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At least 703 records · Page 39

Solid-state platform for cooperative quantum dynamics driven by correlated emission

While traditionally regarded as an obstacle to quantum coherence, recent breakthroughs in quantum optics have shown that the dissipative interaction of a qubit with its environment can be leveraged to protect quantum states and synthesize many-body entanglement. Inspired by this progress, here we set the stage for the—as yet uncharted—exploration of analogous cooperative phenomena in hybrid solid-state platforms. We develop a comprehensive formalism for the quantum many-body dynamics of an ensemble of solid-state spin defects interacting with the magnetic field fluctuations of a common solid-state reservoir. Our framework applies to any solid-state reservoir whose fluctuating spin, pseudospin, or charge degrees of freedom generate magnetic fields. To understand whether correlations induced by dissipative processes can play a relevant role in a realistic experimental setup, we apply our model to a qubit array interacting via the spin fluctuations of a ferromagnetic bath. Our results show that the low-temperature collective relaxation rates of the qubit ensemble can display clear signatures of super- and subradiance, i.e., forms of cooperative dynamics traditionally achieved in atomic ensembles. We find that the solid-state analog of these cooperative phenomena is robust against spatial disorder in the qubit ensemble and thermal fluctuations of the magnetic reservoir, providing a route for their feasibility in near-term experiments. Finally, our work lays the foundation for a multiqubit approach to quantum sensing of solid-state systems and the direct generation of many-body entanglement in spin-defect ensembles. Furthermore, we discuss how the tunability of solid-state reservoirs opens up novel pathways for exploring cooperative phenomena in regimes beyond the reach of conventional quantum optics setups.

NV centers↗

Dynamics of rapidly depressurized multiphase shock tubes

Rapid depressurization is a fluid phenomenon that occurs in many industrial and natural applications. Its behaviour is often complicated by the formation, propagation and interaction of waves. In this work, we perform computer simulations of the rapid depressurization of a gas–solid mixture in a shock tube. Our problem set-up mimics previously performed experiments, which have been historically used as a laboratory surrogate for volcanic eruptions. The simulations are carried out with a discontinuous Galerkin compressible fluid solver with four-way coupled Lagrangian particle tracking capabilities. The results give an unprecedented look into the complex multiphase physics at work in this problem. Different regimes have been characterized in a regime map that highlights the key observations. While the mean flow behaviour is in good agreement with experiments, the simulations show unexpected accelerations of the particle front as it expands. Additionally, a new lifting mechanism for gas bubble (void) growth inside the gas–solid mixture is detailed.

Mechanics↗

Effects of Fe concentration on helium bubble formation in NiFe x single-phase concentrated solid solution alloys

The formation of helium bubbles and the consequential property degradation are critical challenges for materials used in advanced nuclear energy systems. The mechanism of helium bubble formation in a series of NiFe x (x = 0, 20, 35, or 50 at.%) single-phase concentrated solid solution alloys (SP-CSAs) are studied in this work. Transmission electron microscopy analysis shows that with increasing Fe concentration, the average bubble size decreases while the bubble number density increases, indicating the growth of large helium bubbles in NiFe x SP-CSAs is suppressed by increasing the alloy chemical complexity through increased Fe concentration. Mechanisms for the slower bubble growth rate in NiFe x binary SP-CSAs compared Ni are identified. These mechanisms include promotion of Frenkel pair recombination, denser and more homogeneously distributed nucleation sites, and increased helium atom densities inside the bubbles. Here, the results demonstrate that optimizing the chemical complexity in SP-CSAs can be an effective approach to design materials with superior resistance to helium bubble nucleation and growth.

