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DOE OSTI2025

Multiscale electro-chemo-mechanical model of high-capacity amorphous silicon anode material in sodium-ion batteries

The growing interest in sodium-ion batteries (SIBs) is fueled by their abundant resources and environmentally friendly nature, with amorphous silicon (a-Si) emerging as a promising anode material for enhancing capacity. However, the key challenge lies in sustaining reversible capacity during cycling. Here, in this work, we developed a multiscale electrochemical model incorporating an a-Si anode to elucidate the performance parameters of SIBs. Additionally, we integrated an electro-chemo-mechanical model at the particle level to capture stress generation, an essential factor in the degradation of high-capacity electrodes. Unlike existing models, our approach accounts for large-deformation chemo-mechanics at the particle scale and includes simulations under varying charge rates to explore multiscale behavior. The results reveal that coupled sodiation significantly prolongs complete cycling times and influences discharge dynamics, indicating that neglecting this coupling leads to an underestimation of actual capacity. Furthermore, we observed pronounced polarization effects at higher charge rates, resulting in heterogeneous stress distributions across the anode. With the identification of critical failure parameters for both active particles and binder materials, offering novel insights for mitigating degradation in high-capacity electrode systems.

Amorphous silicon anode↗

NASA NTRS1999

Comparative Wide Temperature Core Loss Characteristics of Two Candidate Ferrites for the NASA/TRW 1500 W PEBB Converter

High frequency core loss and magnetization properties of commercial type MN8CX and PC40, high resistivity, MnZn based, power ferrites are presented over the temperature range of -l50 C to 150 C, at selected values of peak flux density (B (sub p)). Most of the data is at 100 kHz, with some data extended to 200 and 300 kHz for the MN8CX. Plots of the specific Core loss against temperature exhibit the minimal characteristic of such ferrites. These plots show that the MN8CX is optimized for minimum loss at about 25 C, whereas the PC40 is optimized at about 80 C. At the points of minimum loss and for the same B (sub p), the MN8CX has roughly half the losses of the PC40 at the lower flux densities. This loss ratio continues down to cryogenic temperatures. However, above about 80 C the losses are practically equal. The lowest 100 kHz loss recorded, 50 mW/cm3 for the MNGCX at a B (sub p) of 0.1T, equals that of a very low loss, Co based, transverse magnetically annealed, amorphous ribbon material. Except possibly at lower B (sub p) or much higher frequencies, these ferrites are not competitive for low losses over a wide temperature range with certain specialty amorphous materials. Permeability is computed from a linear model, plots against temperature are presented and again compared to the specialty amorphous materials.

Niedra, Janis M.↗

NASA NTRS2000

From Interstellar PAHs and Ices to the Origin of Life

Tremendous strides have been made in our understanding of interstellar material over the past twenty years thanks to significant, parallel developments in observational astronomy and laboratory astrophysics. Twenty years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds ignored, and the notion of large, abundant, gas phase, carbon rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of dust in the diffuse ISM is reasonably well constrained to micron-sized cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. In dense molecular clouds, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose composition is very well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by earlier interstellar chemistry standards, is widespread throughout the Universe. The first part of this lecture will describe how infrared studies of interstellar space, combined with laboratory simulations, have revealed the composition of interstellar ices (the building blocks of comets) and the high abundance and nature of interstellar PAHs. The laboratory database has now enabled us to gain insight into the identities, concentrations, and physical state of many interstellar materials. Within a dense molecular cloud, and especially in the solar nebula during the star and planet formation stage, the materials frozen into interstellar/precometary ices are photoprocessed by ultraviolet light, producing more complex molecules. The remainder of the presentation will focus on the photochemical evolution of these materials and the possible role of these compounds on the early Earth. As these materials are thought to be the building blocks of comets and related to the carbonaceous components of micrometeorites, they are likely to have been important sources of complex organic materials on the early Earth and their composition may be related to the origin of life.

