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At least 37 records · Page 2

Explainable machine learning reveals that local structural motifs encode the thermodynamic state across the CuZr metallic glass-forming range

Metallic glasses derive their properties from the statistics of local atomic motifs rather than from long-range order, yet a quantitative, chemistry-specific link between motif populations and the underlying glassy state has remained elusive. In this work we combine large-scale molecular dynamics, Voronoi tessellation, deep neural networks, and SHapley Additive exPlanations (SHAP) to identify which local structural motifs define the glassy state of Cu—Zr metallic glasses. A dataset of 17,180 atomistic configurations spanning ten compositions (Cu 20 Zr 80 –Cu 80 Zr 20 ) and four quench rates (10 9 –10 12 K/s) is used to train a feed-forward neural network that regresses temperature across the 50–2000 K liquid–supercooled–glass range, achieving a mean absolute error of 19.89 K and R 2 = 0.9974, confirming that the local structural state is faithfully encoded in motif-level structure. SHAP analysis then reveals that a tightly coupled near-icosahedral family of motifs (coordination numbers (CN) 11–13, including the full icosahedron 001200 and its single-atom-perturbation sibling 10930) collectively encodes the thermodynamic state of the system across the full glass-forming range. The CN = 11–13 ordered members carry negative SHAP values at high populations, tracking the most deeply-quenched configurations, while 10930 shows the reversed signature consistent with its role as a soft-spot host whose population shrinks as the icosahedral network deepens. The analysis demonstrates that explainable machine learning can isolate the minimal motif vocabulary defining the glassy state and recovers the near-icosahedral building blocks previously identified by data-driven analyses of Cu—Zr. The approach provides a general, chemistry-specific route for characterizing the structural state of disordered materials.

36 MATERIALS SCIENCE↗

Lightweight, Self-Deployable Wheels

Ultra-lightweight, self-deployable wheels made of polymer foams have been demonstrated. These wheels are an addition to the roster of cold hibernated elastic memory (CHEM) structural applications. Intended originally for use on nanorovers (very small planetary-exploration robotic vehicles), CHEM wheels could also be used for many commercial applications, such as in toys. The CHEM concept was reported in "Cold Hibernated Elastic Memory (CHEM) Expandable Structures" (NPO-20394), NASA Tech Briefs, Vol. 23, No. 2 (February 1999), page 56. To recapitulate: A CHEM structure is fabricated from a shape-memory polymer (SMP) foam. The structure is compressed to a very small volume while in its rubbery state above its glass-transition temperature (Tg). Once compressed, the structure can be cooled below Tg to its glassy state. As long as the temperature remains <Tg the structure remains compacted (in a cold hibernated state), even when the external compressive forces are removed. When the structure is subsequently heated above Tg, it returns to the rubbery state, in which a combination of elasticity and the SMP effect cause it to expand (deploy) to its original size and shape. Once thus deployed, the CHEM structure can be rigidified by cooling below Tg to the glassy state. The structure could be subsequently reheated above Tg and recompacted. The compaction/deployment/rigidification cycle could be repeated as many times as needed.

