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At least 631 records · Page 35

Solvable theory of a strange metal at the breakdown of a heavy Fermi liquid

In this work, we introduce an effective theory for quantum critical points (QCPs) in heavy-fermion systems, involving a change in carrier density without symmetry breaking. Our theory captures a strongly coupled metallic QCP, leading to robust marginal Fermi-liquid transport phenomenology, and associated linear in temperature (T) "strange metal" resistivity, all within a controlled large-N limit. In the parameter regime of strong damping of emergent bosonic excitations, the QCP also displays a near-universal "Planckian" transport lifetime τ tr ~ℏ/(k B T). This is contrasted with the conventional so-called "slave boson" theory of the Kondo breakdown, where the large-N limit describes a weak coupling fixed point and nontrivial transport behavior may only be obtained through uncontrolled 1/N corrections. We also compute the weak-field Hall coefficient within the effective model as the system is tuned across the transition. We then find that, between the two plateaus reflecting the different carrier densities in the two Fermi-liquid phases, the Hall coefficient can develop a peak in the critical crossover regime, like in recent experimental findings, in the parameter regime of weak boson damping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Oh, My Darling Clementine: A Detailed History and Data Repository of the Los Alamos Plutonium Fast Reactor

The Los Alamos Plutonium Fast Reactor, Clementine, provided the first fast neutron spectrum using a metallic plutonium fuel system and liquid mercury coolant. Clementine is often mentioned in the history of fast, metal-fueled, or metal-cooled designs, with little public information regarding the specifications or timeline. This paper contains a synopsis of each report regarding the development, operation, experimental results, failures, and subsequent disassembly of Clementine to explore this unique reactor within the context of modern advanced reactor development.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Capturing the swelling of solid-electrolyte interphase in lithium metal batteries

Although liquid-solid interfaces are foundational in broad areas of science, characterizing this delicate interface remains inherently difficult because of shortcomings in existing tools to access liquid and solid phases simultaneously at the nanoscale. This leads to substantial gaps in our understanding of the structure and chemistry of key interfaces in battery systems. We adopt and modify a thin film vitrification method to preserve the sensitive yet critical interfaces in batteries at native liquid electrolyte environments to enable cryo–electron microscopy and spectroscopy. We report substantial swelling of the solid-electrolyte interphase (SEI) on lithium metal anode in various electrolytes. Here, the swelling behavior is dependent on electrolyte chemistry and is highly correlated to battery performance. Higher degrees of SEI swelling tend to exhibit poor electrochemical cycling.

25 ENERGY STORAGE↗

Hydrogen, lithium, and lithium hydride production

A hydrogen, lithium, and lithium hydride processing apparatus includes a hot zone to heat solid-phase lithium hydride to form liquid-phase lithium hydride; a vacuum source to extract hydrogen and gaseous-phase lithium metal from the liquid-phase lithium hydride; a cold zone to condense the gaseous-phase lithium metal as purified solid-phase lithium metal; and a heater to melt the purified solid-phase lithium metal in the cold zone and form refined liquid-phase lithium metal in the hot zone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Reversible Electrochemical Phase Change in Monolayer to Bulk-like MoTe 2 by Ionic Liquid Gating

Transition-metal dichalcogenides (TMDs) exist in various crystal structures with semiconducting, semi-metallic, and metallic properties. The dynamic control of these phases is of immediate interest for next-generation electronics such as phase change memories. Of the binary Mo and W-based TMDs, MoTe 2 is attractive for electronic applications because it has the lowest energy difference (40 meV) between the semiconducting (2H) and semi-metallic (1T') phases, allowing for MoTe 2 phase change by electrostatic doping. Here, we report phase change between the 2H and 1T' polymorphs of MoTe 2 in thicknesses ranging from the monolayer to bulk-like case (73 nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-1T' transition using in situ Raman spectroscopy where the phase change occurs in the topmost layers of the MoTe 2 flake. We find a thickness-dependent transition voltage where higher voltages are necessary to drive the phase change for thicker flakes. We also show evidence of electrochemical activity during the gating process by observation of Te metal formation. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and 1T' phases, potentially aiding the phase change process. Furthermore, our discovery that the phase change can be achieved on the surface layer of bulk-like materials reveals that this electrochemical mechanism does not require isolation of a single layer and the effect may be more broadly applicable than previously thought.

