chemical processing on polar stratospheric clouds are discussed.

Tabazadeh, Azadeh↗

NASA NTRS2014

X-Ray Absorption near Edge Structure Spectroscopic Study of Hayabusa Category 3 Carbonaceous Particles

Analyses with a scanning transmission x-ray microscope (STXM) using x-ray absorption near edge structure (XANES) spectroscopy were applied for the molecular characterization of two kinds of carbonaceous particles of unknown origin, termed category 3, which were collected from the Hayabusa spacecraft sample catcher. Carbon-XANES spectra of the category 3 particles displayed typical spectral patterns of heterogeneous organic macromolecules; peaks corresponding to aromatic/olefinic carbon, heterocyclic nitrogen and/or nitrile, and carboxyl carbon were all detected. Nitrogen-XANES spectra of the particles showed the presence of N-functional groups such as imine, nitrile, aromatic nitrogen, amide, pyrrole, and amine. An oxygen-XANES spectrum of one of the particles showed a ketone group. Differences in carbon- and nitrogen-XANES spectra of the category 3 particles before and after transmission electron microscopic (TEM) observations were observed, which demonstrates that the carbonaceous materials are electron beam sensitive. Calcium-XANES spectroscopy and elemental contrast mapping identified a calcium carbonate grain from one of the category 3 particles. No fluorine-containing molecular species were detected in fluorine-XANES spectra of the particles. The organic macromolecular features of the category 3 particles were distinct from commercial and/or biological ‘fresh (non-degraded)’ polymers, but the category 3 molecular features could possibly reflect degradation of contaminant polymer materials or polymer materials used on the Hayabusa spacecraft. However, an extraterrestrial origin for these materials cannot currently be ruled out.

Asteroides↗

NASA NTRS2018

Implementation of a Comprehensive Ice Crystal Formation Parameterization for Cirrus and Mixed-Phase Clouds in the EMAC Model (Based on MESSy 2.53)

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to realistically represent ice crystal number concentrations. The parameterization of Barahona and Nenes (2009, hereafter BN09) allows the treatment of ice nucleation, taking into account the competition for water vapour between homogeneous and heterogeneous nucleation and pre-existing ice crystals in cold clouds. Furthermore, the influence of chemically-heterogeneous, polydisperse aerosols is considered via multiple ice nucleating particle spectra, which are included in the parameterization to compute the heterogeneously formed ice crystals. BN09 has been implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC results, BN09 produces fewer ice crystals in the upper troposphere but higher ice crystal number concentrations in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. The comparison with a climatological data set of aircraft measurements shows that BN09 used in the cirrus regime improves the model results and, therefore, is recommended for future EMAC simulations.

EMAC↗

NASA NTRS1998

Galileo Probe Measurements of Thermal and Solar Radiation Fluxes in the Jovian Atmosphere

The Galileo probe net flux radiometer (NFR) measured radiation fluxes in Jupiter's atmosphere from about 0.44 to 14 bars, using five spectral channels to separate solar and thermal components. Onboard calibration results confirm that the NFR responded to radiation approximately as expected. NFR channels also responded to a superimposed thermal perturbation, which can be approximately removed using blind channel measurements and physical constraints. Evidence for the expected NH3 cloud was seen in the spectral character of spin-induced modulations of the direct solar beam signals. These results are consistent with an overlying cloud of small NH3 ice particles (0.5-0.75 microns in radius) of optical depth 1.5-2 at 0.5 microns. Such a cloud would have so little effect on thermal fluxes that NFR thermal channels provide no additional constraints on its properties. However, evidence for heating near 0.45 bar in the NFR thermal channels would seem to require either an additional opacity source beyond this small-particle cloud, implying a heterogeneous-cloud structure to avoid conflicts with solar modulation results, or a change in temperature lapse rate just above the probe measurements. The large thermal flux levels imply water vapor mixing ratios that are only 6% of solar at 10 bars, but possibly increasing with depth, and significantly subsaturated ammonia at pressures less than 3 bars. If deep NH3 mixing ratios at the probe entry site are 3-4 times ground-based inferences, as suggested by probe radio signal attenuation, then only half as much water is needed to match NFR observations. No evidence of a water cloud was seen near the 5-bar level. The 5 microns thermal channel detected the presumed NH4SH cloud base near 1.35 bars. Effects of this cloud were also seen in the solar channel upflux measurements but not in the solar net fluxes, implying that the cloud is a conservative scatterer of sunlight. The minor thermal signature of this cloud is compatible with particle radii near 3 microns, but it cannot rule out smaller particles. Deeper than about 3 bars, solar channels indicate unexpectedly large absorption of sunlight at wavelengths longer than 0.6 microns, which might be due to unaccounted-for absorption by NH3 between 0.65 and 1.5 microns.