Chmielewski, Artur↗

Lightweight, Self-Deploying Foam Antenna Structures

Lightweight, deployable antennas for a variety of outer-space and terrestrial applications would be designed and fabricated according to the concept of cold hibernated elastic memory (CHEM) structures, according to a proposal. Mechanically deployable antennas now in use are heavy, complex, and unreliable, and they utilize packaging volume inefficiently. The proposed CHEM antenna structures would be simple and would deploy themselves without need for any mechanisms and, therefore, would be more reliable. The proposed CHEM antenna structures would also weigh less, could be packaged in smaller volumes, and would cost less, relative to mechanically deployable antennas. The CHEM concept was described in two prior NASA Tech Briefs articles: "Cold Hibernated Elastic Memory (CHEM) Expandable Structures" (NPO-20394), Vol. 23, No. 2 (February 1999), page 56; and "Solar Heating for Deployment of Foam Structures" (NPO-20961), Vol. 25, No. 10 (October 2001), page 36. To recapitulate from the cited prior articles: The CHEM concept is one of utilizing opencell foams of shape-memory polymers (SMPs) to make lightweight, reliable, simple, and inexpensive structures that can be alternately (1) compressed and stowed compactly or (2) expanded, then rigidified for use. A CHEM structure is fabricated at full size from a block of SMP foam in its glassy state [at a temperature below the glass-transition temperature (Tg) of the SMP]. The structure is heated to the rubbery state of the SMP (that is, to a temperature above Tg) and compacted to a small volume. After compaction, the structure is cooled to the glassy state of the SMP. The compacting force can then be released and the structure remains compact as long as the temperature is kept below Tg. Upon subsequent heating of the structure above Tg, the simultaneous elastic recovery of the foam and its shape-memory effect cause the structure to expand to its original size and shape. Once thus deployed, the structure can be rigidified by cooling below Tg. Once deployed and rigidified, the structure could be heated and recompacted. In principle, there should be no limit on the achievable number of compaction/deployment/ rigidification cycles. Thus far, several different designs of a 3.5-m-long CHEM conical corrugated horn antenna have been analyzed (see figure). A small CHEM structural antenna model was fabricated and a thin, electrically conductive layer of aluminum was deposited on the inner surface of the model. This structural model was then subjected to the compaction and deployment treatments described above to demonstrate the feasibility of a CHEM corrugated horn antenna.

Sokolowski, Witold↗

Morphological evolution and transition at nanoscale in BSTO ceramic materials

Considerable efforts have been devoted for the development of low cost ferroelectric and clean energy storage multifunctional materials. Modification in design and production of a low cost material with well proven process provides pathway for high energy density dielectric energy storage. We studied fluorine doped a commercially well-established material system barium strontium titanate with two different concentrations of dopants and studied the morphological transition and its effect on properties. It was observed that sample with higher concentration transitioned much faster into glassy state, followed by growth of fibers which turned into a self-arranged bird nest type shape. The sample with lower concentration changed slowly into glassy state and only few fibers were farmed. Dielectric was highly dependent on processing methods and shows variation with crystallinity of material, temperature and cooling conditions during processing. In the higher concentration range, we observed nano-scale interface breakdown very similar to that of solid-liquid interface breakdown during crystal growth.

dielectric↗

Lubricant rheology applied to elastohydrodynamic lubrication

Viscosity measurements in a high pressure rheometer, elastohydrodynamic simulator studies (including the development of a temperature measuring technique), and analytical fluid modeling for elastohydrodynamic contacts are described. The more recent research which is described concerns infrared temperature measurements in elastohydrodynamic contacts and the exploration of the glassy state of lubricants. A correlation, of engineering significance, was made between transient surface temperature measurements and surface roughness profiles. Measurements of glass transitions of lubricants and the study of the effect of rate processes on materials lead to the conclusion that typical lubricants go into the glassy state as they pass through the contact region of typical elastohydrodynamic contacts.

Winer, W. O.↗

Intermolecular correlations of liquid and glassy CS 2 studied by synchrotron radiation x-ray diffraction

How is the orientation of molecular liquids ordered on cooling? What are the basic structures of molecular glasses, e.g., close to the crystalline structure or some special structures such as icosahedral cluster? These are long-standing questions in liquid and glass physics. Here, we have constructed a novel cryostat to prepare simple molecular glasses by vapor deposition and performed in situ synchrotron radiation x-ray diffraction experiments. The glassy state of a simple molecule CS 2 , which cannot be vitrified by normal liquid quenching, was successfully prepared with this instrument, and its diffraction data were collected in a wide Q-range of 0.16–25.7 Å -1 with a high-energy diffractometer at BL04B2, SPring-8. The diffraction data of liquid CS 2 were also recorded in a wide temperature range of 160–300 K. These diffraction data were analyzed with molecular dynamics simulations and reverse Monte Carlo modelings to investigate orientational correlation. From the obtained 3D structure models, the orientational correlation between neighboring CS 2 molecules was investigated quantitatively as a function of temperature. At room temperature, the parallel and T-shaped arrangements are preferred for the nearest neighbor correlation. On cooling, these arrangements are developed gradually, and its rate became prominent below the melting temperature (162 K). In the glassy state, the slipped-parallel arrangement is dominant as well as the T-shaped arrangement. Both arrangements appear in the CS 2 crystal, indicating that the structure of glassy CS 2 is close to that of crystalline CS 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermal processing of omicron-terphenyl - A Raman study