2d materials↗

Numerical and Experimental Study of a Novel Additively Manufactured Metal-Polymer Composite Heat-Exchanger for Liquid Cooling Electronics

In order to meet increasing power-dissipation requirements of the electronics industry, compact, low-cost, and lightweight heat exchangers (HXs) are desired. With proper design, materials, and manufacture, polymer composite heat exchangers could meet these requirements. This paper presents a novel crossflow air-to-water, low-cost, and lightweight metal-polymer composite HX. This HX, which is entirely additively manufactured, utilizes a novel cross-media approach that provides direct heat exchange between air and liquid sides by using connecting fins. A robust numerical model was developed, which includes the dimensional effects of additive manufacturing. The study consists of a simplified 3D CFD model based on ellipsoidal-shaped staggered tube banks for the laminar range. It then uses an analytical approach to compute entire HX performance. The model is validated experimentally within 8% for thermal performance, 12% for air-side impedance, and 18% for water-side impedance. Finally, HX is compared with a conventional CPU radiator and performs within 10% of the conventional unit for reasonable flow rates and pressure-drop ranges. Moreover, HX also provides added design and cost advantages over the conventional unit, which makes the HX a potential candidate for electronic cooling applications.

30 DIRECT ENERGY CONVERSION↗

Phase diagram of the anisotropic triangular lattice Hubbard model

In a recent study [Phys. Rev. X 10, 021042 (2020)], we showed using large-scale density matrix renormalization group (DMRG) simulations on infinite cylinders that the triangular lattice Hubbard model has a chiral spin liquid phase. In this work, we introduce hopping anisotropy in the model, making one of the three distinct bonds on the lattice stronger or weaker compared with the other two. We implement the anisotropy in two inequivalent ways, one which respects the mirror symmetry of the cylinder and one which breaks this symmetry. In the full range of anisotropy, from the square lattice to weakly coupled one-dimensional chains, we find a variety of phases. Near the isotropic limit we find the three phases identified in our previous work: metal, chiral spin liquid, and 120$^\circ$ spiral order; we note that a recent paper suggests the apparently metallic phase may actually be a Luther-Emery liquid, which would also be in agreement with our results. Furthermore, when one bond is weakened by a relatively small amount, the ground state quickly becomes the square lattice N\'{e}el order. When one bond is strengthened, the story is much less clear, with the phases that we find depending on the orientation of the anisotropy and on the cylinder circumference. While our work is to our knowledge the first DMRG study of the anisotropic triangular lattice Hubbard model, the overall phase diagram we find is broadly consistent with that found previously using other methods, such as variational Monte Carlo and dynamical mean field theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Characterizing Olefin Selectivity and Stability of Silver Salts in Ionic Liquids Using Inverse Gas Chromatography

Separation systems utilizing silver(I) ion-olefin complexation have limitations since silver(I) ions can be poisoned or reduced to metallic silver. Ionic liquids (ILs) are used as solvents for silver(I) ions to facilitate separations since their physico-chemical properties can be easily tuned. To develop separation systems with sustainable olefin selectivity, factors that affect silver(I) ion stability need to be understood. In this study, a total of 13 silver salt/IL mixtures were examined by inverse gas chromatography to identify the effects of silver salt anion and IL cation/anion combination on silver(I) ion stability. The effects of temperature and three different exposure gases on silver(I) ion stability were systematically studied. Exposing silver salt/IL mixtures to hydrogen at high temperatures had a greater effect on decreasing silver(I) ion-olefin complexation. Silver(I) ions from the silver bis[(trifluoromethyl)sulfonyl]imide ([NTf 2 – ]) salt were more stable in [NTf 2 – ]-containing ILs than in [BF 4 – ]-containing ILs. Optimum mixtures exhibited high olefin selectivity and were stable beyond 90 h when exposed to hydrogen gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

