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At least 253 records · Page 14

Filterscope Techniques for Parasitic Signal Screening

Here, the filterscope diagnostic uses bandpass filters and photomultiplier tubes (PMTs) to detect specific spectral emission lines. A filterscope was used to measure the W I 400.88 nm line emission as a function of ion energy on the Radio Frequency Plasma Interaction Experiment (RF PIE) for the purpose of assessing W erosion on plasma-facing components (PFCs). Different filter techniques are being explored and compared in order to effectively screen out nearby impurity lines, like the Ar II 401.39 nm line. The effectiveness of these techniques is determined by comparing the measurements to a high-resolution 1.0 m Czerny–Turner spectrometer with 0.012 nm spectral resolution. The ability to filter out nearby impurity emissions is useful when imaging PFCs in fusion devices including divertor and antenna guard limiters. Initial results with a helium plasma show little difference between the two techniques at higher bias voltages. In a helium plasma at lower dc bias voltages, a two-filter technique with filters at two separate wavelengths was shown to be more effective at screening out background signals. Data collected with an argon plasma however show the technique with overlapping filters on the line of interest is a closer match to spectrometer data at lower dc bias voltages.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The Role of Metal Oxides in Li-S Batteries: A High-Areal-Capacity Sulfur Composite Cathode Investigation

Compared to lithium-ion batteries (LIB), lithium-sulfur (Li-S) batteries have low cost and high theoretical specific energy (2510 Wh/kg or about 10 times of the LIB). However, Li-S batteries have several challenges, including large volume expansion, poor utilization of the end products, sluggish kinetics of polysulfides, and crossover, so-called the "shuttle effect". To address these issues, we have introduced metal oxides to the Li-S electrode to develop a metal-oxide-sulfur composite electrode. We aim to use metal oxides to assist the Li-S formation (dissociation) during discharge (charge) cycles. We elect to focus on LIB-based metal oxides to ensure that the added material can contribute storage capacity to the battery. Our cathodes are fabricated by both the conventional slurry casting and air-controlled electrospray. LIB electrode materials, such as Li(Ni 0.6 Mn 0.6 Co 0.2 )O 2 , LiMn 2 O 4 , Li 2 TiO 3 , etc, were incorporated with the sulfur-carbon composite and their charge-discharge performances are compared. We found that the presence of metal oxides increased sulfur utilization with stable cycling performance, even in cells with high areal capacities. To unveil the interactions between lithium metal oxides and sulfur, the cathodes were analyzed by various characterization techniques, including scanning electron microscopy, X-ray diffraction, thermogravimetric analysis, and electrochemistry. The analysis of the role of the oxides will be presented along with the reaction mechanism.

25 ENERGY STORAGE↗

Orienting Strained Interfaces designed to Direct Energy Flow (Final Technical Report)

This proposal aims to establish a transformative paradigm for oxide heterostructures with an exceptionally large number of interfaces designed to direct energy flow through controlled interface orientation, enabling fast ion transport. A primary focus is on unveiling the key role of interfacial strain in oxygen ion migration at low temperatures. The central challenge is to create, understand, utilize self-assembled vertical heteroepitaxial nanostructures with the goal of obtaining and understanding fast ion transport properties by modulating interfacial strain. The specific objectives are: (1) to synthesize multilayer thin films and vertical heteroepitaxial nanostructures with fluorite Gd-doped CeO 2 (GDC) and bixbyite RE 2 O 3 (RE = Y and Sm), (2) to evaluate the interfacial strain states under various temperatures and ambient conditions, (3) to understand the effect of interfacial strain on ionic conductivity of the proposed nanostructures, (4) to understand the three-dimensional (3D) atomic structure of the proposed material design and interface phenomena at the atomic scale.