36 MATERIALS SCIENCE↗

Analysis of Technology for Solid State Coherent Lidar

Over the past few years, considerable advances have been made in the areas of the diode-pumped, eye-safe, solid state lasers, wide bandwidth, semiconductor detectors operating in the near-infrared region. These advances have created new possibilities for the development of low-cost, reliable, and compact coherent lidar systems for measurements of atmospheric winds and aerosol backscattering from a space-based platform. The work performed by the UAH personnel concentrated on design and analyses of solid state pulsed coherent lidar systems capable of measuring atmospheric winds from space, and design and perform laboratory experiments and measurements in support of solid state laser radar remote sensing systems which are to be designed, deployed, and used by NASA to measure atmospheric processes and constituents. A lidar testbed system was designed and analyzed by considering the major space operational and environmental requirements, and its associated physical constraints. The lidar optical system includes a wedge scanner and the compact telescope designed by the UAH personnel. The other major optical components included in the design and analyses were: polarizing beam splitter, routing mirrors, wave plates, signal beam derotator, and lag angle compensator. The testbed lidar optical train was designed and analyzed, and different design options for mounting and packaging the lidar subsystems and components and support structure were investigated. All the optical components are to be mounted in a stress-free and stable manner to allow easy integration and alignment, and long term stability. This lidar system is also intended to be used for evaluating the performance of various lidar subsystems and components that are to be integrated into a flight unit and for demonstrating the integrity of the signal processing algorithms by performing actual atmospheric measurements from a ground station.

Amzajerdian, Farzin↗

Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO 4 (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle neutron scattering (SANS) data reveal that PEO chains are adsorbed on the surface of LFP particles during slurry processing to make the composite electrode. The strong interaction between LFP and PEO chains leads to greatly reduced segmental dynamics of PEO, as discovered by quasi-elastic neutron scattering (QENS). The reduced segmental dynamics results in 70% decreased Li + mobility of the polymer electrolyte in the composite cathode. The combined SANS and QENS study indicates that one of the key bottlenecks that limits the rate performance of PEO-based polymer batteries originates from molecular interactions within the cathode.

25 ENERGY STORAGE↗

Solid-State, Single-Ion Conducting, Polymer Blend Electrolytes with Enhanced Li + Conduction, Electrochemical Stability, and Limiting Current Density

The development of solid-state polymer electrolytes with high lithium conductivity is crucial to improve lithium-ion battery performance and ameliorate the safety challenges associated with current solvent-based electrolytes. Unfortunately, sluggish polymer segmental dynamics are known to constrain conductivity enhancements in solid-state polymer electrolyte systems, limiting overall performance. In this work, a glassy single-ion-conducting polymer, poly[lithium sulfonyl(trifluoromethane sulfonyl)imide methacrylate] (PLiMTFSI), was blended with a flexible polymer, poly(oligo-oxyethylene methyl ether methacrylate) (POEM), and the impact of PLiMTFSI molecular weight and ion concentration on the thermal and ion-conducting behavior of blend electrolytes was investigated. High ionic conductivities approaching 1 × 10 -2 S/cm at 150 °C were realized in this polymer blend electrolyte system as a result of decoupling Li + transport from polymer segmental dynamics. The decoupled ion transport was attributed to the packing frustration of the glassy PLiMTFSI – sufficient percolating free volume was generated to produce effective ion diffusion pathways. This decoupling was tunable as the ion transport could be altered from being closely coupled to the polymer segmental dynamics (Vogel–Tammann–Fulcher-like) to hopping (Arrhenius-like) by increasing the PLiMTFSI molecular weight and ion concentration. Moreover, the immobilized TFSI anion resulted in high Li + selectivity (Li + transference number = 0.9), high electrochemical stability (up to 4.7 V against Li + / Li), and limiting current density of 1.8 mA/cm 2 (electrolyte thickness = 0.05 cm). These features suggest that this single-ion-conducting, polymer blend electrolyte might be a promising alternative to a benchmark system – salt-doped polyethylene oxide. Moreover, the above characteristics can support the battery operation at higher voltages using energy-dense Li metal anodes, with faster charging rates and enhanced energy/power densities. Altogether, the results suggest that polymer chain packing frustration can be exploited to overcome the constraints of slow polymer segmental relaxations to achieve rapid and highly selective ion transport and enhanced performance in solid-state polymer electrolytes.

36 MATERIALS SCIENCE↗

Recent advances in solid polymer electrolyte fuel cell technology with low platinum loading electrodes

Of all the fuel cell systems only alkaline and solid polymer electrolyte fuel cells are capable of achieving high power densities (greater than 1 W/sq cm) required for terrestrial and extraterrestrial applications. Electrode kinetic criteria for attaining such high power densities are discussed. Attainment of high power densities in solid polymer electrolyte fuel cells has been demonstrated earlier by different groups using high platinum loading electrodes (4 mg/sq cm). Recent works at Los Alamos National Laboratory and at Texas A and M University (TAMU) demonstrated similar performance for solid polymer electrolyte fuel cells with ten times lower platinum loading (0.45 mg/sq cm) in the electrodes. Some of the results obtained are discussed in terms of the effects of type and thickness of membrane and of the methods platinum localization in the electrodes on the performance of a single cell.