One-dimensional heterocyclic carbene–Au metal–organic frameworks bridging ultra-high vacuum models and scalable liquid-phase growth

The controlled design of molecule–metal interfaces is central to the development of functional nanomaterials for catalysis, sensing, and molecular electronics. Here we show that the adsorption of a Janus-type diimidazolium precursor on gold yields one-dimensional (1D) N-heterocyclic carbene (NHC)–Au–NHC metal organic frameworks (MOFs) featuring positively charged gold nodes. Using synchrotron X-ray photoemission spectroscopy (XPS), near edge X-ray adsorption fine structure (NEXAFS) spectroscopy and scanning tunnelling microscopy (STM), we demonstrate that thermal activation promotes counterion removal and drives the formation of extended 1D arrays, characterized by ∼1.0 nm Au–Au spacing and adatom densities up to 0.6 atom nm −2 (∼4% of surface atoms). Importantly, we translate this ultra-high vacuum (UHV) benchmark into a scalable solution-phase protocol in ethanol, enabling 1D-MOF growth under mild, base-free, open-air conditions. The resulting films retain structural and electronic signatures of UHV-grown systems, bridging model studies and practical synthesis. This approach establishes NHC–metal frameworks as accessible, tunable platforms for catalysis and materials design.

Gold adatoms↗

Combustion of metal powder with dinitrogen tetroxide

In this work, we present analysis of a novel reactive material system that employs dinitrogen tetroxide (N 2 O 4 ) as a liquid oxidizer with metal powder fuels. The oxidizer was added to micron scale aluminum and zirconium powders by a remote injection system. When ignited with a high voltage spark, the mixtures were observed to possess reactivity comparable to nanocomposite reactive materials, with open-tube flame expansion velocities from 500 to 1400 m/s depending on fuel/oxidizer ratio and tube diameter. Temperatures were observed to range from 3000 to 3500 K as measured with gray body fits to 16-channel time-resolved pyrometer and time-integrated spectrometer data. These values were significantly below calculated adiabatic flame temperatures, which we attribute to local deviations from stoichiometry and kinetic/energetic limitations similar to those observed in studies of particles burning in high pressures gaseous oxidizers. Al/N 2 O 4 reactivity was found to be most likely limited by the vaporization of the metal from the particle surface and Zr/N 2 O 4 was limited by slower burning and complex interactions involving the solubility of nitrogen and oxygen in the molten Zr. We also discuss the potential for these materials to be used to create an “on/off” reactive material, since N2O4 can be added remotely and driven to evaporate via vacuum or purge of inert gases to return it to a safe condition.

36 MATERIALS SCIENCE↗

A comprehensive review on liquid electrolyte design for low-temperature lithium/sodium metal batteries

Lithium/sodium metal batteries (LMBs/SMBs) possess immense potential for various applications due to their high energy density. Nevertheless, LMBs/SMBs are highly susceptible to the detrimental effects of an unstable solid electrolyte interphase (SEI) and dendrites during practical applications, particularly pronounced in low-temperature environments. Furthermore, sluggish ion transportation further compromises the cycling stability of LMBs/SMBs at low temperatures. To achieve stable operation of LMBs/SMBs at low temperatures, researchers have made numerous efforts including electrolyte optimization aimed at creating stable SEIs and suppressing the metal dendrites under low temperature conditions. Despite the significant advancements made recently in the liquid electrolyte design, there remains considerable hurdle in electrolyte engineering for practical low-temperature, high energy density LMBs/SMBs, calling for a profound comprehension of the intricate interplay between the electrochemical reaction kinetics and electrolyte compositions. Here, this review provides a thorough overview of various strategies in optimizing liquid electrolytes covering weakly solvating electrolytes, concentration-designed electrolytes, and solvation structure-designed electrolytes, to address the challenges faced by LMBs/SMBs at low temperatures, including slow reaction kinetics and the difficulties in Li + /Na + solvation/desolvation. Furthermore, this review discusses future prospects for the advancement of this field, intending to provide valuable insights and support for subsequent research undertakings.