Sromovsky, L. A.↗

DOE OSTI2025

Trends in spatial correlations, two-phase coexistence, and criticality in a class of type-2 Schloegl models for autocatalysis

A class of type-2 Schloegl models is considered for particles on a square lattice with variable-range cooperativity. These models involve: (i) spontaneous particle annihilation at rate p; (ii) autocatalytic particle creation at unoccupied sites (i, j) with n ⩾ 2 particles within a specified neighborhood, Ω 𝑁 (i, j), of sites at rate $k_n$ = $\frac{^{(^n_2)}}{_{(^N_2)}}$ = $\frac{n{(n-1)}}{_{N(N-1)}}$; and (iii) possible spontaneous particle creation at unoccupied sites at “small” rate ɛ ⩾ 0. In some cases, Ω 𝑁 just includes all symmetry-equivalent sites at a single specific distance 𝑑 (in units of lattice constants) from the unoccupied site, e.g., 𝑑 = 1 (nearest-neighbor sites) where 𝑁 = 4, or 𝑑 = √5 (or √13 or…) where 𝑁 = 8. In other cases, Ω 𝑁 includes sites multiple distances from the unoccupied site, e.g., 𝑑 = {1,√2}, where 𝑁 = 8. Kinetic Monte Carlo (KMC) simulation reveals that these models exhibit a nonequilibrium discontinuous phase transition between high- and low-density states below a critical point, ɛ < ɛ c , with generic two-phase coexistence (2PC) at least for smaller 𝑁. With some exceptions, there is an approach toward mean-field behavior with increasing 𝑁 (so the regime of generic 2PC shrinks, and ɛ c approaches the mean-field value of 1/27). Additional insight into trends is provided by analysis of the exact master equations for the models via hierarchical truncation. These truncations utilize suitably tailored pair approximations which reflect the dominant nonequilibrium spatial correlations. These correlations in turn are shown to reflect the details of the autocatalytic particle creation process. For spatially heterogeneous states, the truncations produce coupled sets of lattice differential equations (LDE) which can describe orientation-dependent propagation of an interface between high- and low-density steady states for ɛ < ɛ c . Pair approximation values of 𝑝 = 𝑝 eq where the interface is stationary, and its orientation-dependence, are in semiquantitative agreement with KMC results. In conclusion, this comparison accounts for propagation failure in the LDE which complicates interpretation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS1986

Laser microprobe study of cosmic dust (IDPs) and potential source materials

The study of cosmic dust or interplanetary dust particles (IDP) can provide vital information about primitive materials derived primarily from comets and asteroids along with a small unknown fraction from the nearby interstellar medium. The study of these particles can enhance our understanding of comets along with the decoding of the history of the early solar system. In addition the study of the cosmic dust for IDP particles can assist in the elucidation of the cosmic history of the organogenic elements which are vital to life processes. Studies to date on these particles have shown that they are complex, heterogeneous assemblages of both amorphous and crystalline components. In order to understand the nature of these particles, any analytical measurements must be able to distinguish between the possible sources of these particles. A study was undertaken using a laser microprobe interfaced to a quadrupole mass spectrometer for the analysis of the volatile components present in cosmic dust particles, terrestrial contaminants present in the upper atmosphere, and primitive carbonaceous chondrites. From the study of the volatiles released from the carbonaceous materials it is hoped that one could distinguish between components and sources in the IDP particles analyzed. The technique is briefly described and results for the CI, CM, and CV chondrites and cosmic dust particle W7027B8 are presented.

