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At least 883 records · Page 49

Low-temperature domain-wall freezing and nonequilibrium dynamics in the transverse-field Ising model material CoNb 2 O 6

CoNb 2 O 6 is a rare realization of the transverse-field Ising model, making it a useful tool for studying both equilibrium and nonequilibrium many-body quantum physics. Despite a large body of work dedicated to characterizing this material, details of the ordered states in the presence of relatively weak transverse fields have not been discussed in detail. Here, we present a detailed study of CoNb 2 O 6 via ac susceptibility measurements in order to further characterize its low-temperature behavior in the presence of a transverse field. Specifically, we call attention to an unconventional freezing transition in zero field below T F = 1.2 K, occurring within the well-known commensurate antiferromagnetic (CAFM) state that onsets at T N2 = 1.9 K. We performed a series of transverse-field quenches into this frozen state, which resulted in a slowly relaxing susceptibility, χ' (t), that followed a logarithmic decay within the time range measured. Additionally, we discuss the frozen state in the context of the freezing of previously discussed “free” chains arising from domain walls between the four degenerate sublattices of the CAFM state. We also attempted to observe Kibble-Zurek scaling by quenching the transverse field into the frozen state at different rates. This produced a null result; the behavior can be fully explained by coarsening of domains over the time scale of the quenches. The absence of a clear Kibble-Zurek scaling is itself surprising, given the proposed ubiquity of the phenomenon for general second-order phase transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Deployment of Low Temperature Aluminum Dissolution (LTAD) Technology to Retrieve H-Modified (HM) Sludge in SRS Tank 15 – 25672

Tank 15 is a 4,234,000-liter (1,118,500-gallon) Type 2 high-level waste storage tank located in H Tank Farm at the Savannah River Site. It was put into service in 1960 to receive high-activity, H-Modified (HM) waste from H Canyon. Between June 1964 and November 1972, the waste tank was filled six times, and supernate was decanted five times, leaving behind the sludge solids. Tank 15 also received a mixture of high-activity and low-activity HM waste from Tank 16. Tank 15 has more recently undergone several mixing campaigns to remove much of the sludge waste; however, the effectiveness of suspending the sludge heel via mechanical mixing has significantly diminished. Low Temperature Aluminum Dissolution (LTAD) is a process developed for the dissolution of suspended aluminum solids in a large waste storage tank. Originally intended for deployment during the preparation of sludge batches in H Tank Farm for the Defense Waste Processing Facility (DWPF), the process involves maintaining the waste storage tank at a slightly elevated temperature and highly alkaline chemistry to facilitate dissolution of aluminum solids. As mechanical heel removal efforts diminished in effectiveness in Tank 15, LTAD was selected to both reduce the volume of sludge solids remaining in the heel and to modify the sludge rheology to facilitate the suspension of additional solids using the installed mixing devices.

Campbell, Seth G.↗

Cell model and elastic moduli of disordered solids - Low temperature limit

The cell theory has been previously employed to compute the equation of state of a disordered condensed system. It is now generalized to include anisotropic stresses. The condition of affine deformation is adopted, transforming an orginally spherical into an ellipsoidal cell. With a Lennard-Jones n-m potential between nonbonded centers, the formal expression for the deformational free energy is derived. It is to be evaluated in the limit of the linear elastic range. Since the bulk modulus in this limit is already known, it is convenient to consider a uniaxial deformation. To begin with, restrictions are made to the low-temperature limit in the absence of entropy contributions. Young's modulus and Poisson's ratio then follow.

Peng, S. T. J.↗

The superior hydrothermal stability of Pd/SSZ-39 in low temperature passive NOx adsorption (PNA) and methane combustion