Srinivasan, Supramaniam↗

Crystal engineering of heterocyclic arylene(ethynylene) oligomers through programmed aromatic stacking

Conjugated oligomers and polymers consisting of aromatic heterocycles are examples of next-generation organic electronic materials. However, control and optimization of the self-assembly of these materials in the solid-state, which is a crucial parameter for high efficiency performance, remains an unsolved challenge in materials development. In this work, we provide valuable insight into aromatic stacking interactions between fluorinated arene rings (ArF) and heterocycles with different electronic character (Het), and elaborate on the prospect of using these interactions to control the solid-state configurations of three-ring phenyleneethynylene oligomers (PEs). Oligomers possessing heterocycles typically thought of as electron-rich (ER) show blue-shifted optical spectra in the solid-state, while those incorporating heterocycles typically thought of us electron deficient (ED) show red-shifted solid-state optical spectra. Crystal structures show ArF-Het stacking interactions between the fluorinated side-chains and ER units, which twist the backbone out of planarity and prevent chromophore aggregation. Further, the interactions are absent in ED oligomers, highlighting cofacial incompatibility between ArF rings and ED units. A combination of TD-DFT computations and novel heterocycle descriptors reinforce our assignment of the oligomers as ED or ER, while exhaustive conformer analysis shows ArF-Het stacking interactions are a significant contributor to compound stability. Overall, this work describes the importance of heterocycle electronics in conformational control in the solid state, understanding of which can be a valuable asset in the development of novel optoelectronic materials.

36 MATERIALS SCIENCE↗

Growth Angle - a Microscopic View

The growth angle that is formed between the side of the growing crystal and the melt meniscus is an important parameter in the detached Bridgman crystal growth method, where it determines the extent of the crystal-crucible wall gap, and in the Czochralski and float zone methods, where it influences the size and stability of the crystals. The growth angle is a non-equilibrium parameter, defined for the crystal growth process only. For a melt-crystal interface translating towards the crystal (melting), there is no specific angle defined between the melt and the sidewall of the solid. In this case, the corner at the triple line becomes rounded, and the angle between the sidewall and the incipience of meniscus can take a number of values, depending on the position of the triple line. In this work, a microscopic model is developed in which the fluid interacts with the solid surface through long range van der Waals or Casimir dispersive forces. This growth angle model is applied to Si and Ge and compared with the macroscopic approach of Herring. In the limit of a rounded corner with a large radius of curvature, the wetting of the melt on the crystal is defined by the contact angle. The proposed microscopic approach addresses the interesting issue of the transition from a contact angle to a growth angle as the radius of curvature decreases.

Mazurak, K.↗

Tackling issues of lithium metal anodes with a novel polymeric lithicone coating

Lithium metal (Li) has been hindered from as anodes in commercial batteries for over 50 years, due to two main issues: continuous formation of solid electrolyte interphase (SEI) and lithium dendritic growth. In this work, we report a new strategy to tackle these issues, i.e., using molecular layer deposition (MLD) to grow an ionically conducting but electrically insulating polymeric lithicone coating, an Li-containing triethanolamine (LiTEA). Our electrochemical tests revealed that this LiTEA coating could serve as an exceptional protection layer over Li anodes. Consequently, the LiTEA-coated Li electrodes could achieve a superior cyclability of > 10000 Li stripping/plating cycles at a current density of 5 mA cm -2 and a long cyclability of > 5500 cycles at 2 mA cm -2 in Li||Li symmetric cells without failures, under a fixed areal capacity of 1 mAh cm -2 . Characterizations using scanning electron microscopy and X-ray photoelectron microscopy verified that Li + ions could be easily extracted through and deposited under the LiTEA coating during the stripping/plating processes. Consequently, this LiTEA coating significantly inhibited the formation of SEI and Li dendrites. This underlies the long cycling lifetime of the LiTEA-coated Li||Li cells. Coupling with the nickel-rich LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes, more encouragingly, the LiTEA-coated Li anodes could remarkably extend the cyclability and sustainable capacity of the resultant Li||NMC full cells. Finally, we also demonstrated that the performance of Li||NMC cells could be further improved through combining an LiTEA-coated Li anode with an Li 2 S-modified NMC811 via atomic layer deposition (ALD). Thus, this study is inspiring for developing high-energy Li||NMC lithium metal batteries.