36 MATERIALS SCIENCE↗

Magnetism of Nd 2 O 3 single crystals near the Néel temperature

Single crystals of Nd 2 O 3 were grown and characterized using neutron scattering and thermodynamic measurements. Nd 2 O 3 has long-range antiferromagnetic order below T N =0.55 K and specific-heat measurements have demonstrated that a significant amount of the magnetic entropy is released above T N . Inelastic neutron scattering experiments reveal a magnetic mode(s) with little dispersion peaked at ≈0.37meV that is of greatest intensity below T N but persists above 2T N . This persistence of dynamic correlations is likely related to frustrated interactions associated with the nearly ideal stacked triangular lattice geometry of J eff =12 spins on Nd 3+ ions. Furthermore, the magnetization is observed to be strongly anisotropic at all temperatures due to crystal field effects, with easy-plane anisotropy observed. Additionally, a noncompensated magnetic structure is inferred from the temperature dependence of the magnetization when a magnetic field of sufficient strength is applied within the basal plane near T N , and the evolution of the long-range order is summarized in a temperature-field phase diagram.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nanoengineering Porous Silica for Thermal Management

Thermal insulation of solid materials originates from the nanoscale porous architectures to regulate thermal management in energy-critical applications from energy-efficient buildings to heat-sensitive energy devices. Here, we show nanoengineering of porous silica materials to control the architecture transition from mesoporous to nanocage networks. A low thermal conductivity of such a porous silica network is achieved at 0.018 W/(m K) while exhibiting a porosity of 92.05%, specific surface area of 504 m 2 /g, and pore volume of 2.37 cm 3 /g after ambient pressure drying. Meanwhile, the crosslinking of the porous silica and ceramic fiber frameworks show a tensile Young’s modulus of 2.8 MPa while maintaining high thermal insulation, which provides an effective thermal runway mitigation strategy for rechargeable lithium-ion batteries. Furthermore, the nanoengineering strategy reported here would shed light on achieving superthermal insulation of nanostructures for energy-critical applications.

36 MATERIALS SCIENCE↗

Quantum Approximate Optimization Algorithm on Different Qubit Systems

Solving optimization problems is critical across many research domains, but the high dimensionality of parameter spaces often poses significant challenges. The Quantum Approximate Optimization Algorithm (QAOA) has emerged as a promising approach for accelerating optimization in the Noisy Intermediate-Scale Quantum (NISQ) era by leveraging both classical and quantum computational resources. However, its performance can vary depending on the underlying quantum hardware architecture. In this work, we evaluate the performance of QAOA on different quantum hardware platforms, specifically, superconducting transmon qubits and trapped-ion qubits, targetting real-world optimization problems formulated as fully connected Quadratic Unconstrained Binary Optimization (QUBO) instances. We evaluate both the solution quality and time-to-solution using dense QUBO matrices. Furthermore, we show that large-scale problems, such as a 100-bit QUBO instance, can be effectively tackled by integrating quantum computing with high-performance computing (HPC) resources. This study provides practical insights into the strengths and limitations of different qubit technologies and advances the application of quantum computing in solving real-world optimization problems.

Kim, Seongmin [ORNL] (ORCID:0000000159063004)↗

Conformational Changes Induced by Methyl Side-Chains in Protonated Tripeptides Containing Glycine and Alanine Residues

We present a systematic study of the conformational and isomeric populations in gas-phase protonated tripeptides containing glycine and alanine residues using infrared predissociation spectroscopy of cryogenically cooled ions. Specifically, the protonated forms of Gly-Gly-Gly, Ala-Gly-Gly, Gly-Ala-Gly, Gly-Gly-Ala, Ala-Ala-Gly, Ala-Gly-Ala, Gly-Ala-Ala, and Ala-Ala-Ala allow us to sample all permutations of the methyl side-chain position, providing a comprehensive view of the effects of this simple side-chain on the 3-D structure of the peptide. The individual structural populations for all but one of these peptide species are determined via conformer-specific IR–IR double-resonance spectroscopy and comparison with electronic structure predictions. The observed structures can be classified into three main families defined by the protonation site and the number of internal hydrogen bonds. The relative contribution of each structural family is highly dependent on the exact amino acid sequence of the tripeptide. Here, these observed changes in structural population can be rationalized in terms of the electron-donating effect of the methyl side-chain modulating the local proton affinities of the amine and various carbonyl groups in the tripeptide.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stability and Control of Burning Tokamak Plasmas with Resistive Walls (Second Year Report/ Final Report)