Allamandola, Louis J.↗

NASA NTRS1998

Fifteen Years of Laboratory Astrophysics at Ames

Tremendous strides have been made in our understanding of interstellar material over the past fifteen years thanks to significant, parallel developments in two closely related areas: observational astronomy and laboratory astrophysics. Fifteen years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds ignored, and the notion of large, abundant, gas phase, carbon-rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of dust in the diffuse ISM is reasonably well constrained to cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. In the dense ISM, these cold dust particles are coated with mixed-molecular ices whose compositions are very well known. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by early interstellar chemistry standards, is widespread throughout the ISM. This great progress has only been made possible by the close collaboration of laboratory experimentalists with observers and theoreticians, all with the goal of applying their skills to astrophysical problems of direct interest to NASA programs. Such highly interdisciplinary collaborations ensure fundamental, in depth coverage of the wide-ranging challenges posed by astrophysics. These challenges include designing astrophysically focused experiments and data analysis, tightly coupled with astrophysical searches spanning 2 orders of magnitude in wavelength, and detailed theoretical modeling. The impact of our laboratory has been particularly effective as there is constant cross-talk and feedback between quantum theorists; theoretical astrophysicists and chemists; experimental physicists; organic, physical and petroleum chemists; and infrared and UV/Vis astronomers. In this paper, two examples of the Ames Program will be given. We have been involved in identifying 9 out of the 14 interstellar pre-cometary ice species known, determined their abundances and the physical nature of the ice structure. Details on our ice work are given in the paper by Sandford et al. Our group is among the pioneers of the PAH model. We built the theoretical framework, participated in the observations and developed the experimental techniques needed to test the model. We demonstrated that the ubiquitous infrared emission spectrum associated with many interstellar objects can be matched by laboratory spectra of neutral and positively charged PAHs and that PAHs were excellent candidates for the diffuse interstellar band (DIB) carriers. See Salama et al. and Hudgins et al.

Allamandola, L. J.↗

NASA NTRS2002

The Exobiological Role of Interstellar Polycyclic Aromatic Hydrocarbons and Ices

Tremendous strides have been made in our understanding of interstellar material over the past twenty years thanks to significant, parallel developments in observational astronomy and laboratory astrophysics. Before this time, the composition of interstellar dust was largely guessed-at, the presence of ices in interstellar clouds ignored, and the notion that large, gas phase, carbon rich molecules might be abundant and widespread throughout the interstellar medium (ISM) considered impossible. Today, the composition of dust in the ISM is reasonably well constrained to micron-sized cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. Shrouded within the protective confines of cold, opaque molecular clouds--the birthplace of stars and planets--these cold dust particles secrete mantles of mixed molecular ices whose compositions are also well constrained. Finally, amidst the molecular inventory of these ice mantles are likely to be found polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by the standards of interstellar chemistry, the telltale infrared spectral signature of which is now recognized throughout the Universe. In the first part of this talk, we will review the spectroscopic evidence that forms the basis for the currently accepted abundance and ubiquity of PANs in the ISM. We will then look at a few specific examples which illustrate how experimental and theoretical data can be applied to interpret the interstellar spectra and track how the PAN population evolves as it passes from its formation site in the circumstellar outflows of dying stars, through the various phases of the ISM, and into forn~iing planetary systems. Nevertheless, despite the fact that PANs likely represent the single largest molecular reservoir of organic carbon in evolving planetary systems, they are not what would be considered "biogenic" molecules. Although interesting from a chemical and astrophysical standpoint, in the absence of a mechanism by which this population can be dislodged from the precipitous thermodynamic well afforded by their extensive aromatic networks, they are of little Astrobiological significance. Consequently, for the remainder of the talk, we will consider the photochemical evolution of PANS under conditions similar to those found in the ISM and in proto-planetary systems with an eye toward means by which this rich repository of pre-biotic organic "ore" might be converted into materials of greater importance to Astrobiology.