We successfully synthesized uniform SSZ-39 with an average crystal size of about a micron. Pd (0.7 - 3 wt%) was supported on SSZ-39 with Si/Al ratio ~12. The as-synthesized materials were characterized by FTIR, XRD, Helium Ion Microscopy, HAADF-STEM imaging, 27 Al, 29 Si and H solid state NMR spectroscopic techniques. FTIR studies with CO and NO probe molecules reveal that the 0.7 wt% Pd/SSZ-39 material with Si/Al ~12 has the majority of Pd dispersed atomically as isolated Pd(II) and Pd(II)-OH centers, and thus can be used as a low-temperature passive NOx adsorber. Pd(II)-NO, Pd(II)(OH)(NO) and Pd(II)(CO)(NO) complexes form during PNA in this material. We compare this PNA material directly with the Pd/SSZ-13 system (with Si/Al ratio ~12) and show its superior hydrothermal stability. Remarkably, Pd/SSZ-39 with Si/Al ratio ~12 survives hydrothermal aging up to 815 ºC in 10% H 2 O/Air vapor for 16 hours without significant loss in activity. The SSZ-39 crystal structure remains intact during hydrothermal aging up to 1,000 ºC as we elucidate it with XRD and HAADF-STEM imaging/EDS mapping. However, changes to the framework during such harsh hydrothermal treatment significantly change the NOx release profiles during PNA as evidenced by high-field 27 Al NMR on fresh and aged Pd/SSZ-39 samples as well as PNA performance measurements. Besides PNA application, these hydrothermally very stable materials (3 wt% Pd on SSZ-39 with Si/Al ratio ~12) can be used as a robust methane combustion catalyst under industrially relevant conditions (GHSV~600,000hr -1 ). This catalyst shows minimal deactivation after both harsh hydrothermal aging at 750 and 800 ºC, and prolonged time on stream (105 hrs) at 425 °C. In contrast, both 3wt% Pd/alumina and 3wt% SSZ-13 supported samples lose a significant portion of their activity. Our study opens new avenues to prepare the most hydrothermally stable known Pd/zeolite materials with applications for adsorption and catalytic hydrocarbon combustion under industrially relevant conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gas Hydrate Stability at Low Temperatures and High Pressures with Applications to Mars and Europa

Gas hydrates are implicated in the geochemical evolution of both Mars and Europa [1- 3]. Most models developed for gas hydrate chemistry are based on the statistical thermodynamic model of van der Waals and Platteeuw [4] with subsequent modifications [5-8]. None of these models are, however, state-of-the-art with respect to gas hydrate/electrolyte interactions, which is particularly important for planetary applications where solution chemistry may be very different from terrestrial seawater. The objectives of this work were to add gas (carbon dioxide and methane) hydrate chemistries into an electrolyte model parameterized for low temperatures and high pressures (the FREZCHEM model) and use the model to examine controls on gas hydrate chemistries for Mars and Europa.

Marion, G. M.↗

Spatially resolved structural order in low-temperature liquid electrolyte

Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiP 6 ) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at -30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high–salt concentration domains of the liquid electrolyte from liquid phase separation at the low temperature. Molecular dynamics simulations suggest the SRO originates from the Li + - (PF 6 - ) n (n > 2) local structural order induced by high LiP 6 salt concentration.

42 ENGINEERING↗

Electrolyte Design for NMC811||SiO x -Gr Lithium-Ion Batteries with Excellent Low-Temperature and High-Rate Performance

The use of high-nickel NMC811 cathode and SiO x -Gr anode can greatly improve the overall energy densities of lithium-ion batteries. However, the unfavorable solid electrolyte interphase (SEI) layer generated from the decomposition of EC-based electrolytes lead to the poor cycling stability of NMC811||SiO x -Gr cells. Here we report an electrolyte design of 1.5 M LiPF 6 dissolved in FEC/MA/BN 2:2:6 by volume, which can form thin, robust, and homogeneous SEI layer to greatly improve the charge transfer at the electrode-electrolyte interface. Importantly, the designed electrolyte shows an outstanding low temperature performance that it can deliver a capacity of 123.3 mAh g –1 after 50 cycles at −20 °C with a current density of 0.5 C, overwhelming the standard EC-based electrolyte (1.2 M LiPF 6 EC/EMC 3:7 by volume) with a capacity of 35.7 mAh g –1 . The electrolyte also has a superior rate performance that it achieves a capacity of 122.5 mAh g −1 at a high current density of 10 C. Moreover, the LTE electrolyte holds the great potential of extreme fast-charging ability because of the large part of CC contribution in the CCCV charging model at high charging current densities.

Electrochemistry↗

Low Temperature Dynamic Polaron Liquid in a Manganite Exhibiting Colossal Magnetoresistance

Polarons - fermionic charge carriers bearing a strong companion lattice deformation - exhibit a natural tendency for self-localization due to the recursive interaction between electrons and the lattice. While polarons are ubiquitous in insulators, how they evolve in transitions to metallic and superconducting states in quantum materials remains an open question. Here, we use resonant inelastic x-ray scattering to track the electron-lattice coupling in the colossal magneto-resistive bi-layer manganite La 1.2 Sr 1.8 Mn 2 O 7 across its metal-to-insulator transition. The response in the insulating high-temperature state features harmonic emissions of a dispersionless oxygen phonon at small energy transfer. Additionally, upon cooling into the metallic state, we observe a drastic redistribution of spectral weight from the region of these harmonic emissions to a broad high energy continuum. In concert with theoretical calculations, we show that this evolution implies a shift in electron-lattice coupling from static to dynamic lattice distortions that leads to a distinct polaronic ground state in the low temperature metallic phase - a dynamic polaron liquid.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Heavy-Duty Low-Temperature and Diesel Combustion & Heavy-Duty Combustion Modeling (FY 2018 Annual Progress Report)