Gibson, E. K., Jr.↗

NASA NTRS2012

The Mars Dust Cycle: Investigating the Effects of Radiatively Active Water Ice Clouds on Surface Stresses and Dust Lifting Potential with the NASA Ames Mars General Circulation Model

The dust cycle is a critically important component of Mars' current climate system. Dust is present in the atmosphere of Mars year-round but the dust loading varies with season in a generally repeatable manner. Dust has a significant influence on the thermal structure of the atmosphere and thus greatly affects atmospheric circulation. The dust cycle is the most difficult of the three climate cycles (CO2, water, and dust) to model realistically with general circulation models. Until recently, numerical modeling investigations of the dust cycle have typically not included the effects of couplings to the water cycle through cloud formation. In the Martian atmosphere, dust particles likely provide the seed nuclei for heterogeneous nucleation of water ice clouds. As ice coats atmospheric dust grains, the newly formed cloud particles exhibit different physical and radiative characteristics. Thus, the coupling between the dust and water cycles likely affects the distributions of dust, water vapor and water ice, and thus atmospheric heating and cooling and the resulting circulations. We use the NASA Ames Mars GCM to investigate the effects of radiatively active water ice clouds on surface stress and the potential for dust lifting. The model includes a state-of-the-art water ice cloud microphysics package and a radiative transfer scheme that accounts for the radiative effects of CO2 gas, dust, and water ice clouds. We focus on simulations that are radiatively forced by a prescribed dust map, and we compare simulations that do and do not include radiatively active clouds. Preliminary results suggest that the magnitude and spatial patterns of surface stress (and thus dust lifting potential) are substantial influenced by the radiative effects of water ice clouds.

Kahre, Melinda A.↗

DOE OSTI2022

Reaction Heterogeneity in LiFePO 4 Agglomerates and the Role of Intercalation-Induced Stress

As an important battery cathode material, reaction distribution in lithium iron phosphate (LiFePO4) has been extensively studied in dispersed particle systems, but remains poorly understood for mesoscopic agglomerates (or secondary particles) that are used in most commercial batteries. Herein, we apply three-dimensional X-ray spectroscopic imaging to characterize the two-phase structure in LiFePO4 secondary particles during electrochemical cycling. (De)lithiated domains are found to not form the commonly assumed core-shell structure but develop highly anisotropic filamentary morphology that is rate independent and symmetric between charging and discharging. Phase-field simulations elucidate that the observed 1D phase growth behavior is not caused by the 1D lithium diffusivity of LiFePO4 but the elastic interaction between primary particles, which gives rise to stronger reaction heterogeneity than dispersed nanoparticles. As a result, uniform lithium (de)intercalation does not occur on the secondary particle surface even at high cycling rates.

36 MATERIALS SCIENCE↗

DOE OSTI2022

The influence of multiple groups of biological ice nucleating particles on microphysical properties of mixed-phase clouds observed during MC3E