Hudgins, Douglas M.↗

NASA NTRS2004

From Interstellar Polycyclic Aromatic Hydrocarbons and Ice to the Origin of Life

Tremendous strides have been made in our understanding of interstellar material over the past twenty years thanks to significant, parallel developments in observational astronomy and laboratory astrophysics. Twenty years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds ignored, and the notion of large, abundant, gas phase, carbon rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of dust in the diffuse ISM is reasonably well constrained to cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. In the dense ISM, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose composition is very well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by early interstellar chemistry standards, is widespread throughout the Universe. The first part of this talk will describe how infrared studies of interstellar space, combined with laboratory simulations, have revealed the composition of interstellar ices (the building blocks of comets) and the high abundance and nature of interstellar PAHs. The laboratory database has now enabled us to gain insight into the identities, abundances, and physical state of many interstellar materials. Within a dense molecular cloud, and especially in the presolar nebula, the materials frozen into the interstellar/precometary ices are photoprocessed by ultraviolet light and produce more complex molecules. The remainder of the presentation will focus on the photochemical evolution of these materials and the possible role of these compounds on the to the carbonaceous components of micrometeorites, they are likely to have been important sources of complex materials on the early Earth and their composition may be related to the origin of life.

Allamandola, Louis↗

DOE OSTI2026

A Review of Advanced Characterization Methods and Techniques for Amorphous and Poorly Crystalline Materials Applicable to Cementitious Waste Forms

This review covers advanced characterization methods of cementitious materials. The particular focus is to understand cementitious compositions with amorphous content because conventional techniques such as X-ray diffraction are more applicable to materials with long range order. Also of interest is advanced characterization that provides deeper insights into properties such as porosity. There are five groups of characterization methods discussed in this review which are: electron beam/microscopy, X-ray, neutron diffraction and scattering, nuclear magnetic resonance, and optical techniques. The techniques can be further grouped by the categories of nanoscale structural understanding (transmission electron microscopy and pair distribution function), microscale structural understanding (focused ion beam and x-ray tomography), microscopic elemental distributions (energy dispersive spectroscopy and X-ray fluorescence), and chemical binding information (electron energy loss spectroscopy, x-ray absorption spectroscopy, nuclear magnetic resonance, Raman spectroscopy, and infrared spectroscopy), with advantages and disadvantages of each method discussed. The recommendation for further research is to begin with techniques that are easier to prepare samples for, measure, and analyze, such as the optical techniques of Raman and infrared spectroscopy. If more information is needed, pursue collaborations, other techniques, or proposals for beam time at the synchrotron sources.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1994

Radiation Resistance Studies of Amorphous Silicon Alloy Photovoltaic Materials

The radiation resistance of commercial solar cells fabricated from hydrogenated amorphous silicon alloys was investigated. A number of different device structures were irradiated with 1.0 MeV protons. The cells were insensitive to proton fluences below 1E12 sq cm. The parameters of the irradiated cells were restored with annealing at 200 C. The annealing time was dependent on proton fluence. Annealing devices for one hour restores cell parameters for fluences below lE14 sq cm require longer annealing times. A parametric fitting model was used to characterize current mechanisms observed in dark I-V measurements. The current mechanisms were explored with irradiation fluence, and voltage and light soaking times. The thermal generation current density and quality factor increased with proton fluence. Device simulation shows the degradation in cell characteristics may be explained by the reduction of the electric field in the intrinsic layer.

Woodyard, James R.↗

DOE OSTI2024

Reverse Polarizability of Rare Earth Ions (La 3+ , Gd 3+ , Lu 3+ , Y 3+ ) in Tellurite Glasses and Glass Ceramics for Optical Limiting