Regulatory drivers and market demands for lower pollutant emissions, lower carbon dioxide emissions, and lower fuel consumption motivate the development of clean and fuel-efficient engine operating strategies. Most current production engines use a combination of both in-cylinder and exhaust emission control strategies to achieve these goals. The emissions and efficiency performance of in-cylinder strategies depend strongly on flow and mixing processes associated with fuel injection. Both heavy- and light-duty engine/vehicle manufacturers use multiple-injection strategies to reduce noise, emissions, and fuel consumption. For both conventional and low-temperature diesel combustion, the state of knowledge and modeling tools for multiple injections are far less advanced than for single-injection strategies. Engine efficiency is limited to some degree by tradeoffs that must be accepted to meet particulate matter (including soot) emissions limits. Recent work on this project has filled some knowledge gaps on soot oxidation with multiple injections, and the current work for Fiscal Year (FY) 2018 addresses knowledge gaps on soot formation for multiple injections. While total in-cylinder soot is readily measured, discerning formation from oxidation is difficult. The FY 2018 experiments are designed to create in-cylinder conditions at the threshold of soot formation, where processes that affect soot formation can be more readily discerned. Soot formation pathways under such conditions are fraught with uncertainties, and soot models significantly overpredict polyaromatic hydrocarbon (PAH) and soot, so experimental data at these conditions will provide much needed data for improvements to PAH and soot models.

02 PETROLEUM↗

Chemistry of the CO dimer at low temperatures

Researchers conducted a series of experiments on the chlorine-catalyzed photodecomposition of O sub 3 both in the gas and in inert solvents such as CF sub 4 and CO sub 2 in the temperature range about 190 to 225 K. The liquid medium was chosen in order to minimize possible surface loss of long-lived ClO dimer, and to aid in the stabilization of transient excited intermediates. The mechanism of dimer formation was as follows: (1) Cl sub 2 + hv yields Cl + Cl; (2) Cl + O sub 3 yields ClO + O sub 2; (3) ClO + ClO yields Cl sub 2 O sub 2. The experiments were done in cooled low temperature cells, with irradiation from an Osram high pressure mercury arc, filtered to remove radiation below 325 nm. Spectral analysis was by means of a Cary Model 2200 UV spectrometer. The principal objectives were: (1) to determine the lifetime of the dimer as a function of temperature; (2) to observe spectral changes in the mixtures which could be attributed to dimer or related products; and (3) to observe chemical or photochemical reactions of the dimer.

Demore, W. B.↗

Ambient-Pressure Chemical Recycling of Thermoset Carbon Fiber-Reinforced Polymers via Low-Temperature Solvolysis: Techno-Economic and Life-Cycle Assessment

Carbon fiber-reinforced polymer (CFRP) waste is rapidly accumulating, with global volumes projected to exceed 500,000 tons annually by 2050. Virgin carbon fiber production is extremely energy- and cost-intensive, and growing demand has intensified supply-chain vulnerabilities associated with precursor availability and reliance on critical materials. Scalable recycling technologies therefore offer not only environmental benefits but also opportunities to reduce material costs and strengthen domestic composite supply chains. This study introduces an efficient, mild chemical recycling method for epoxy-amine CFRPs, utilizing acetic acid (80 wt%) and zinc acetate (1 wt%) at atmospheric pressure and low temperature (~110 °C). The solvolysis process preserves residual resin (~40%) on recycled carbon fibers (rCF), enhancing interfacial bonding in remanufactured composite materials. Recycled fibers retain ~90% of their mechanical properties, and recovered oligomers show potential for reuse in epoxy formulations, supporting material circularity. Techno-economic analysis (TEA) and life-cycle assessment (LCA) confirm the scalability and sustainability of this process.

