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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Pair distribution functions of amorphous organic thin films from synchrotron X-ray scattering in transmission mode

Using high-brilliance high-energy synchrotron X-ray radiation, for the first time the total scattering of a thin organic glass film deposited on a strongly scattering inorganic substrate has been measured in transmission mode. The organic thin film was composed of the weakly scattering pharmaceutical substance indomethacin in the amorphous state. The film was 130 µm thick atop a borosilicate glass substrate of equal thickness. The atomic pair distribution function derived from the thin-film measurement is in excellent agreement with that from bulk measurements. This ability to measure the total scattering of amorphous organic thin films in transmission will enable accurate in situ structural studies for a wide range of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Sputtered Aluminum Oxide and p+ Amorphous Silicon Back-Contact for Improved Hole Extraction in Polycrystalline CdSexTe1-x and CdTe Photovoltaics

A thin layer of Al 2 O 3 at the back of CdSe x T e1-x /CdTe devices is shown to passivate the back interface and drastically improve surface recombination lifetimes and photoluminescent response. Despite this, such devices do not show an improvement in open-circuit voltage (VOC.) Adding a p + amorphous silicon layer behind the Al 2 O 3 bends the conduction band upward, reducing the barrier to hole extraction and improving collection. Further optimization of the Al 2 O 3 , amorphous silicon (a-Si), and indium-doped tin oxide (ITO) layers, as well as their interaction with the CdCl 2 passivation process, are necessary to translate these electro-optical improvements into gains in voltage.

14 SOLAR ENERGY↗
DOE OSTI2017

Structural Basis for Metastability in Amorphous Calcium Barium Carbonate (ACBC)

Metastable amorphous precursors are emerging as valuable intermediates for the synthesis of materials with compositions and structures far from equilibrium. Recently, it was found that amorphous calcium barium carbonate (ACBC) can be converted into highly barium-substituted “balcite,” a metastable high temperature modification of calcite with exceptional hardness. A systematic analysis ACBC (Ca 1-x Ba x CO 3 ·1.2H 2 O) in the range from x = 0–0.5 is presented. Combining techniques that independently probe the local environment from the perspective of calcium, barium, and carbonate ions, with total X-ray scattering and a new molecular dynamics/density functional theory simulations approach, provides a holistic picture of ACBC structure as a function of composition. With increasing barium content, ACBC becomes more ordered at short and medium range, and increasingly similar to crystalline balcite, without developing long-range order. This is not accompanied by a change in the water content and does not carry a significant energy penalty, but is associated with differences in cation coordination resulting from changing carbonate anion orientation. Therefore, the local order imprinted in ACBC may increasingly lower the kinetic barrier to subsequent transformations as it becomes more pronounced. This pathway offers clues to the design of metastable materials by tuning coordination numbers in the amorphous solid state.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Amorphous and partially-amorphous metal coatings for corrosion resistance in molten chloride salt

In this study, amorphous metal coatings were developed to improve the corrosion resistance of structural alloys in molten salts for use as salt-facing materials in concentrating solar power (CSP) and molten salt reactor (MSR) applications. Three coatings were tested. One Fe-based, fully amorphous coating, and two Ni-based partially amorphous coatings. The candidate coatings were applied to samples made from Ni-based alloy 230, and exposed to KCl–MgCl 2 at 750 °C for 300 h in sealed Mo capsules. After exposure, uncoated alloy 230 samples were depleted in chromium near the surface, as measured by SEM-EDS. The attack had an average depth of 33 μm. Lastly, all three coatings performed well, showing no observable degradation during exposure, despite chromium contents between 20% and 40%. XRD and TEM measurements showed the coatings were fully crystallized after exposure, so the excellent corrosion resistance can likely be attributed to the recrystallized microstructure of the coatings.