All-optical modulation using inherent third-order optical nonlinearity of a medium has garnered considerable interest in photonics and optoelectronics. Herein, nonlinear optical (NLO) properties of tellurite glasses and glass ceramics (GCs) containing four different rare earths (RE = La, Gd, Lu, and Y) have been deliberated in near-infrared regions under an ultrafast regime. The La-based glass exhibits ~10 times higher nonlinear refraction (n 2 ) and absorption (α 2 ) than reported NLO materials. The NLO susceptibility [χ (3) ] trend in the studied glasses is La > Gd > Lu > Y, matching with RE 3+ polarizability. Furthermore, Ln 2 Te 6 O 15 nanocrystallite-embedded transparent GCs exhibit a larger NLO coefficient due to the enhanced local field from oxygen vacancies in crystallites. Interestingly, the trend of χ (3) in GCs follows the sequence of Y > Lu > Gd > La, precisely opposite to the glasses. This observation challenges the general polarizability approach of RE 3+ ions, emphasizing that quadratic hyperpolarizability of RE 3+ is pivotal for NLO properties of GCs. Among the studied matrices, Y-containing GCs showed the lowest optical limiting (OL) threshold (5.4 mJ/cm 2 at 800 nm), much lower than those of the reported NLO materials, suggesting its potential as a femtosecond NIR-laser safety material. A combination of large α 2 and n 2 from the studied matrices indicates their advantage for harmonic generation, potentially aiding in the design of ultrafast signal processing devices.

36 MATERIALS SCIENCE↗

NASA NTRS2010

Formation, Structure and Properties of Amorphous Carbon Char from Polymer Materials in Extreme Atmospheric Reentry Environments

Amorphous carbonaceous char produced from the pyrolysis of polymer solids has many desirable properties for ablative heat shields for space vehicles. Molecular dynamics simulations are presented to study the transformation of the local atomic structure from virgin polymer to a dense, disordered char [1]. Release of polymer hydrogen is found to be critical to allow the system to collapse into a highly coordinated char structure. Mechanisms of the char formation process and the morphology of the resulting structures are elucidated. Thermal conductivity and mechanical response of the resulting char are evaluated [2]. During reenty, the optical response and oxidative reactivity of char are also important properties. Results of ab initio computations of char optical functions [3] and char reactivity [4] are also presented.

Lawson, John W.↗

NASA NTRS2020

Phyllosilicate Transitions in Ferromagnesian Soils: Short-Range Order Materials and Smectites Dominate Secondary Phases

Analyses of X-ray diffraction (XRD) patterns taken by the CheMin instrument on the Curiosity Rover in Gale crater have documented the presence of clay minerals interpreted as smectites and a suite of amorphous to short-range order materials termed X-ray amorphous materials. These X-ray amorphous materials are commonly ironrich and aluminum poor and likely some of them are weathering products rather than primary glasses due to the presence of volatiles. Outstanding questions remain regarding the chemical composition and mineral structure of these X-ray amorphous materials and the smectites present at Gale crater and what they indicate about environmental conditions during their formation. To gain a better understanding of the mineral transitions that occur within ferromagnesian parent materials, we have investigated the development of secondary clay minerals and shortrange order materials in two soil chronosequences with varying climates developing on ultramafic bedrock. Field Sites: We investigated soil weathering within two field locations, the Klamath Mountains of Northern California, and the Tablelands of Newfoundland, Canada. Both sites possess age dated or correlated recently deglaciated soils and undated but substantially older soils. In the Klamath mountains the Trinity Ultramafic Body was deglaciated roughly 15,000 years bp while in the Tablelands a moraine was dated to about 17,600 years bp. The Klamath Mountains feature a seasonally wet and dry climate while the Tablelands are wet year-round with saturated soil conditions observed during sampling and standing water observed within 3 of 4 soil pit sampling locations.