This research will focus on quantitative prediction of the stability, control, and equilibrium state evolution in toroidal burning plasmas. The stability of long pulse burning plasmas is highly sensitive to the physics of resonant layers in the plasma, sources of momentum and ow, kinetic effects of energetic particles, and boundary conditions at the wall, including feedback control and error fields. In ITER in particular, the low toroidal ow equilibrium state, sustained primarily by energetic alpha particles from fusion reactions, will require the consideration of all of these key elements to predict quantitatively the stability and evolution. The principal investigators on this proposal are leading experts in the relevant theoretical and computational areas, and aim to perform computations guided by analytic modeling, to address this physics in realistic configurations. The overall goal is to understand the key physics mechanisms that describe resistive toroidal burning plasmas, surrounded by a resistive wall, under active feedback control. With the physics of the energetic ions, resonant layers, resistive wall, and toroidal momentum transport included, this study will extend from recent publications in theory and simulation of individual effects and move toward predictive modeling for burning plasmas.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Easy-plane anisotropic-exchange magnets on a honeycomb lattice: Quantum effects and dealing with them

We provide analytical and numerical insights into the phase diagram and other properties of the extended Kitaev-Heisenberg model on the honeycomb lattice in the easy-plane limit, in which interactions are only between spin components that belong to the plane of magnetic ions. This parameter subspace allows for a much-needed systematic quantitative investigation of spin excitations in the ordered phases and of their generic features. Specifically, we demonstrate that in this limit one can consistently take into account magnon interactions in both zero-field zigzag and field-polarized phases. For the nominally polarized phase, we propose a regularization of the unphysical divergences that occur at the critical field and are plaguing the 1/S approximation in this class of models. For the explored parameter subspace, all symmetry-allowed terms of the standard parametrization of the extended Kitaev-Heisenberg model, such as K, J, and Γ, are significant, making the offered consideration relevant to a much wider parameter space. Furthermore, the dynamical structure factor near the paramagnetic critical point illustrates this relevance by showing features that are reminiscent of the ones observed in α–RuCl 3 , underscoring that they are not unique and should be common to a wide range of parameters of the model and, by extension, to other materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Simulating the effects of warm O + ions on the growth of electromagnetic ion cyclotron (EMIC) waves

Electromagnetic ion cyclotron (EMIC) waves are believed to play a crucial role in the dynamics of the Earth’s magnetosphere. It has been widely accepted that plasma compositions can influence the growth rate of EMIC waves in the inner magnetosphere, but how warm O + ions change the wave growth rate is not well known. In this study, we investigate the impact of ring current O + concentration on the EMIC growth rate during a specific storm when the O + ion flux significantly increases. We calculate the growth rate of EMIC waves by using physics-based ion distributions output from the Ring current–Atmosphere interactions Model with Self-Consistent magnetic (B) and Electric (E) fields (RAM-SCBE) model. The percentage of warm O + is parametrically varied to examine how the maximum EMIC growth rate changes over time and how the global distribution of the maximum EMIC growth rate is affected. We found that the maximum growth rate of H-band appears in the dusk-to-midnight sector near the plasmapause, while O-band is excited at a slightly outer region. The maximum growth rate of He-band is closely related to the cold plasma density. With the increase of warm O + density, the maximum growth rate of H-band and He-band EMIC wave is reduced, while that of O-band EMIC wave is increased, and the region with this wave excitation is widened. Furthermore, such variation in the maximum EMIC growth rate implies a potential impact on the associated wave–particle interactions and change of the decay rate in the ring current.

79 ASTRONOMY AND ASTROPHYSICS↗

Calcium-Doped High-Voltage Spinel Cathode for Long Cycle Life Lithium-Ion Batteries

With the promises of low cost, high operating voltage, and excellent rate capability, the high-voltage spinel material with the formula of LiNi 0.5 Mn 1.5 O 4 (LNMO) has been considered as one of the most promising cathode materials for nextgeneration lithium-ion batteries (LIBs). However, the adoption of LNMO into practical LIBs is greatly hindered due to its rapid capacity decay associated with its bulk structural instability and interfacial side reactions. To address these issues, we proposed to use the cost-effective calcium (Ca) element as a dopant to stabilize the oxygen framework and surface of the LNMO crystal. The experimental results showed that, with moderate Ca doping, the obtained cathode (Ca 0.05 LNMO) retained a specific capacity of ∼121 mAh/g (∼94.4% capacity retention) after 500 cycles at 0.5 C, compared to ∼73% for the baseline bare sample. Furthermore, the Ca 0.05 LNMO cathode retained ∼84% of its initial capacity, vs the baseline with ∼69%, after 150 cycles at the high temperature of 55 °C. The excellent battery performance of the moderately Ca-doped LNMO cathode is ascribed to its structural and kinetic advantages.