Abstract. A new empirical parameterization (EP) for multiple groups of primary biological aerosol particles (PBAPs) is implemented in the aerosol–cloud model (AC) to investigate their roles as ice nucleating particles (INPs). The EP describes the heterogeneous ice nucleation by (1) fungal spores, (2) bacteria, (3) pollen, (4) detritus of plants, animals, and viruses, and (5) algae. Each group includes fragments from the originally emitted particles. A high-resolution simulation of a midlatitude mesoscale squall line by AC is validated against airborne and ground observations. Sensitivity tests are carried out by varying the initial vertical profiles of the loadings of individual PBAP groups. The resulting changes in warm and ice cloud microphysical parameters are investigated. The changes in warm microphysical parameters, including liquid water content and cloud droplet number concentration, are minimal (<10 %). Overall, PBAPs have little effect on the ice number concentration (<6 %) in the convective region. In the stratiform region, increasing the initial PBAP loadings by a factor of 1000 resulted in less than 40 % change in ice number concentrations. The total ice concentration is mostly controlled by various mechanisms of secondary ice production (SIP). However, when SIP is intentionally shut down in sensitivity tests, increasing the PBAP loading by a factor of 100 has an effect of less than 3 % on the ice phase. Further sensitivity tests revealed that PBAPs have little effect on surface precipitation and on the shortwave and longwave flux (<4 %) for a 100-fold perturbation in PBAPs.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage

Abstract Single-crystal cathode materials for lithium-ion batteries have attracted increasing interest in providing greater capacity retention than their polycrystalline counterparts. However, after being cycled at high voltages, these single-crystal materials exhibit severe structural instability and capacity fade. Understanding how the surface structural changes determine the performance degradation over cycling is crucial, but remains elusive. Here, we investigate the correlation of the surface structure, internal strain, and capacity deterioration by using operando X-ray spectroscopy imaging and nano-tomography. We directly observe a close correlation between surface chemistry and phase distribution from homogeneity to heterogeneity, which induces heterogeneous internal strain within the particle and the resulting structural/performance degradation during cycling. We also discover that surface chemistry can significantly enhance the cyclic performance. Our modified process effectively regulates the performance fade issue of single-crystal cathode and provides new insights for improved design of high-capacity battery materials.

25 ENERGY STORAGE↗

DOE OSTI2025

Elucidating the phase transformations and grain growth behavior of O3-type sodium-ion layered oxide cathode materials during high temperature synthesis

Understanding the formation mechanism of layered oxide cathodes via solid-state synthesis is imperative to achieving controllability over their materials properties and electrochemical behaviors. In this work, we investigate the phase and microstructure evolution during the synthesis of NaNi 1/3 Fe 1/3 Mn 1/3 O 2 , a model sodium-ion layered oxide cathode, using a combination of imaging, diffraction, and spectroscopic techniques. We unravel the synthetic mechanistic pathways involved in the high-temperature calcination reaction, as well as elaborate the synthesis-microstructure-performance relationship of this material. The formation of the final layered oxide phase involves a gradual transformation through a sodiated oxyhydroxide intermediate. During the reaction, the precursor dehydration reaction dominates at 250–550 °C, while the major sodiation reaction occurs at 550–850 °C. Alongside multiple stages of phase transformations, the final grain structure formation occurs through the continuous growth of the (003) and (104) facets. During the reaction, Mn acts as the charge-compensating element and exhibits depth-dependent characteristics. When the sodiation reaction dominates over dehydration, the reaction intermediates undergo gradual electronic structure changes with increasing temperature, as indicated by the spectral features of TM3d-O2p hybrid states. Calcination duration is also a critical parameter governing the microstructure, surface reactivity, phase fraction distribution and electrochemical performance of the material. The optimal calcination duration was determined to be 18 hours at 850 °C under the conditions evaluated here. Calcination beyond this duration was found to be detrimental to electrochemical performance due to Na and O loss and heterogeneous sodium distribution throughout the particles. Our work sheds light on the complex crystallographic-chemical-microstructural evolution of sodium ion layered oxide cathodes and provides insight into precisely tuning material properties which are intimately linked to battery performances.

25 ENERGY STORAGE↗

NASA NTRS1978

Condensation and its growth down the test-section of the Langley 0.3-m transonic cryogenic tunnel

Four total pressure probes were used to measure the growth of condensation down the test section of the Langley 0.3-m tunnel, and the condensation data were employed to verify a mathematical model which assumes condensation results from heterogeneous nucleation on preexisting seed particles. The onset of effects occurs throughout the test section at the same total temperature but the magnitude of the effects increases with increasing length down the test section. Condensation is important because it determines the minimum operating temperature of transonic cryogenic wind tunnels.