Feldman, A. D.↗

NASA NTRS2018

Amorphous Phase Characterization Through X-Ray Diffraction Profile Modeling: Implications for Amorphous Phases in Gale Crater Rocks and Soils

The CheMin X-ray diffraction instrument on the Mars Science Laboratory rover has analyzed 18 rock and soil samples in Gale crater. Diffraction data allow for the identification of major crystalline phases based on the positions and intensities of well-defined peaks and also provides information regarding amorphous and poorly-ordered materials based on the shape and positions of broad scattering humps. The combination of diffraction data, elemental chemistry from APXS (Alpha Particle X-ray Spectrometer) and evolved gas analyses (EGA) from SAM (Sample Analysis at Mars) help constrain possible amorphous materials present in each sample (e.g., glass, opal, iron oxides, sulfates) but are model dependent. We present a novel method to characterize amorphous material in diffraction data and, through this approach, aim to characterize the phases collectively producing the amorphous profiles in CheMin diffraction data. This method may be applied to any diffraction data from samples containing X-ray amorphous materials, not just CheMin datasets, but we re-strict our discussion to Martian-relevant amorphous phases and diffraction data measured by CheMin or CheMin-like instruments.

Achilles, C. N.↗

NASA NTRS1989

Thin film memory matrix using amorphous and high resistive layers

Memory cells in a matrix are provided by a thin film of amorphous semiconductor material overlayed by a thin film of resistive material. An array of parallel conductors on one side perpendicular to an array of parallel conductors on the other side enable the amorphous semiconductor material to be switched in addressed areas to be switched from a high resistance state to a low resistance state with a predetermined level of electrical energy applied through selected conductors, and thereafter to be read out with a lower level of electrical energy. Each cell may be fabricated in the channel of an MIS field-effect transistor with a separate common gate over each section to enable the memory matrix to be selectively blanked in sections during storing or reading out of data. This allows for time sharing of addressing circuitry for storing and reading out data in a synaptic network, which may be under control of a microprocessor.

Thakoor, Anilkumar P.↗

NASA NTRS1993

A photovoltaic catenary-tent array for the Martian surface

To provide electrical power during an exploration mission to Mars, a deployable tent-shaped structure with a flexible photovoltaic (PV) blanket is proposed. The array is designed with a self-deploying mechanism utilizing pressurized gas expansion. The structural design for the array uses a combination of cables, beams, and columns to support and deploy the PV blanket. Under the force of gravity, a cable carrying a uniform load will take the shape of a catenary curve. A catenary-tent collector is self shading which must be taken into account in the solar radiation calculation. The shape and the area of the shadow on the array was calculated and used in the determination of the global irradiance on the array. The PV blanket shape and structure dimensions were optimized to achieve a configuration which maximizes the specific power (W/kg). The optimization was performed for three types of PV blankets (silicon, gallium arsenide over germanium, and amorphous silicon) and two types of structural materials (carbon composite and arimid fiber composite). The results show that the catenary shape of the PV blanket corresponding to zero end angle at the base with respect to the horizontal results in the highest specific power. The tent angle is determined by optimizing the specific mass and the output power for maximum specific power. The combination of carbon fiber structural material and amorphous silicon blanket produces the highest specific power.

Colozza, Anthony J.↗

NASA NTRS2009

Amorphous Silk Fibroin Membranes for Separation of CO2

Amorphous silk fibroin has shown promise as a polymeric material derivable from natural sources for making membranes for use in removing CO2 from mixed-gas streams. For most applications of silk fibroin, for purposes other than gas separation, this material is used in its highly crystalline, nearly natural form because this form has uncommonly high tensile strength. However, the crystalline phase of silk fibroin is impermeable, making it necessary to convert the material to amorphous form to obtain the high permeability needed for gas separation. Accordingly, one aspect of the present development is a process for generating amorphous silk fibroin by treating native silk fibroin in an aqueous methanol/salt solution. The resulting material remains self-standing and can be prepared as thin film suitable for permeation testing. The permeability of this material by pure CO2 has been found to be highly improved, and its mixed-gas permeability has been found to exceed the mixed-gas permeabilities of several ultrahigh-CO2-permeable synthetic polymers. Only one of the synthetic polymers poly(trimethylsilylpropyne) [PTMSP] may be more highly permeable by CO2. PTMSP becomes unstable with time, whereas amorphous silk should not, although at the time of this reporting this has not been conclusively proven.