14 SOLAR ENERGY↗
DOE OSTI2018

Metastable Intermediates in Amorphous Titanium Oxide: A Hidden Role Leading to Ultra-Stable Photoanode Protection

Metastable intermediates represent a non-equilibrium state of matter that may impose profound impacts to materials properties beyond our understandings of monolithic and equilibrium systems. Here, we report a discovery of hidden metastable intermediates in amorphous TiO 2 thin films and their critical role in electrochemical damage. These intermediates have a non-bulk crystal-like structure and exhibit significantly higher electrical conductivity than both the amorphous and the crystalline phases. When these TiO 2 films are applied to protect Si photoelectrochemical (PEC) photoanodes, the intermediates can induce localized high electrical currents that largely accelerate the etching of the TiO 2 film and the Si electrode underneath. The intermediates can be effectively suppressed by raising their nucleation barrier via reducing the film thickness from 24 to 2.5 nm. The homogeneous amorphous TiO 2 -film-coated Si photoanodes achieved more than 500 h of PEC water oxidation at a steady photocurrent density of over 30 mA·cm –2 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ab Initio Molecular Dynamics Simulations of Amorphous Calcium Carbonate: Interpretation of Pair Distribution Function and X-Ray Absorption Spectroscopy Data

The structure and transformation of hydrous amorphous calcium carbonate (ACC) are key to understanding biomineralization pathways and their relationship with the properties of the resulting material. Quantitative interpretation of scattering experiments aimed at elucidating the structure of ACC is challenging, due to the amorphous nature of this material, and, therefore, requires models for the structure and the scattering physics. Here, we generate physically realistic ensembles of hydrated ACC structures and their vibrational disorder from ab initio molecular dynamics (AIMD) simulations with an emphasis on enabling the consistent interpretation of the finer details of three complementary structural probes: neutron and x-ray pair distribution experiments and x-ray absorption spectroscopy (XAS). In each case, we simulate the signal directly in reciprocal space and then manipulate it into the real-space pair distribution function (PDF) or spectrum using the same procedures for the experimental and theoretical data. Good agreement with experiment was obtained across the three techniques with the simulations accounting well for all features in the spectra. Remaining small discrepancies pointed to differences between real samples and the idealized simulated systems such as deviations from the nominal CaCO3·nH2O stoichiometry. Additionally, the simulations offered a more accurate description of the local coordination environment of calcium than previous shell-by-shell fits to spectra of synthetic ACC and classical molecular dynamics simulations. This work demonstrates that AIMD is a powerful approach for extracting detailed structural information from neutron PDF, x-ray PDF, and XAS of amorphous carbonate phases.

Prange, Micah P.↗
DOE OSTI2021

Effect of Cd on the Nucleation and Transformation of Amorphous Calcium Carbonate

Qualitative measurements observations and field observations measurements indicate mineral coatings are one of the most abundant ways earth materials form, including in sedimentary deposits and certain biominerals. Formation of amorphous carbonates and other metastable intermediates in such these mixed cation systems is poorly understood, however. Using in situ PDF and SAXS, along with ICP-MS and SEM, results from this study 1) determines identify a novel short-range ordered Cd-ACC phase and 2) finds determine amorphous carbonate is stabilized by Cd2+, and 3) support formation of Cd-substituted vaterite, a polymorph of Ca that is not natively formed by Cd CO3. Results are highly dependent on ACC supersaturation, suggesting Cd-induced stability of Cd-ACC are is dependent primarily very sensitive on amorphous phase kinetics rather than thermodynamics to the rate of Cd-ACC nucleation and transformation. Findings provide a quantitative understanding of precursor intermediate phase structure and stability in mixed cation carbonate systems and aggregation that impact and suggest alternate pathways to forming the chemical heterogeneities frequently observed in natural mineral coatings.

Mergelsberg, Sebastian T.↗
DOE OSTI2021

Li + Diffusion in Amorphous and Crystalline Al 2 O 3 for Battery Electrode Coatings

Al 2 O 3 is often applied protectively to lithium-ion battery anode and cathode materials to inhibit surface degradation, suppress dendrite formation, and relieve mechanical stresses. Given the very high intrinsic band gap and diffusion barrier of the material, the mechanism that allows Li diffusion through these coatings is not well understood, and widely varying laboratory results indicate that there may be dependencies on morphology and stoichiometry. Using nudged elastic band calculations and ab initio molecular dynamics, we perform a systematic investigation across Al 2 O 3 structures, both crystalline and amorphous, and at various concentrations of Li + to uncover the optimal parameters for maximally diffusive coatings. We find a correlation between the low proximity of Li + to Al 3+ and the low Li + migration barrier. Although barriers are the lowest in the highly diffusive one-dimensional channels of crystalline θ-Al 2 O 3 , the system is structurally delicate and subject to detrimental distortion as the Li + content is increased. The α-Al 2 O 3 lattice is, conversely, highly stable against distortion at all Li + concentrations but disadvantageous for Li + migration. In amorphous systems, unscreened Li + –Li + Coulomb repulsion and pre-emptive occupation of “trapping sites” combine to lower the energy barriers as a function of increasing concentration. One of our most important findings is that Al-deficient materials can sharply increase Li + movement, and we predict that an amorphous material with a combination of high Li + concentration and Al deficiency would enable highly Li + -conductive protective coatings for electrodes.