Hall, R. M.↗

NASA NTRS1990

SMM mesospheric ozone measurements

The main objective was to understand the secular and seasonal behavior of ozone in the lower mesosphere, 50 to 70 km. This altitude region is important in understanding the factors which determine ozone behavior. A secondary objective is the study of stratospheric ozone in the polar regions. Use is made of results from the SBUV satellite borne instrument. In the Arctic the interaction between chlorine compounds and low molecular weight hydrocarbons is studied. More than 30,000 profiles were obtained using the UVSP instrument on the SMM spacecraft. Several orbits of ozone data per day were obtained allowing study of the current rise in solar activity from the minimum until the present. Analysis of Nimbus 7 SBUV data in Antarctic spring indicates that ozone is depleted within the polar vortex relative to ozone outside the vortex. This depletion confirms the picture of ozone loss at altitudes where polar stratospheric clouds exist. In addition, there is ozone loss above the cloud level indicating that there is another mechanism in addition to ozone loss initiated by heterogeneous chlorine reactions on cloud particles.

Aikin, A. C.↗

NASA NTRS1987

Zone heating for fluidized bed silane pyrolysis

An improved heated fluidized bed reactor and method for the production of high purity polycrystalline silicon by silane pyrolysis wherein silicon seed particles are heated in an upper heating zone of the reactor and admixed with particles in a lower reaction zone, in which zone a silane-containing gas stream, having passed through a lower cooled gas distribution zone not conducive to silane pyrolysis, contacts the heated seed particles whereon the silane is heterogeneously reduced to silicon.

Iya, Sridhar K.↗

NASA NTRS1989

Reactor for fluidized bed silane decomposition

An improved heated fluidized bed reactor and method for the production of high purity polycrystalline silicon by silane pyrolysis wherein silicon seed particles are heated in an upper heating zone of the reactor and admixed with particles in a lower zone, in which zone a silane-containing gas stream, having passed through a lower cooled gas distribution zone not conducive to silane pyrolysis, contacts the heated seed particles whereon the silane is heterogeneously reduced to silicon.

Iya, Sridhar K.↗

NASA NTRS2012

Formation and Processing of Amorphous Silicates in Primitive Carbonaceous Chondrites and Cometary Dust

Chondritic-porous interplanetary dust particles (CP IDPs) exhibit strongly heterogeneous and unequilibrated mineralogy at sub-micron scales, are enriched in carbon, nitrogen and volatile trace elements, and contain abundant presolar materials [1-4]. These observations suggest that CP IDPs have largely escaped the thermal processing and water-rock interactions that have severely modified or destroyed the original mineralogy of primitive meteorites. CP IDPs are believed to represent direct samples of the building blocks of the Solar System - a complex mixture of nebular and presolar materials largely unperturbed by secondary processing. The chemical and isotopic properties of CP IDPs and their atmospheric entry velocities are also consistent with cometary origins. GEMS (glass with embedded metal and sulfides) grains are a major silicate component of CP IDPs. GEMS grains are < 0.5 microns in diameter objects that consist of numerous 10 to 50 nm-sized Fe-Ni metal and Fe-Ni sulfide grains dispersed in a Mg-Si-Al-Fe amorphous silicate matrix [2, 5]. Based on their chemistry and isotopic compositions, most GEMS appear to be non-equilibrium condensates from the early solar nebula [2]. If GEMS grains are a common nebular product, then they should also be abundant in the matrices of the most physically primitive chondritic meteorites. Although amorphous silicates are common in the most primitive meteorites [6-9], their relationship to GEMS grains and the extent to which their compositions and microstructure have been affected by parent body processing (oxidation and aqueous alteration) is poorly constrained. Here we compare and contrast the chemical, microstructural and isotopic properties of amorphous silicates in primitive carbonaceous chondrites to GEMS grains in IDPs.

Keller, Lindsay P.↗

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↗