25 ENERGY STORAGE↗

Reactive ion etched, self-aligned, selective area poly-Si/SiO 2 passivated contacts

Front/back poly-Si/SiO 2 contact devices suffer from low short-circuit current density, J sc , due to parasitic optical absorption in the front poly-Si layer. Thin poly-Si (~20 nm) allows for high J sc but is not compatible with screen-printed fire-through contacts. We therefore study the effects of post-deposition etching of a thick poly-Si (200 nm) front layer by reactive ion etching (RIE) using the metal grid lines as a self-aligned mask. We show that passivation is maintained in the device during RIE and that J sc is increased by a gain in the blue quantum efficiency response. However, our specific etching parameters cause non-uniform etching of the poly-Si leading to premature loss of passivation without optimal gain in J sc . Etched, unpassivated layers can be re-passivated with a H-containing dielectric layer leading to a gain in Jsc, open circuit voltage, V oc , Fill-Factor, FF, and efficiency.

14 SOLAR ENERGY↗

Unveiling the lithium-ion transport mechanism in Li{sub 2}ZrCl{sub 6} Solid-State Electrolyte {ital via} deep learning-accelerated molecular dynamics simulations.

Lithium zirconium chlorides (LZCs) present a promising class of cost-effective solid electrolytes for next-generation all-solid-state batteries. The unique crystal structure of LZCs plays a crucial role in facilitating lithium-ion mobility, which further affects the electrochemical performance. To understand the underlying mechanism governing ion transport, we employed deep learning-accelerated molecular dynamics simulation on Li2ZrCl6 (trigonal alpha- and monoclinic beta-LZC), focusing specifically on the zirconium coordination environment. Our results reveal that disordered alpha-LZC exhibits the highest ionic conductivity, while beta-LZC demonstrates significantly lower conductivity, closely aligning with experimental findings. The study confirms that across all phases, lithium migration proceeds via the site-to-site hopping mechanism, where variations in site residence times critically impact the overall ionic conductivity. In alpha-LZCs, lithium ions prefer to anisotropically diffuse across interlayers as the result of a lower energy barrier, driven primarily by collective diffusion. In contrast, lithium ions in beta-LZC primarily isotropically diffuse within the intralayer, hindered by higher energy barriers and determined by individual diffusion. The variation in ZrCl6 2- octahedral unit softening, induced by the specific layered arrangement of zirconium atoms, emerges as a critical determinant of the energy barriers across the LZC phases. These atomic-scale insights into the transport processes provide valuable guidance for the rational design and optimization of LZCs-based electrolytes, accelerating their practical application in advanced energy storage technologies.

Guo, Hanzeng↗

Survival of itinerant excitations and quantum spin state transitions in YbMgGaO 4 with chemical disorder

A recent focus of quantum spin liquid (QSL) studies is how disorder/randomness in a QSL candidate affects its true magnetic ground state. The ultimate question is whether the QSL survives disorder or the disorder leads to a “spin-liquid-like” state, such as the proposed random-singlet (RS) state. Since disorder is a standard feature of most QSL candidates, this question represents a major challenge for QSL candidates. YbMgGaO 4 , a triangular lattice antiferromagnet with effective spin-1/2 Yb 3+ ions, is an ideal system to address this question, since it shows no long-range magnetic ordering with Mg/Ga site disorder. Despite the intensive study, it remains unresolved as to whether YbMgGaO 4 is a QSL or in the RS state. Here, through ultralow-temperature thermal conductivity and magnetic torque measurements, plus specific heat and DC magnetization data, we observed a residual κ 0 /T term and series of quantum spin state transitions in the zero temperature limit for YbMgGaO 4 . These observations strongly suggest that a QSL state with itinerant excitations and quantum spin fluctuations survives disorder in YbMgGaO 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Toward a Photomagnetic Mechanism for f-element separations (Final Technical Report)