25 ENERGY STORAGE↗
DOE OSTI2022

Intrinsic glassy-metallic transport in an amorphous coordination polymer

Conducting organic materials, such as doped organic polymers, molecular conductors and emerging coordination polymers4, underpin technologies ranging from displays to flexible electronics. Realizing high electrical conductivity in traditionally insulating organic materials necessitates tuning their electronic structure through chemical doping6. Furthermore, even organic materials that are intrinsically conductive, such as single-component molecular conductors, require crystallinity for metallic behavior. However, conducting polymers are often amorphous to aid durability and processability. Using molecular design to produce high conductivity in undoped amorphous materials would enable tunable and robust conductivity in many applications, but there are no intrinsically conducting organic materials that maintain high conductivity when disordered. Here we report an amorphous coordination polymer, Ni tetrathiafulvalene tetrathiolate, which displays markedly high electronic conductivity (up to 1,200 S cm –1 ) and intrinsic glassy-metallic behavior. Theory shows that these properties are enabled by molecular overlap that is robust to structural perturbations. This unusual set of features results in high conductivity that is stable to humid air for weeks, pH 0–14 and temperatures up to 140 °C. Furthermore, these findings demonstrate that molecular design can enable metallic conductivity even in heavily disordered materials, raising fundamental questions about how metallic transport can exist without periodic structure and indicating exciting new applications for these materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

First principles-based multiparadigm, multiscale strategy for simulating complex materials processes with applications to amorphous SiC films

Progress has recently been made in developing reactive force fields to describe chemical reactions in systems too large for quantum mechanical (QM) methods. In particular, ReaxFF, a force field with parameters that are obtained solely from fitting QM reaction data, has been used to predict structures and properties of many materials. Important applications require, however, determination of the final structures produced by such complex processes as chemical vapor deposition, atomic layer deposition, and formation of ceramic films by pyrolysis of polymers. This requires the force field to properly describe the formation of other products of the process, in addition to yielding the final structure of the material. We describe a strategy for accomplishing this and present an example of its use for forming amorphous SiC films that have a wide variety of applications. Extensive reactive molecular dynamics (MD) simulations have been carried out to simulate the pyrolysis of hydridopolycarbosilane. The reaction products all agree with the experimental data. After removing the reaction products, the system is cooled down to room temperature at which it produces amorphous SiC film, for which the computed radial distribution function, x-ray diffraction pattern, and the equation of state describing the three main SiC polytypes agree with the data and with the QM calculations. Extensive MD simulations have also been carried out to compute other structural properties, as well the effective diffusivities of light gases in the amorphous SiC film.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Pressure tunes electrical resistivity by four orders of magnitude in amorphous Ge[subscript 2]Sb[subscript 2]Te[subscript 5] phase-change memory alloy