25 ENERGY STORAGE↗

Method to produce salts containing actinide halides

A method of producing uranium halides is disclosed in which chlorine gas is introduced into a liquid uranium-nickel alloy. NaCl salt is surrounding the crucible containing the liquid uranium-nickel alloy, producing a eutectic mixture of NaCl—UCl3. Upon chlorination, the metal halide dissolves in the matrix salt forming a solution. Adding the reactant metal, uranium to the nickel, the alloy is able to remain molten throughout processing. The liquid metal alloy may be removed from the salt bath, while the halogen gas continues to enter the system through the sparge until the desired composition of NaCl—UCl3—UCl4 is achieved. The method and system can be used to produce other metal halide salts such as actinide, lanthanide or transition metal halides contained in a matrix salt consisting of alkali and/or alkaline earth halides.

Williamson, Mark A.↗

Composite Fermi Liquid at Zero Magnetic Field in Twisted MoTe 2

Here, the pursuit of exotic phases of matter outside of the extreme conditions of a quantizing magnetic field is a long-standing quest of solid state physics. Recent experiments have observed spontaneous valley polarization and fractional Chern insulators in zero magnetic field in twisted bilayers of MoTe 2 , at partial filling of the topological valence band (ν =-2/3 and -3/5). We study the topological valence band at half filling, using exact diagonalization and density matrix renormalization group calculations. We discover a composite Fermi liquid (CFL) phase even at zero magnetic field that covers a large portion of the phase diagram near twist angle ~3.6°. The CFL is a non-Fermi liquid phase with metallic behavior despite the absence of Landau quasiparticles. We discuss experimental implications including the competition between the CFL and a Fermi liquid, which can be tuned with a displacement field. The topological valence band has excellent quantum geometry over a wide range of twist angles and a small bandwidth that is, remarkably, reduced by interactions. These key properties stabilize the exotic zero field quantum Hall phases. Finally, we present an optical signature involving “extinguished” optical responses that detects Chern bands with ideal quantum geometry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Extracted Water Induces Concentration Fluctuations in Model Ternary Liquid–Liquid Extraction System

Organic phase aggregation and phase splitting are two important (and connected) phenomena in liquid–liquid extraction of metal ions. Previously, we demonstrated how structure in binary mixtures of extractant and diluent originates from concentration fluctuations associated with the so-called “third-phase formation” liquid–liquid phase instability. For more complex systems, we sought to understand how extracted aqueous components affect these concentration fluctuations. Here, in this study, we use small-angle X-ray scattering and molecular dynamics simulations to investigate organic phase structural changes upon contact with water in a model ternary system of water/alkane/extractant. Critical exponents were determined from scattering with temperature variation and were consistent with mean field values. Then, by controlling the water content in the organic phase through direct dissolution of fixed quantities at constant temperature, we relate the observed increase in the fluctuation length scale to changes to the spinodal temperature of the third-phase formation phase boundary. We find a roughly linear relationship between water concentration and the spinodal temperature and a similar slope in that relationship for different linear alkane diluents. This suggests that the mechanism by which water extraction impacts the organic phase structure is to enhance concentration fluctuations through the introduction of additional polar extractant-water complexes, which increases the spinodal temperature and thereby decreases the reduced temperature, i.e., the distance to the instability. This explanation for how solutes induce aggregation in liquid–liquid extraction organic phases may extend to more complex systems, explaining the large increases in correlation lengths reported under high acid and metal loading.