Recycling CFRP↗

Low-temperature T -linear resistivity due to umklapp scattering from a critical mode

In this study, we consider the transport properties of a model of fermions scattered by a critical bosonic mode. The mode is overdamped and scattering is mainly in the forward direction. Such a mode appears at the quantum critical point for an electronic nematic phase transition and in gauge theories for a U(1) spin liquid. It leads to a short fermion lifetime, violating Landau's criterion for a Fermi liquid. In spite of this, transport can be described by a Boltzmann equation. We include momentum relaxation by umklapp scattering, supplemented by weak impurity scattering. We find that above a very low temperature which scales with Δ q 3 , where Δ q is the minimum umklapp scattering vector, the resistivity is linear in T with a coefficient which is independent of the amount of disorder. This picture holds until the temperature dependent part of the resistivity exceeds that due to impurity scattering. We compare the relaxation time approximation with an exact numerical solution of the Boltzmann equation. Surprisingly we find that, unlike the resistivity, the Hall coefficient strongly deviates from the relaxation time approximation and shows a strong reduction with increasing temperature. We comment on possible comparisons with experiments on high T c cuprates.

36 MATERIALS SCIENCE↗

Spatial variation of the low-temperature micro-photoluminescence of THM-grown CdZnTeSe

The quaternary compound CdZnTeSe (CZTS) has emerged as a next-generation detector material. Unlike CdZnTe (CZT), CZTS has the distinct advantages of little or no sub-grain boundary networks and a much lower concentration of Te inclusions, plus better compositional homogeneity. Thus, the material is expected to offer better spatial charge-transport homogeneity compared to CZT. However, an inhomogeneous distribution of point defects in both CZT and CZTS, such as Cd vacancies and residual impurities, can impose additional spatial inhomogeneity of the resistivity, carrier mobilities, and carrier lifetimes of the material. To investigate the spatial distribution of such defects in CZTS, low-temperature photoluminescence (PL) spectroscopic studies were performed at different positions along a single crystalline CZTS sample surface, which was grown by the traveling heater method (THM). In conclusion, the intensity variation of the PL emission of excitons bound to a neutral acceptor defect (A 0 , X), which is likely dominated by an acceptor like Cu-related level, with respect to the PL emission line from a neutral donor-bound exciton (D 0 , X) exhibited significant spatial variation, while the peak energy positions were approximately uniform due to the high compositional and bandgap homogeneity of the material.

II-VI semiconductor↗

Enabling Low-Temperature (LTP) Ignition Technologies for Multi-Mode Engines through the Development of a Validated High-Fidelity LTP Model for Predicative Simulations Tools

The goal of multi-mode engine architectures is to extend current lean-burn dilution limits with renewable fuels, which requires spark plugs to deposit high energies (hundreds of mJ) in order to initiate ignition and complete combustion. At elevated energy deposition rates, spark plugs experience increased electrode erosion and thermal losses, which ultimately shortens the spark-plug lifetime and lowers ignition efficiency. As such, in order to safeguard the efficiency gains of multi-mode concepts, new and improved ignition technologies are required. Recently, non-equilibrium low-temperature plasmas (LTP) have been shown to promote energy-efficient ignition via quenching and transport of electronically excited atoms and molecules, selective radical production and fast heating of hydrocarbon/air mixtures [1-2]. Thus, LTP is seen as a technology that can potentially improve the energy extraction efficiency of fuels, while enabling kinetically controlled combustion modes towards fuel leaner conditions to realize current DOE VTO goals of improving the sustainability of future mobility [3]. Although many previous studies have demonstrated the efficacy of plasma-assisted ignition to enhance combustion, the detailed enhancement mechanisms remain largely unknown, especially for oxygenated fuels and at elevated pressures that are most relevant to practical engine conditions. These barriers hinder the development of accurate and comprehensive numerical models that seek to describe LTP-based ignition in existing engine design software tools and methods. Current state-of-the-art simulation capabilities for LTP ignition systems are in need of improvements since they deliver qualitative results only due to important limitations of existing approaches. Firstly, validated kinetic models with elementary steps for plasma discharges in oxygenated fuel/air mixtures of relevance to the transportation sector are required. Such kinetic models do not exist at present and will be developed and validated within this project. Secondly, plasma discharges and reactive mixture ignition are multi-scale, unsteady processes requiring high-performance numerical methods and software that execute efficiently on DOE supercomputers. Such software does not exist at present and will be developed and applied to practical LTP ignition scenarios as part of this project. Thirdly, experimental databases that are tailored to serve as benchmark in support of the development of predictive computational models of LTP ignition do not exist and will be part of this project.