Ge-Sb-Te-based phase-change memory is one of the most promising candidates to succeed the current flash memories. The application of phase-change materials for data storage and memory devices takes advantage of the fast phase transition (on the order of nanoseconds) and the large property contrasts (e.g., several orders of magnitude difference in electrical resistivity) between the amorphous and the crystalline states. Despite the importance of Ge-Sb-Te alloys and the intense research they have received, the possible phases in the temperature-pressure diagram, as well as the corresponding structure-property correlations, remain to be systematically explored. In this study, by subjecting the amorphous Ge{sub 2}Sb{sub 2}Te{sub 5} (a-GST) to hydrostatic-like pressure (P), the thermodynamic variable alternative to temperature, we are able to tune its electrical resistivity by several orders of magnitude, similar to the resistivity contrast corresponding to the usually investigated amorphous-to-crystalline (a-GST to rock-salt GST) transition used in current phase-change memories. In particular, the electrical resistivity drops precipitously in the P = 0 to 8 GPa regime. A prominent structural signature representing the underlying evolution in atomic arrangements and bonding in this pressure regime, as revealed by the ab initio molecular dynamics simulations, is the reduction of low-electron-density regions, which contributes to the narrowing of band gap and delocalization of trapped electrons. At P > 8 GPa, we have observed major changes of the average local structures (bond angle and coordination numbers), gradually transforming the a-GST into a high-density, metallic-like state. This high-pressure glass is characterized by local motifs that bear similarities to the body-centered-cubic GST (bcc-GST) it eventually crystallizes into at 28 GPa, and hence represents a bcc-type polyamorph of a-GST.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2017

Irradiation-driven amorphous-to-glassy transition in quartz: The crucial role of the medium-range order in crystallization

Noncrystalline solids can be classified into glassy and amorphous, wherein glasses and amorphous solids relax toward the supercooled liquid and crystalline states upon heating, respectively. However, the structural origin of such distinction remains unknown. Here in this study, based on molecular-dynamics simulations of irradiation-induced disordering of α-quartz, we demonstrate the existence of an amorphous-to-glassy transition. We show that the transition to the glassy state originates from the appearance of structural defects within the medium-range order of the atomic network. Such defects arise from the percolation of short-range defects and kinetically prevent crystallization. Overall, this suggests that the propensity of a disordered system for crystallization is controlled by the similarity between its medium-range order and that of the isochemical crystal.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Phase Transitions in Amorphous Germanium under Non-Hydrostatic Compression

As the pioneer semiconductor in transistor, germanium (Ge) has been widely applied in information technology for over half a century. Although many phase transitions in Ge have been reported, the complicated phenomena of the phase structures in amorphous Ge under extreme conditions are still not fully investigated. Here, we report the different routes of phase transition in amorphous Ge under different compression conditions utilizing diamond anvil cell (DAC) combined with synchrotron-based X-ray diffraction (XRD) and Raman spectroscopy techniques. Upon non-hydrostatic compression of amorphous Ge, we observed that shear stress facilitates a reversible pressure-induced phase transformation, in contrast to the pressure-quenchable structure under a hydrostatic compression. These findings afford better understanding of the structural behaviors of Ge under extreme conditions, which contributes to more potential applications in the semiconductor field.

Xu, Jianing (ORCID:0000000325474344)↗
DOE OSTI2014

Corrosion resistant amorphous metals and methods of forming corrosion resistant amorphous metals

A system for coating a surface comprises providing a source of amorphous metal, providing ceramic particles, and applying the amorphous metal and the ceramic particles to the surface by a spray. The coating comprises a composite material made of amorphous metal that contains one or more of the following elements in the specified range of composition: yttrium (.gtoreq.1 atomic %), chromium (14 to 18 atomic %), molybdenum (.gtoreq.7 atomic %), tungsten (.gtoreq.1 atomic %), boron (.ltoreq.5 atomic %), or carbon (.gtoreq.4 atomic %).

36 MATERIALS SCIENCE↗
DOE OSTI2012

Tuning the properties of Ge-quantum dots superlattices in amorphous silica matrix through deposition conditions

In this work, we investigate the structural properties of Ge quantum dot lattices in amorphous silica matrix, prepared by low-temperature magnetron sputtering deposition of (Ge+SiO{sub 2})/SiO{sub 2} multilayers. The dependence of quantum dot shape, size, separation, and arrangement type on the Ge-rich (Ge + SiO{sub 2}) layer thickness is studied. We show that the quantum dots are elongated along the growth direction, perpendicular to the multilayer surface. The size of the quantum dots and their separation along the growth direction can be tuned by changing the Ge-rich layer thickness. The average value of the quantum dots size along the lateral (in-plane) direction along with their lateral separation is not affected by the thickness of the Ge-rich layer. However, the thickness of the Ge-rich layer significantly affects the quantum dot ordering. In addition, we investigate the dependence of the multilayer average atomic composition and also the quantum dot crystalline quality on the deposition parameters.

36 MATERIALS SCIENCE↗