Raman spectra from omicron-terphenyl sealed in glass capillary tubes were acquired over temperatures ranging from 233 to 343 K. Over this temperature range, omicron-terphenyl can exist in the solid-crystalline, molten, supercooled-liquid, and amorphous-glassy states. Representative structure-sensitive spectra are presented along with a qualitative description. The lattice spectral feature occurring at a Raman shift of 123/cm displays abrupt changes in profile and intensity as melting and glass transition occur. The intensity ratio of the C-C stretching 996/cm line and C-H stretching line at 1008/cm displays a change related to the transformation of the ordered-crystalline phase to the disordered-liquid or glassy state. At a Raman shift of 1162/cm the solid-crystalline state shows a splitting due to the effect of the crystal field. The possibility of using these structure-sensitive Raman characteristics for in situ diagnostics during materials processing is discussed.

Biswas, A.↗

Glassy correlated state induced by disorder in the frustrated antiferromagnet Tb 2 Zr 2 O 7

Here, we study the low-temperature thermomagnetic properties of the polycrystalline material Tb 2 Zr 2 O 7 through ac susceptibility and specific heat measurements. This zirconate displays a defect-fluorite structure in which the magnetic Tb 3+ and nonmagnetic Zr 4+ cations sit randomly on the same metal sublattice. No long-range magnetic order is found down to 100 mK, although dominant antiferromagnetic interactions are observed and the spins remain dynamic down to the lowest temperatures investigated. We observed a frequency-dependent peak around 2.5 K which is well described by many models of a canonical spin-glass transition. In-field specific heat measurements and the recovered entropy of the system R ln(4) suggest a two doublets ground state separated by 7 K. Comparisons to the pyrochlores Tb 2 Ti 2 O 7 and Tb 2 Hf 2 O 7 reinforce the collective spin-glass-type behavior and the opening for discussions of an exotic Coulomb phase in this material.

36 MATERIALS SCIENCE↗

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.

tropopause↗

Electronic glasses from a broken gauge symmetry in disorder-free systems

Glass phases can be stabilized by quenched disorders, as in most spin-glass materials, or self-generated through kinetic freezing in disorder-free systems. A canonical example of the latter is structural glasses, which have been extensively studied for many decades. Yet, how the rugged energy landscape of a glass phase is spontaneously generated in disorder-free systems remains one of the key questions in glass physics. Here, in this work, we present a general electronic mechanism for the emergence of glassy phase using the example of itinerant electrons coupled to XY spins on a lattice. This model can also be viewed as the mean-field theory of a superconducting system with attractive density-density interactions. Intriguingly, the electron gauge symmetry in the strong pairing limit gives rise to a macroscopic degeneracy of XY spins. In the presence of electron hopping that breaks the gauge symmetry, the lifting of the extensive degeneracy leads to a glass phase with disordered pairings. Our findings highlight a scenario in which a glassy state originates from the breaking of quantum gauge symmetry without quenched disorders.

