Spontaneous cracking of amorphous solid water films and the dependence on microporous structure
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Caixia Bu↗
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Effect of microstructure on spontaneous polarization in amorphous solid water films
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Caixia Bu↗
The Refractive Index of Amorphous and Crystalline Water Ice in the UV-vis
Amorphous solid water (ASW) is found on icy dust grains in the interstellar medium (ISM), as well as on comets and other icy objects in the outer solar system. The optical properties of ASW are thus relevant for many astrophysical environments, but in the ultraviolet–visible (UV–vis), its refractive index is not well constrained. Here, we introduce a new method based on UV–vis broadband interferometry to measure the wavelength dependent refractive index n(λ) of amorphous water ice from 10 to 130 K, i.e., for different porosities, in the wavelength range of 210–757 nm. We also present n(λ) for crystalline water ice at 150 K, which allows us to compare our new method with literature data. Based on this, a method to calculate n(λ, ρ) as a function of wavelength and porosity is reported. This new approach carries much potential and is generally applicable to pure and mixed ice, both amorphous and crystalline. The astronomical and physical–chemical relevance and future potential of this work are discussed.
Kofman, Vincent↗
Adsorption of Water on Simulated Moon Dust Samples
A lunar regolith simulant dust sample (JSC-1a) supported on a silica wafer (SiO2/Si(111)) has been characterized by scanning electron microscopy (SEM), energy dispersive x-ray spectroscopy (EDX), and Auger electron spectroscopy (AES). The adsorption kinetics of water has been studied primarily by thermal desorption spectroscopy (TDS) and also by collecting isothermal adsorption transients. The support has been characterized by water TDS. JSC-1a consists mostly of aluminosilicate glass and other minerals containing Fe, Na, Ca, and Mg. The particle sizes span the range from a few microns up to 100 microns. At small exposures, H2O TDS is characterized by broad (100 to 450 K) structures; at large exposures distinct TDS peaks emerge that are assigned to amorphous solid water (145 K) and crystalline ice (165 K). Water dissociates on JSC-1a at small exposures but not on the bare silica support. It appears that rather porous condensed ice layers form at large exposures. At thermal impact energies, the initial adsorption probability amounts to 0.92+/-0.05.
Goering, John P.↗
Amorphous ice and the behavior of cometary nuclei
The gradual heating of the nucleus of a comet approaching the sun may produce solid-state phase changes that are of particular importance for new comets, which may never have been heated before. The water-ice component of new comets is expected to be amorphous rather than crystalline, and its subsequent crystallization should produce gaseous tails and flareups at heliocentric distances about 70% greater than those expected for crystalline nuclei. These distances and the size of the flareups depend strongly on the inclination of the rotation axis and on the porosity of the ice. The effect should be weaker for older comets, but it may be related to the behavior of P/Schwassmann-Wachmann 1 if the layers of the crystallized ice peel off.
Smoluchowski, R.↗
Titania and Oberon: Surface Composition from New Near-Infrared Observations and Reflectance Models
Here we report the combination of new near-ir spectra (1.45-2.48 micrometers), of Titania and Oberon obtained in September 1995 at a resolving power of approx. 800, with older near-ir observations (0.5- 1.44 micrometers), and recent UV (0.22-0.48 micrometers) observations obtained with HST. Previous interpretations suggest these surfaces are chiefly composed of water ice and varying amounts of spectrally neutral material. The new near-ir data provide the opportunity to search for absorption bands that could be attributable to surface materials other than water ice and because the combined spectra include such a broad wavelength region, to undertake improved models of water and neutral components on the surface. The calculated near-ir geometric albedos clearly exhibit three broad spectral features. Two (1.52- & 2.05 micrometer) have previously been used to demonstrate the presence of water ice on these satellites. The third (approx. 1.65 micrometer), suggests the presence of hexagonal water ice at low temperatures, and may provide a mechanism of estimating the surface temperature. There is no spectral evidence for ices of CO2, CO, NH3 or CH4. At UV wavelengths there is a broad absorption near 0.27-0.28 micrometer previously attributed to OH formed by magnetospheric-surface interactions and retained at the low surface temperatures of these satellites. Surface components used in a Hapke scattering models include values for a combination of irradiated water ice in the UV and hexagonal water ice at 100k in the near-ir (IR), amorphous carbon (AC), and tholins (T) (produced from gas and solid). Results of these models suggest the surfaces of Titania/Oberon are composed of IW (-77/52%) with AC the next most abundant component (approx. 19/52%) and finally T (approx. 4/7%).