25 ENERGY STORAGE↗

An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries

All-solid-state sodium batteries (ASSSBs) are promising candidates for grid-scale energy storage. However, there are no commercialized ASSSBs yet, in part due to the lack of a low-cost, simple-to-fabricate solid electrolyte (SE) with electrochemical stability towards Na metal. In this work, we report a family of oxysulfide glass SEs (Na 3 PS 4-x O x , where 0 < x ≤ 60) that not only exhibit the highest critical current density among all Na-ion conducting sulfide-based SEs, but also enable high-performance ambient-temperature sodium-sulfur batteries. By forming bridging oxygen units, the Na 3 PS 4-x Ox SEs undergo pressure-induced sintering at room temperature, resulting in a fully homogeneous glass structure with robust mechanical properties. Furthermore, the self-passivating solid electrolyte interphase at the Na|SE interface is critical for interface stabilization and reversible Na plating and stripping. The new structural and compositional design strategies presented here provide a new paradigm in the development of safe, low-cost, energy-dense, and long-lifetime ASSSBs.

25 ENERGY STORAGE↗

Solid medium thermal engine

A device is described which uses a single phase metallic working substance to convert thermal energy directly into mechanical energy. The device consists of a cylindrical metal tube which is free to rotate about its axis while being subjected to continuous bending moment stresses along the longitudinal axis of rotation. The stressing causes portions of the tube to be under compression while other parts are under tension which in turn causes the tube to rotate and provide mechanical energy.

Jedlicka, J. R.↗

Measurements of the quantum geometric tensor in solids

Understanding the geometric properties of quantum states and their implications in fundamental physical phenomena is a core aspect of contemporary physics. The quantum geometric tensor (QGT) is a central physical object in this regard, encoding complete information about the geometry of the quantum state. The imaginary part of the QGT is the well-known Berry curvature, which plays an integral role in the topological magnetoelectric and optoelectronic phenomena. The real part of the QGT is the quantum metric, whose importance has come to prominence recently, giving rise to a new set of quantum geometric phenomena such as anomalous Landau levels, flat band superfluidity, excitonic Lamb shifts and nonlinear Hall effect. Despite the central importance of the QGT, its experimental measurements have been restricted only to artificial two-level systems. Here, in this work, we develop a framework to measure the QGT in crystalline solids using polarization-, spin- and angle-resolved photoemission spectroscopy. Using this framework, we demonstrate the effective reconstruction of the QGT in the kagome metal CoSn, which hosts topological flat bands. Establishing this momentum- and energy-resolved spectroscopic probe of the QGT is poised to significantly advance our understanding of quantum geometric responses in a wide range of crystalline systems.

36 MATERIALS SCIENCE↗

Mechanistic Study of Lead Adsorption on Activated Carbon

Activated carbon (AC) is a carbonaceous material broadly applied in filters to remove lead (Pb(II)) from drinking water through adsorption. However, the chemical interactions between Pb(II) and the reactive sites on AC or other carbonaceous materials are not well understood, yet. The understanding of the mechanism of Pb(II) adsorption onto AC would allow to optimally design AC-based materials even in the presence of a complex liquid phase. Here in this paper, the interaction between Pb(II) and functional groups on AC was investigated at the molecular scale to help identifying the chemical reactions at the solid-liquid interface. Spectroscopic analyses and chemical quantum calculations were performed and indicated the formation of monodentate mononuclear Pb(II)-phenol and bidentate mononuclear Pb(II)-carboxyl complexes on AC. Competitive adsorption behavior was observed between Pb(II) and calcium (Ca(II)) because of their similar adsorption configurations on AC. In contrast, anions, including sulfate and phosphate, were observed to enhance Pb(II) adsorption on AC by forming ternary complexes. On the basis of these observations, a new surface complexation model of Pb(II) adsorption onto AC was formulated and validated with batch tests. Overall, this work presents a new set of chemical reactions at the solid-liquid interface between Pb(II) and AC under various conditions of interest for the application of AC or other carbonaceous materials in water treatment.