XY model↗

Non-Equilibrium relaxation, aging scaling, and critical depinning dynamics of skyrmions in disordered magnetic films. Final Report

Technical applications of type-II superconductors, especially high-Tc compounds, in external magnetic fields require an effective flux pinning mechanism to reduce Ohmic losses due to flux creep and flow. Naturally abundant point defects, dislocations, and twin boundaries as well as artificially introduced disorder may serve as effective pinning centers for magnetic vortices. The properties of interacting flux lines subject to strong thermal fluctuations and point-like or extended pinning centers have therefore been a major research focus in condensed matter physics, and considerable progress has been achieved in the characterization and mathematical description of the equilibrium phases and non-equilibrium steady states of vortex matter. Detailed studies of the rich phase diagrams that reveal novel glassy states as well as the associated complex dynamical phenomena have in turn enriched the theoretical understanding of condensed matter systems, elucidating specifically the kinetics of elastic objects driven through disordered media and the important role of topological defects such as vortices and dislocations in various materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Operando Optical Microscopy for Visualization of Dendrite Growth in an Argyrodite LPSCl–Polymer Composite Electrolyte

Herein, we demonstrate the utility of optical microscopy as an accessible technique for the in situ visualization of dendrite growth within polymer–sulfide composite solid-state electrolytes. The composite electrolyte features in situ polymerization and cross-linking of the polymer between ceramic particles, which opens up extensive opportunities for accelerated materials discovery, given the vast array of acrylate/methacrylate monomers available. Specifically, the cross-linked polymer poly(triethylene glycol dimethacrylate) (poly(TEGDMA)) was observed to effectively fill pores and inhibit dendrite growth at the lithium metal interface, attributed to its glassy state at room temperature. This work represents the first application of optical microscopy to illustrate that the incorporation of glassy, undoped polymers such as poly(TEGDMA) can serve as a viable strategy for dendrite suppression in solid-state composite electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Flow behavior of droplet chondrules in the Manych /L-3/ chondrite

The Manych (L-3) chondrite contains chondrules that have radically different thermal histories. The high-SiO2 composition cooled at about 1 K/min to a glassy state or more slowly to form a variety of fractions of crystals. The low-SiO2 composition cooled at about 3000 K/min to form a glassy coating or much more slowly to form microporphyry. The extreme range of cooling rates displayed by objects in the Manych chondrite is difficult to reconcile with a model involving droplet condensation at low pressure which provides a uniform temperature, a uniform cooling rate, and an ambient that is not necessarily cold. The experimental results presented here are interpreted to mean that the origin of the chondrules is likely a result of impact melting because of the range of cooling histories represented in the chondrite.

Klein, L. C.↗

Computational investigation of water glasses using machine-learning potentials

The molecular origins of water’s anomalous properties have long been a subject of scientific inquiry. The liquid–liquid phase transition hypothesis, which posits the existence of distinct low-density and high-density liquid states separated by a first-order phase transition terminating at a critical point, has gained increasing experimental and computational support and offers a thermodynamically consistent framework for many of water’s anomalies. However, experimental challenges in avoiding crystallization near the postulated liquid–liquid critical point have focused attention to water’s canonical glassy states: low-density and high-density amorphous ice. Here, we use two Deep Potential machine-learning models, trained on the Strongly Constrained and Appropriately Normed density functional and the highly accurate Many-Body Polarizable potential, to conduct an investigation of water’s glassy phenomenology based on quantum mechanical calculations. Despite not being explicitly trained on amorphous ices, both models accurately capture the structure and transformation of the water glasses, including their interconversion along different thermodynamic paths. Isobaric quenching of liquid water at various pressures generates a continuum of intermediate amorphous ices and density fluctuations increase near the liquid–liquid critical pressure. The glass transition temperatures of the amorphous ices produced at different pressures exhibit two distinct branches, corresponding to low-density and high-density amorphous ice behaviors, consistent with experiment and the liquid–liquid transition hypothesis. Extrapolating transformation pressures from isothermal compressions to experimental compression rates brings our simulations into excellent agreement with data. Our findings demonstrate that machine-learning potentials trained on equilibrium phases can effectively model nonequilibrium glassy behavior and pave the way for studying long-timescale, out-of-equilibrium processes with quantum mechanical accuracy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Defect-induced formation and frustration-driven multiple magnetic transitions in Gd 2 Co 0.90 Si 2.90