Roush, Ted L.↗
Solar system ice - Amorphous or crystalline?
The meteoritic bombardment of icy surfaces is discussed, focusing on the formation of amorphous ice and its thermal, mechanical, and optical properties. A numerical code has been developed for evaluating the ratio of the volume of the melted and vaporized ice target to the volume of the projectile that has impacted the surface and left a crater. However, water will only vaporize with impact speeds over 4 to 6 km/sec, and subsequent condensation into ice below 150 K will produce amorphous ice. A denser form of amorphous ice exists below 10 K, with the transition into a crystalline form occurring above 150 K. Maximum impact velocities have been defined for all major bodies in the solar system, with the finding that crystalline ice will form in the crater while amorphous ice will form on the ejecta. The amount of each is dependent on the ratio of solidified water to condensed water vapor and on the fraction of solid ejecta.
Smoluchowski, R.↗
Observation of interstellar ammonia ice
An absorption band probably due to solid ammonia on interstellar grains has been detected in the infrared spectrum at 2.97 microns of the Becklin-Neugebauer object and probably in NGC 2264-IR. An ammonia-water amorphous ice mixture can explain the structure of the new band and of the 3.07 microns interstellar absorption. Laboratory data suggest that a long wavelength wind extending to 3.5 microns in interstellar dust spectra may be absorption by NH3-H2O complexes in the ices. In the molecular cloud obscuring the BN object, about 20 times as much NH3 is frozen in grains as exists in the gas phase, suggesting the gas-grain interactions may be important in the ammonia chemistry of molecular clouds. Arguments are given that interstellar features at 6.0 and 6.8 microns are also ammonia-related absorptions.
Knacke, R. F.↗
Crystallization of amorphous water ice in the solar system
Electron diffraction studies of vapor-deposited water ice have characterized the dynamical structural changes during crystallization that affect volatile retention in cometary materials. Crystallization is found to occur by nucleation of small domains, while leaving a significant part of the amorphous material in a slightly more relaxed amorphous state that coexists metastably with cubic crystalline ice. The onset of the amorphous relaxation is prior to crystallization and coincides with the glass transition. Above the glass transition temperature, the crystallization kinetics are consistent with the amorphous solid becoming a "strong" viscous liquid. The amorphous component can effectively retain volatiles during crystallization if the volatile concentration is approximately 10% or less. For higher initial impurity concentrations, a significant amount of impurities is released during crystallization, probably because the impurities are trapped on the surfaces of micropores. A model for crystallization over long timescales is described that can be applied to a wide range of impure water ices under typical astrophysical conditions if the fragility factor D, which describes the viscosity behavior, can be estimated.
NASA Center ARC↗
Comparing Wild 2 Particles to Chondrites and IDPS
We compare the observed composition ranges of olivine, pyroxene and Fe-Ni sulfides in Wild 2 grains, comparing these with chondritic IDPs and chondrite classes to explore whether these data suggest affinities to known hydrous materials in particular. Wild 2 olivine has an extremely wide composition range, from Fo4-100 with a pronounced frequency peak at Fo99. The composition range displayed by the low-calcium pyroxene is also very extensive, from En52 to En100, with a significant frequency peak centered at En95. These ranges are as broad or broader than those reported for any other extraterrestrial material. Wild 2 Fe-Ni sulfides mainly have compositions close to that of FeS, with less than 2 atom % Ni - to date, only two pentlandite grains have been found among the Wild-grains suggesting that this mineral is not abundant. The complete lack of compositions between FeS and pentlandite (with intermediate solid solution compositions) suggests (but does not require) that FeS and pentlandite condensed as crystalline species, i.e. did not form as amorphous phases, which later became annealed. While we have not yet observed any direct evidence of water-bearing minerals, the presence of Ni-bearing sulfides, and magnesium-dominated olivine and low-Ca pyroxene does not rule out their presence at low abundance. We do conclude that modern major and minor element compositions of chondrite matrix and IDPs are needed.