The intent behind this proposal was to evaluate magnetic field effects of rare-earth ions on radical pairs. Rare-earth ions are notoriously challenging to separate based on similar thermodynamic characteristics (e.g. solubility) or ion radius, whereas magnetism varies starkly from rare-earth to rare-earth, even when ions are immediately adjacent on the periodic table. Magnetism could be a useful property then for separations, but a mechanism that is effective and selective for magnetic characteristics must be produced. A reactive mechanism for separations could likewise be interesting for selective separations, if a magnetic handle for such a separation could be defined. This proposal sought to understand a specific reactive, magnetic handle for a reactive separations scheme by creating proof of concept model complexes that place rare earths in proximity to photochemically active functional groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In situ microscopy and spectroscopy characterization of microsized Sn anode for sodium-ion batteries

Microsized Sn is a promising anode material for sodium-ion batteries in terms of cost, specific capacity, and volumetric energy density, which however suffers from huge volume changes and rapid cell degradation upon cycling. Despite recent advances via nanostructured electrode design and interface engineering, the correlation between mechanical stability, solid-electrolyte interphase (SEI) and reaction kinetics/reversibility remains controversial and elusive. Here, in this work, by combining in situ scanning electron microcopy and X-ray absorption spectroscopy as well as X-ray photoelectron spectroscopy, we have investigated the underlying electro-chemo-mechanical behavior and their coupling effects during charge/discharge of microsized Sn anode. Our results revealed that microsized Sn is pulverized into nanoparticles with simultaneous formation of numerous voids and pores upon the 1st charge/discharge, while the electrolytes composition plays a critical role on the consequent parasitic reactions and eventually the sodiation/de-sodiation reversibility. In contrast to carbonate-based electrolytes, ether-based electrolytes enabled formation of inorganic species dominated SEI with improved mechanical strength, thus leading to higher specific capacity and improved cycling stability. The present findings are crucial for future development of microsized anode materials for rechargeable batteries with high volumetric energy density.

25 ENERGY STORAGE↗

Origins of magnetic memory and strong exchange bias bordering magnetic compensation in mixed-lanthanide systems

Here, the unexpected physical phenomena resulting from the seemingly inconsequential substitutions of chemically similar lanthanide elements in the Pr 1-x Gd x ScGe system are exploited to further the understanding of rare-earth magnetism and inform materials design. By directly probing magnetic moments of crystallographically indistinguishable Pr and Gd we solve the puzzles of how an unusual magnetic memory and strong exchange bias emerge at specific, easily predictable chemistries. Both effects are rooted in a robust antiparallel arrangement of large 4f magnetic moments of light and heavy lanthanides. This enables precise control of nearly zero net magnetization either opposed to, or aligned with, the external magnetic field that persists over a wide range of temperatures and fields. Further, spontaneous perturbations in the random distribution of lanthanide ions makes strong exchange bias possible in bulk single-phase compounds bordering magnetic compensation, consequently expanding the materials base beyond artificial magnetic multilayers and broadening the range of potential applications of the phenomenon.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Theory-guided experimental design in battery materials research

A reliable energy storage ecosystem is imperative for a renewable energy future, and continued research is needed to develop promising rechargeable battery chemistries. To this end, better theoretical and experimental understanding of electrochemical mechanisms and structure-property relationships will allow us to accelerate the development of safer batteries with higher energy densities and longer lifetimes. This Review discusses the interplay between theory and experiment in battery materials research, enabling us to not only uncover hitherto unknown mechanisms but also rationally design more promising electrode and electrolyte materials. We examine specific case studies of theory-guided experimental design in lithium-ion, lithium-metal, sodium-metal, and all-solid-state batteries. We also offer insights into how this framework can be extended to multivalent batteries. To close the loop, we outline recent efforts in coupling machine learning with high-throughput computations and experiments. Last, recommendations for effective collaboration between theorists and experimentalists are provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