A new ternary compound, Gd 2 Co 0.90 Si 2.90 , has been synthesized in a chemically single phase by deliberately introducing lattice vacancies in the Co and Si sites. The system is characterized by DC magnetization, heat capacity, resistivity and density functional theory (DFT) calculations. Here, a detailed experimental study reveals that the system exhibits an antiferromagnetic transition below T N = 11.3 K followed by spin freezing behaviour below T B ~ 4.8 K. An additional high-temperature magnetic transition could also be detected at T H ~ 150 K, which is short range in character and is associated with defect-induced polarization of the conduction electrons. The spin-glass-like state formation in the system is additionally bolstered by the observation of magnetic relaxation and associated aging phenomena as well as the magnetic memory effect. On the basis of non-equilibrium dynamical behaviour, we argue that the glassy state in this compound favours the hierarchical model over the droplet model. DFT calculations and experimental outcomes establish that the ground state is magnetically frustrated due to the small energy difference between distinct spin configurations having closely spaced ground-state energies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Joining and Assembly of Bulk Metallic Glass Composites Through Capacitive Discharge

Bulk metallic glasses (BMGs), a class of amorphous metals defined as having a thickness greater than 1 mm, are being broadly investigated by NASA for use in spacecraft hardware. Their unique properties, attained from their non-crystalline structure, motivate several game-changing aerospace applications. BMGs have low melting temperatures so they can be cheaply and repeatedly cast into complex net shapes, such as mirrors or electronic casings. They are extremely strong and wear-resistant, which motivates their use in gears and bearings. Amorphous metal coatings are hard, corrosion-resistant, and have high reflectivity. BMG composites, reinforced with soft second phases, can be fabricated into energy-absorbing cellular panels for orbital debris shielding. One limitation of BMG materials is their inability to be welded, bonded, brazed, or fastened in a convenient method to form larger structures. Cellular structures (which can be classified as trusses, foams, honeycombs, egg boxes, etc.) are useful for many NASA, commercial, and military aerospace applications, including low-density paneling and shields. Although conventional cellular structures exhibit high specific strength, their porous structures make them challenging to fabricate. In particular, metal cellular structures are extremely difficult to fabricate due to their high processing temperatures. Aluminum honeycomb sandwich panels, for example, are used widely as spacecraft shields due to their low density and ease of fabrication, but suffer from low strength. A desirable metal cellular structure is one with high strength, combined with low density and simple fabrication. The thermoplastic joining process described here allows for the fabrication of monolithic BMG truss-like structures that are 90% porous and have no heat-affected zone, weld, bond, or braze. This is accomplished by welding the nodes of stacked BMG composite panels using a localized capacitor discharge, forming a single monolithic structure. This removes many complicated and costly fabrication steps. Moreover, the cellular structures detailed in this work are among the highest- strength and most energy-absorbent materials known. This implies that a fabricated structure made from these materials would have unequaled mechanical properties compared to other metal foams or trusses. The process works by taking advantage of the electrical properties of the matrix material in the metal-matrix composite, which in this case is a metallic glass. Due to the random nanoscale arrangement of atoms (without any grain boundaries), the matrix glass exhibits a near-constant electrical resistivity as a function of temperature. By placing the composite panels between two copper electrode plates and discharging a capacitor, the entire matrix of the panel can be heated to approximately 700 C in 10 milliseconds, which is above the alloy s solidus but below the liquidus. By designing the geometry of the panels into the shape of an egg box, the electrical discharge localizes only in the tips of each pyramidal cell. By applying a forging load during discharge, the nodes of the panels can be fused together into a single piece, which then dissipates heat through radiation back into a glassy state. This means that two panels can be metallurgically fused into one panel with no heat-affected zone, creating a seamless connection between panels. During the process, the soft metal particles (dendrites) that are uniformly distributed in the glassy matrix to increase the toughness are completely unaffected by the thermoplastic joining. The novelty is that a truss (or foam-like) structure can be formed with excellent energy- absorbing capabilities without the need for machining. The technique allows for large-scale fabrication of panels, well-suited for spacecraft shields or military vehicle door panels. Crystalline metal cellular structures cannot be fabricated using the thermoplastic joining technique described here. If metal panels were te assembled into a cellular structure, they would either have to be welded, brazed, bonded, or fastened together, creating a weak spot in the structure at each connection. Welded parts require a welding material to be added to the joint and exhibit a soft and weak heat-affected zone. Brazing and bonding do not form a metallurgical joint and thus exhibit low strengths, especially when the panels are pulled apart and fasteners require high-stress-concentration holes to be drilled. No equivalent rapid heating method exists for assembling metal panels together into cellular structures, and thus, those parts must be foamed, machined, or investment cast if they are to form a monolithic structure. If the crystalline panels were to be joined using capacitive discharge, as with a spot welder, their bond would be very weak, and the panels would have to be extremely thin. In contrast, the strength of joined BMG parts has been demonstrated to have strength comparable to the parent material. This technique opens up the possibility of using large-scale BMG hardware in spacecraft, military, or commercial applications.