Zolensky, Michael↗
Hydrogen Isotopic Composition of Water in the Martian Atmosphere and Released from Rocknest Fines
The Mars Science Laboratory Curiosity rover sampled the aeolian bedform called Rocknest as its first solid samples to be analyzed by the analytical instruments CheMin and SAM. The instruments ingested aliquots from a sieved sample of less than 150 micrometer grains. As discussed in other reports at this conference [e.g., 1], CheMin discovered many crystalline phases, almost all of which are igneous minerals, plus some 10s of percent of x-ray amorphous material. The SAM instrument is focused on understanding volatiles and possible organics in the fines, performing evolved gas analysis (EGA) with the SAM quadrapole mass spectrometer (QMS), isotope measurements using both the QMS and the tunable laser spectrometer (TLS), which is sensitive to CO2, water and methane, and organics with the gas chromatograph mass spectrometer (GCMS). As discussed in the abstract by Franz et al. [2] and others, EGA of Rocknest fines revealed the presence of significant amounts of H2O as well as O-, C- and S-bearing materials. SAM has also tasted the martian atmosphere several times, analyzing the volatiles in both the TLS and QMS [e.g., 3,4]. This abstract will focus on presentation of initial hydrogen isotopic data from the TLS for Rocknest soils and the atmosphere, and their interpretation. Data for CO2 isotopes and O isotopes in water are still being reduced, but should be available by at the conference.
Leshin, L. A.↗
Sublimation and reformation of icy grains in the primitive solar nebula
The quantity of water ice that sublimates during the free fall of grains into the solar nebula from a surrounding interstellar cloud varies from over 90 percent of the grain mass as 30 AU from the nebular center to less than 10 percent at more than 100 AU. Virtually all the water that is sublimated ultimately recondenses, since the cold nebular gas lying beyond 10 AU is unable to hold more than a small portion as vapor. The return of most of the gas to solid phase near the nebular ambient temperature, of about 50 K, may result in at least two grain populations consisting, in one case, of unaltered interstellar grains which did not undergo sublimation, and in the other of water ice which cocondensed with more volatile gases at nebular ambient temperatures to yield volatile-rich amorphous phases.
Lunine, Jonathan I.↗
Applying state diagrams to food processing and development
The physical state of food components affects their properties during processing, storage, and consumption. Removal of water by evaporation or by freezing often results in formation of an amorphous state (Parks et al., 1928; Troy and Sharp, 1930; Kauzmann, 1948; Bushill et al., 1965; White and Cakebread, 1966; Slade and Levine, 1991). Amorphous foods are also produced from carbohydrate melts by rapid cooling after extrusion or in the manufacturing of hard sugar candies and coatings (Herrington and Branfield, 1984). Formation of the amorphous state and its relation to equilibrium conditions are shown in Fig. 1 [see text]. The most important change, characteristic of the amorphous state, is noticed at the glass transition temperature (Tg), which involves transition from a solid "glassy" to a liquid-like "rubbery" state. The main consequence of glass transition is an increase of molecular mobility and free volume above Tg, which may result in physical and physico-chemical deteriorative changes (White and Cakebread, 1966; Slade and Levine, 1991). We have conducted studies on phase transitions of amorphous food materials and related Tg to composition, viscosity, stickiness, collapse, recrystallization, and ice formation. We have also proposed that some diffusion-limited deteriorative reactions are controlled by the physical state in the vicinity of Tg (Roos and Karel, 1990, 1991a, b, c). The results are summarized in this article, with state diagrams based on experimental and calculated data to characterize the relevant water content, temperature, and time-dependent phenomena of amorphous food components.