33 ADVANCED PROPULSION SYSTEMS↗

Indigenous Organic Matter Associated with Unusual Low Temperature Aqueous Secondary Phases in the Mars Meteorite Nakhla

The Martian meteorite Nakhla provides demonstrates evidence of mineral-water interactions that occurred in the Martian regolith within the last 1 Ga, as well as the presence of trace indigenous organic matter. The aim of our research is threefold: [1] provide a context in which to interpret alteration features; [2] determine the physical and chemical environment during alteration; and, [3] investigate the hypothesis that the formation of alteration phases was intimately involved in the accumulation and/or preservation of organic matter. In freshly fractured chips of the Mars meteorite Nakhla, we found carbonaceous matter intimately associated with secondary aqueous alteration phases interpreted to have formed through the low-temperature, mineral-water dissolution of the host Martian basalt. We have characterized the nature of carbonaceous matter and spatially associated secondary phases within Nakhla using a multidisciplinary suite of analytical instrumentation. The aim of our research is to provide a context to interpret the formation of secondary alteration assemblages within the Mars meteorite Nakhla and determine whether, and if so the extent to which, these phases participated in the accumulation and preservation of Martian organic matter.

Mars meteorite↗

The XRS Low Temperature Cryogenic System: Ground Performance Test Results

The X-Ray Spectrometer (XRS) instrument is part of the Astro-E mission scheduled to launch early in 2000. Its cryogenic system is required to cool a 32-element square array of x-ray microcalorimeters to 60-65 mK over a mission lifetime of at least 2 years. This is accomplished using an adiabatic demagnetization refrigerator (ADR) contained within a two-stage superfluid helium/solid neon cooler. Goddard Space Flight Center is providing the ADR and helium dewar. The flight system was assembled in Sept. 1997 and subjected to extensive thermal performance tests. This paper presents test results at both the system and component levels. In addition, results of the low temperature topoff performed in Japan with the engineering unit neon and helium dewars are discussed.

Breon, Susan↗

Composite Materials for Low-Temperature Applications

Composite materials with improved thermal conductivity and good mechanical strength properties should allow for the design and construction of more thermally efficient components (such as pipes and valves) for use in fluid-processing systems. These materials should have wide application in any number of systems, including ground support equipment (GSE), lunar systems, and flight hardware that need reduced heat transfer. Researchers from the Polymer Science and Technology Laboratory and the Cryogenics Laboratory at Kennedy Space Center were able to develop a new series of composite materials that can meet NASA's needs for lightweight materials/composites for use in fluid systems and also expand the plastic-additive markets. With respect to thermal conductivity and physical properties, these materials are excellent alternatives to prior composite materials and can be used in the aerospace, automotive, military, electronics, food-packaging, and textile markets. One specific application of the polymeric composition is for use in tanks, pipes, valves, structural supports, and components for hot or cold fluid-processing systems where heat flow through materials is a problem to be avoided. These materials can also substitute for metals in cryogenic and other low-temperature applications. These organic/inorganic polymeric composite materials were invented with significant reduction in heat transfer properties. Decreases of 20 to 50 percent in thermal conductivity versus that of the unmodified polymer matrix were measured. These novel composite materials also maintain mechanical properties of the unmodified polymer matrix. These composite materials consist of an inorganic additive combined with a thermoplastic polymer material. The intrinsic, low thermal conductivity of the additive is imparted into the thermoplastic, resulting in a significant reduction in heat transfer over that of the base polymer itself, yet maintaining most of the polymer's original properties. Normal polymer processing techniques can turn these composite materials into unique, custom parts for ground support, Shuttle, and Constellation needs. We fabricated test specimens of the composite and base materials for thermal and mechanical characterization and found that the strength of the composite material at nominal-percentage loading remained relatively unchanged from the base material.

Source record↗

Oxidation of NiCr and NiCrMo Alloys at Low Temperatures

Oxidation of Ni-Cr and Ni-Cr-Mo was studied in operando with near ambient pressure x-ray photoelectron spectroscopy in the Cabrera-Mott regime. The oxidation temperature was 200 °C - a severely diffusion limited regime. The near-surface alloy is Cr-enriched after reduction of natives oxide in vacuum, and especially so for Ni-15Cr-6Mo. Mo-cations are integrated in the oxide and Mo(VI) dominates at the surface. The surface chemistry driven promotion of chromia by Mo predicted by theory is negated by the limited surface diffusion of reactants. Furthermore, pre-oxidation processing is proposed to control the oxide properties for use of Ni-Cr superalloys at low temperatures.

36 MATERIALS SCIENCE↗