36 MATERIALS SCIENCE↗

Reduced hazard chemicals for solid rocket motor production

During the last three years. the NASA/Thiokol/industry team has developed and started implementation of an environmentally sound manufacturing plan for the continued production of solid rocket motors. NASA Marshall Space Flight Center (MSFC) and Thiokol Corporation have worked with other industry representatives and the U.S. Environmental Protection Agency (EPA) to prepare a comprehensive plan to eliminate all ozone depleting chemicals from manufacturing processes and reduce the use of other hazardous materials used to produce the space shuttle reusable solid rocket motors. The team used a classical approach for problem-solving combined with a creative synthesis of new approaches to attack this challenge.

Larry A. Caddy↗

Solid Particle Number and Mass Emissions from Lean and Stoichiometric Gasoline Direct Injection Engine Operation

In this work, engine-out particle mass (PM) and particle number (PN) emissions were experimentally examined from a gasoline direct injection (GDI) engine operating in two lean combustion modes and one stoichiometric mode with a fuel of known properties. Ten steady state operating points, two constant speed load steps, and an engine cold start were examined. Results showed that solid particles emitted from the engine under steady state stoichiometric conditions had a uniquely broad size distribution that was relatively flat between the diameters of 10 and 100 nm. In most operating conditions, lean homogenous modes can achieve lower particle emissions than stoichiometric modes while improving engine thermal efficiency. Alternatively, lean stratified operating modes resulted in significantly higher PN and PM emissions than both lean homogeneous and stoichiometric modes with increased efficiency only at low engine load. Stoichiometric load steps showed minimal soot emissions while ash-mode emissions spike dramatically due to oil consumption caused by piston ring adjustment. Correlation of PN to PM for steady state stoichiometric cases was in good agreement with that reported from multiple prior studies for both diesel and stoichiometric GDI engines. However, the lean cases resulted in higher PN to PM ratios indicating more small particles per unit mass. High ash particle concentration, especially in lean operation illustrates that oil control is important for mitigating impacts on downstream gasoline particulate filters (GPF) from which ash particles are cannot be removed during filter regeneration. Further research is necessary to elucidate the origin and composition of sub-23 nm particles from GDI engines and their effect on aftertreatment technology if lean homogeneous modes are to be employed.

Bock, Noah↗

Space-dependent calculation of the multiplicity moments for shells

In earlier work, we extended the methodology of multiplicity counting in nuclear safeguards, by elaborating the one-speed stochastic transport theory of the calculation of the so-called multiplicity moments, i.e. the factorial moments of the number of neutrons emitted from a fissile item, following a source event from an internal neutron source (spontaneous fission and (α, n) reactions). Calculations were made for spheres and cylinders of various shapes. In all our work so far, the material of the items was homogeneous, and the distribution of the internal source was assumed to be uniformly distributed within the item, with the neutron emission assumed to be isotropic. In the present work the calculations are extended to the case of a point source inside either a solid sphere or in a spherical shell. This necessitates the extension of the theory to non-homogeneous items and non-uniform and non-isotropic sources. This work describes the extension of the theory and provides some quantitative results. (authors)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Critical review and future prospects for desiccant coated heat exchangers: Materials, design, and manufacturing

Solid desiccant dehumidification is a promising alternative to vapor compression-based air-dehumidification to reduce energy consumption and improve air quality. Desiccant coated heat exchanger (DCHE), as one type of solid desiccant dehumidification system, can improve system performance and efficiency. The thermal performance and moisture removal capability of the DCHE greatly influence its dehumidification performance.The present work aims to critically analyze the designs, materials, and manufacturing methods of heat exchangers used for solid desiccant coating and look into recent developments in regular heat exchangers, potentially deployed as a substrate for DCHE applications. A comprehensive literature review of publications regarding solid desiccant materials, heat exchangers, manufacturing and coating methods, binder materials, and the performance of heat exchangers has been developed. Alternative heat exchangers are described as better options than fin and tube heat exchangers that have been considered thus far for DCHE applications. Additionally, the heat exchanger's manufacturing process and materials over their thermal and mass exchange performance have been analyzed. Despite the widespread use of fin and tube heat exchangers for solid desiccant coating, recent developments in heat exchanger design, and related fields such as manufacturing methods and materials, open the possibilities for their application in solid desiccant dehumidification systems. Lastly, the authors provide their outlook on possible developments of DCHE technology, aiming to increase systems' energy and dehumidification performance.

36 MATERIALS SCIENCE↗