Non-NASA Center↗
Transformation of Graphitic and Amorphous Carbon Dust to Complex Organic Molecules in a Massive Carbon Cycle in Protostellar Nebulae
More than 95% of silicate minerals and other oxides found in meteorites were melted, or vaporized and recondensed in the Solar Nebula prior to their incorporation into meteorite parent bodies. Gravitational accretion energy and heating via radioactive decay further transformed oxide minerals accreted into planetesimals. In such an oxygen-rich environment the carbonaceous dust that fell into the nebula as an intimate mixture with oxide grains should have been almost completely converted to CO. While some pre-collapse, molecular-cloud carbonaceous dust does survive, much in the same manner as do pre-solar oxide grains, such materials constitute only a few percent of meteoritic carbon and are clearly distinguished by elevated D/H, N-15/N-16, C-13/C-12 ratios or noble gas patterns. Carbonaceous Dust in Meteorites: We argue that nearly all of the carbon in meteorites was synthesized in the Solar Nebula from CO and that this CO was generated by the reaction of carbonaceous dust with solid oxides, water or OH. It is probable that some fraction of carbonaceous dust that is newly synthesized in the Solar Nebula is also converted back into CO by additional thermal processing. CO processing might occur on grains in the outer nebula through irradiation of CO-containing ice coatings or in the inner nebula via Fischer-Tropsch type (FTT) reactions on grain surfaces. Large-scale transport of both gaseous reaction products and dust from the inner nebula out to regions where comets formed would spread newly formed carbonaceous materials throughout the solar nebula. Formation of Organic Carbon: Carbon dust in the ISM might easily be described as inorganic graphite or amorphous carbon, with relatively low structural abundances of H, N, O and S . Products of FTT reactions or organics produced via irradiation of icy grains contain abundant aromatic and aliphatic hydrocarbons. aldehydes, keytones, acids, amines and amides.. The net result of the massive nebular carbon cycle is to convert relatively inert carbonaceous dust from the ISM into the vital organic precursors to life such as amino acids and sugars intimately mixed with dust and ice in primitive planetesimals. Since the number of carbon atoms entering the Solar Nebula as dust exceeds the number of atoms entering the nebula as oxide grains. the formation of large quantities of complex organic molecules may represent the largest single chemical cycle in the nebula.
Nuth, Joseph A., III↗
Toughening of BIS maleimide resins: Synthesis and characterization of maleimide terminated poly(arylene ether) oligomers and polymers
Amine functional poly(arylene ether) sulfones were previously reported. Herein, the chemistry was extended to amorphous poly(arylene ether) ketones because of their higher fracture toughness values, relative to the polysulfones. It was demonstrated that the amino functional oligomers undergo a self-crosslinking reaction at temperatures above about 220 C. This produces an insoluble, but ductile network that has excellent resistance. A ketamine structure hypothesis was proposed and verified using solid state magic angle NMR. In most cases, the water generated upon ketamine formation is too low to produce porosity and solid networks are obtained. The stability of the ketamine networks towards hydrolysis is excellent. The chemistry was further demonstrated to be able to crosslink preformed nonfunctional poly(arylene ether) ketones if a difunctional amine was utilized. This concept has the possibility of greatly improving the creep resistance of thermoplastics. Also, a new technique was developed for converting the amine functional oligomers cleanly into maleimide structures. This method involves reacting maleic anhydride with monomeric aminophenols in the presence of solvent mixtures.