Bonnett, Brittany L. [Argonne National Laboratory ↗

Irradiation Effect on Noble Metal Particles in Water Using in situ Liquid Cell STEM Observation

During geologic disposal of spent nuclear fuel (SNF) in an engineered nuclear waste repository, once all other barriers have degraded, oxidizing may occur at the solid-water interface owing to a self-generated radiolytic field. The repository design includes large quantities of iron (Fe), that is anticipated to corrode under an anoxic environment, and generate hydrogen (H 2 ) gas. This H 2 gas is thought to be able to suppress the dissolution of SNF through a catalytic reaction with noble metal particles (NMP) that are pre-existing in the SNF. This interaction leads to the decomposition of the major oxidant, hydrogen peroxide (H 2 O 2 ). In conclusion, these processes are described in the Fuel Matrix Degradation (FMD) model that is being used to predict SNF degradation rates. The NMP, therefore, plays an important role within the FMD model.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nano-Plasticity of an Electrified Ionic Liquid/Electrode Interface: Uncovering Hard–Soft Structuring via Controlled Metal Fill Factor

Here, ionic liquids (ILs) nanostructuring at electrified interfaces is of both fundamental and practical interest as these materials are increasingly gaining prominence in energy storage and conversion processes. However, much remains unresolved about IL potential-controlled (re)organization under highly polarized interfaces, mostly due to the difficulty of selectively probing both the distal and proximal surface layers of adsorbed ions. In this work, the structural dynamics of the innermost layer (<10 nm from the surface) were independently interrogated from that of the ionic layers in the sub-surface region (>100 nm from the surface), using an infrared (IR) spectroscopy approach. By tuning the metal fill factor of gold films deposited on conductive metal oxide-modified IR internal reflection elements, the charge-driven (re)structuring of the inner and distal layers of 1-butyl-1-methylpyrrolidinium trifluoromethanesulfonate is unveiled. Within a relatively wide potential region (~±1 V) bounding the potential of zero charges, the ionic liquid is shown to undergo a reversible (i.e., soft) reorganization whereby the innermost layer of anions (cations) is exchanged by a layer of cations (anions). Kinetically unhindered changes in the number density of constituent cations and anions largely follow electrostatic expectations in the subsurface region, whereas the innermost layer exhibits a pronounced hysteresis and very slow relaxation. Under larger negative potential bias, IL restructuring is characterized by a highly irreversible (i.e., hard) and intense interfacial densification of the BMPy + cations, consistent with the formation of nanoscale segregated liquids. The outcomes of this work reveal a plastic IL nanostructuring under a strong electric field.

36 MATERIALS SCIENCE↗

Cyclohexene epoxidation with H 2 O 2 in the vapor and liquid phases over a vanadium-based metal–organic framework

A metal–organic framework, MIL-47(V) containing coordinatively saturated V +IV sites linked together by terephthalic linkers, was prepared by a solvothermal method and evaluated as a catalyst in the epoxidation of cyclohexene. We have compared the catalytic activity in the condensed and gas phase oxidation of cyclohexene to discuss the effect of temperature and reaction phase in cyclohexene epoxidation over MIL-47(V). The catalysts were examined for the epoxidation of cyclohexene with H 2 O 2 at 50, 65, 120, and 150 °C. Finally, we observed significant differences in product selectivity between liquid-phase and gas-phase operations and confirmed that the active sites are tightly incorporated into the MOF as node channels and thus resistant to leaching.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Semi-solid alkali metal electrodes enabling high critical current densities in solid electrolyte batteries

The need for higher energy density rechargeable batteries has generated interest in alkali metal electrodes paired with solid electrolytes. However, metal penetration and electrolyte fracture at low current densities have emerged as fundamental barriers. Here, we show that for pure metals in the Li-Na-K system, the critical current densities scale inversely to mechanical deformation resistance. Furthermore, we demonstrate two electrode architectures in which the presence of a liquid phase enables high current densities while preserving the shape retention and packaging advantages of solid electrodes. First, biphasic Na-K alloys show K + critical current densities (with K-β*-Al 2 O 3 electrolyte) that exceed 15 mA∙cm -2 . Second, introducing a wetting interfacial film of Na-K liquid between Li metal and Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) solid electrolyte doubles the critical current density and permits cycling at areal capacities exceeding 3.5 mAh∙cm -2 . These design approaches hold promise for overcoming electro-chemo-mechanical stability issues that have heretofore limited performance of solid-state metal batteries.

25 ENERGY STORAGE↗