Hofmann, Douglas C.↗

A Liquid-Liquid Transition in an Undercooled Ti-Zr-Ni Liquid

If crystallization can be avoided, liquids enter a metastable (undercooled) state below their equilibrium liquidus temperatures, TI, finally freezing into a glass below a characteristic temperature called the glass transition temperature, T,. In rare cases, the undercooled liquid may undergo a liquid-liquid phase transition (liquid polymorphism) before entering the glassy state. This has been suggested from experimental studies of HzO and Si4. Such phase transitions have been predicted in some stable liquids, i.e. above TI at atmospheric pressure, for Si02 and BeF;, but these have not been verified experimentally. They have been observed in liquids of P7, Sis and C9, but only under high pressure. All of these transitions are driven by an anomalous density change, i.e. change in local structure, with temperature or pressure. In this letter we present the first experimental evidence for a phase transition in a low viscosity liquid that is not driven by an anomalous density change, but by an approach to a constant configuration state. A maximum in the specific heat at constant pressure, similar to what is normally observed near T,, is reported here for undercooled low viscosity liquids of quasicrystal- forming Ti-Zr-Ni alloys. that includes cooperativity, by incorporating a temperature dependent excitation energy fits the data well, signaling a phase transition.

Lee, G. W.↗

A Novel Liquid-Liquid Transition in Undercooled Ti-Zr-Ni Liquids

If crystallization can be avoided, liquids enter a metastable (undercooled) state below their equilibrium liquidus temperatures, T(sub l), finally 'freezing' into a glass below a characteristic temperature called the glass transition temperature, T(sub g). In rare cases, the undercooled liquid may undergo a liquid-liquid phase transition (liquid polymorphism) before entering the glassy state. This has been suggested from experimental studies of H2O and Si. Such phase transitions have been predicted in some stable liquids, ie. above T(sub l) at atmospheric pressure, for SiO2 and BeF2, but these have not been verified experimentally. They have been observed in liquids of P, Si and C, but only under high pressure. In this letter we present the first experimental evidence for a phase transition in a low viscosity metallic liquid that is driven by an approach to a constant entropy configuration state and correlated with a growing icosahedral order in the liquid. A maximum in the specific heat at constant pressure, similar to what is normally observed near T(sub g), is reported for undercooled liquids of quasicrystal-forming Ti-Zr-Ni alloys. A two-state excitation model that includes cooperativity by incorporating a temperature-dependent excitation energy, fits the specific heat data well, signaling a phase transition. An inflection in the liquid density with decreasing temperature instead of a discontinuity indicates that this is not a typical first order phase transition; it could be a weakly first order or higher order transition. While showing many similarities to a glass transition, this liquid-liquid phase transition occurs in a mobile liquid, making it novel.

Lee, G. W.↗