Mcgrath, J. E.↗
Far infrared spectra of amorphous and crystalline water ice and changes in these phases as the result of proton irradiation
Far infrared spectra from 20 microns (500 cm(sup -1)) to 100 microns (100 cm(sup -1)) of water ice were measured. Amorphous ice deposited at 13 K has one absorption band at 45 microns (220 cm(sup -1)). Amorphous ice evolves into a crystalline form with absorptions at 44 microns (229 cm(sup -1)) and 62 microns (162 cm(sup -1)) as the temperature is increased to 155 K. Spectra documenting this phase change are presented as well as spectra of crystalline ice at temperatures between 13 K and 155 K. Far infrared spectra of amorphous and crystalline water ice before and after proton irradiation are also presented. Changes in these two forms are discussed in relation to ices in comets, grains, and planetary satellites in various radiation environments. Observations of non-terrestrial clathrate hydrates are still lacking despite the fact that clathrates first were suggested to exist in cometary and interstellar ices over forty years ago. Spectroscopy, the most direct method of astronomical detection, has been hampered by the similarity of clathrate hydrate spectra to those of unenclathrated guest molecules and solid H2O. A methanol (CH3OH) clathrate hydrate, using a recently published procedure, was prepared and its far-IR spectrum investigated. The spectrum is quite differenct from that of either unenclathrated CH3OH or solid H2O and so should be of value in astronomical searches for this clathrate.
Hudson, Reggie L.↗
Spitzer IRS Spectroscopy of the 10 Myr-Old EF Cha Debris Disk: Evidence for Phyllosilicate-Rich Dust in the Terrestrial Zone
We describe Spitzer IRS spectroscopic observations of the approx. 10 Myr-old star, EF Chao Compositional modeling of the spectra from 5 micron to 35 micron confirms that it is surrounded by a luminous debris disk with L(sub D)/L(sub *) approx. 10(exp -3), containing dust with temperatures between 225 K and 430 K characteristic of the terrestrial zone. The EF Cha spectrum shows evidence for many solid-state features, unlike most cold, low-luminosity debris disks but like some other 10-20 Myr-old luminous, warm debris disks (e.g. HD 113766A). The EF Cha debris disk is unusually rich in a species or combination of species whose emissivities resemble that of finely-powdered, laboratory-measured phyllosilicate species (talc, saponite, and smectite), which are likely produced by aqueous alteration of primordial anhydrous rocky materials. The dust and, by inference, the parent bodies of the debris also contain abundant amorphous silicates and metal sulfides, and possibly water ice. The dust's total olivine to pyroxene ratio of approx. 2 also provides evidence of aqueous alteration. The large mass volume of grains with sizes comparable to or below the radiation blow-out limit implies that planetesimals may be colliding at a rate high enough to yield the emitting dust but not so high as to devolatize the planetesimals via impact processing. Because phyllosilicates are produced by the interactions between anhydrous rock and warm, reactive water, EF Cha's disk is a likely signpost for water delivery to the terrestrial zone of a young planetary system.
Currie, Thayne↗
Salt Distribution from Freezing Intrusions in Ice Shells on Ocean Worlds: Application to Europa
Several icy moons and dwarf planets appear to have hosted subsurface liquid water. Liquid water intruding upwards into the icy outer shells of these worlds freezes, forming ice and (from ocean solutes) non-ice solids. Here, we model concentrated aqueous solutions below 273 K to simulate the compositional evolution of freezing spherical intrusions. Starting solutions are based on five previously reported compositional end members for Europa's ocean. For moderate-pH end members dominated by chloride, sulfate, and/or carbonate, the solids formed include Ca-, Mg-, and Na-sulfates and -carbonates, as well as Na- and K-chlorides. For silica-rich, high-pH end members, abundant amorphous silica forms with, potentially, similarly abundant NaOH and KOH. We further develop a new numerical model to compute the spatial distribution of the formed solids and residual brine as freezing progresses. If non-ice solids settle to the bottom, their deposits tend to have stacked hourglass shapes, widening each time the crystallization temperature of a new solid is reached. We discuss the applicability of this model to vertical fractures and global freezing of a subsurface ocean. These results inform (i) how compositional heterogeneities may affect the thermophysical properties of ice shells, which in turn influence convective and cryovolcanic transport, (ii) the compatibility of brine pockets with physicochemical conditions suitable for microbial life, and (iii) possible measurements of compositional heterogeneities within ice shells by spacecraft such as NASA's Europa Clipper and ESA's JUICE missions. The methodology developed here is applicable to other ice-covered ocean worlds.
Planetary structure↗