Aberg, Christopher M.↗

NASA NTRS2016

Mineralogy, Provenance, and Diagenesis of a Potassic Basaltic Sandstone on Mars: CheMin X-Ray Diffraction of the Windjana Sample (Kimberley Area, Gale Crater)

The Windjana drill sample, a sandstone of the Dillinger member (Kimberley formation, Gale Crater, Mars), was analyzed by CheMin X-ray diffraction (XRD) in the MSL Curiosity rover. From Rietveld refinements of its XRD pattern, Windjana contains the following: sanidine (21% weight, approximately Or(sub 95)); augite (20%); magnetite (12%); pigeonite; olivine; plagioclase; amorphous and smectitic material (approximately 25%); and percent levels of others including ilmenite, fluorapatite, and bassanite. From mass balance on the Alpha Proton X-ray Spectrometer (APXS) chemical analysis, the amorphous material is Fe rich with nearly no other cations-like ferrihydrite. The Windjana sample shows little alteration and was likely cemented by its magnetite and ferrihydrite. From ChemCam Laser-Induced Breakdown Spectrometer (LIBS) chemical analyses, Windjana is representative of the Dillinger and Mount Remarkable members of the Kimberley formation. LIBS data suggest that the Kimberley sediments include at least three chemical components. The most K-rich targets have 5.6% K2O, approximately 1.8 times that of Windjana, implying a sediment component with greater than 40% sanidine, e.g., a trachyte. A second component is rich in mafic minerals, with little feldspar (like a shergottite). A third component is richer in plagioclase and in Na2O, and is likely to be basaltic. The K-rich sediment component is consistent with APXS and ChemCam observations of K-rich rocks elsewhere in Gale Crater. The source of this sediment component was likely volcanic. The presence of sediment from many igneous sources, in concert with Curiosity's identifications of other igneous materials (e.g.,mugearite), implies that the northern rim of Gale Crater exposes a diverse igneous complex, at least as diverse as that found in similar-age terranes on Earth.

Treiman, Allan H.↗

NASA NTRS1990

Containerless processing of amorphous ceramics

The absence of gravity allows containerless processing of materials which could not otherwise be processed. High melting point, hard materials such as borides, nitrides, and refractory metals are usually brittle in their crystalline form. The absence of dislocations in amorphous materials frequently endows them with flexibility and toughness. Systematic studies of the properties of many amorphous materials have not been carried out. The requirements for their production is that they can be processed in a controlled way without container interaction. Containerless processing in microgravity could permit the control necessary to produce amorphous forms of hard materials.

Weber, J. K. Richard↗

DOE OSTI2025

Impact of amorphous pockets on displacement damage evolution in silicon

Silicon has long been known to exhibit amorphization in response to heavy particle bombardment. For doses below the total amorphization threshold, partial amorphization is observed in the form of scattered amorphous pockets. While extensive research has gone into modeling the formation and evolution of amorphous pockets in response to irradiation, no studies yet investigate their impact on the evolution of other damage such as interstitial supersaturation and clustering. In this study, we survey the impact of amorphous pockets on defect evolution in silicon when treated as static sinks. MD is first used to show that amorphous pockets provide energetically favorable sites for point defects relative to the crystalline bulk, supporting the hypothesis that they act as sinks. A 0-D cluster dynamics model is then constructed, taking an interstitial clustering model from the literature and including amorphous pockets as a sink species. We conduct our survey for temperatures between 30 and 400 °C and sink strengths between 1 to 6 x 10 10 cm −2 . Both implantation- and radiation-induced damage states are investigated using interstitial and vacancy concentrations as initial condition variables. We find that, due to the differing migration rates of the interstitial and the vacancy, amorphous pockets have a non-monotonic impact on the final damage state depending on the effective sink strength of the amorphous pockets, resulting in increased damage formation in regimes of intermediate amorphization. In conclusion, this result emphasizes the important role of amorphous pockets in governing the evolution of damage in partially amorphized crystalline materials.

36 MATERIALS SCIENCE↗