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All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Chirality reversal at finite magnetic impurity strength and local signatures of a topological phase transition

Here, we study the honeycomb lattice with a single magnetic impurity modeled by adding imaginary next-nearest-neighbor hopping 𝑖⁢ℎ on a single hexagon. This Haldane defect gives a topological mass term to the gapless Dirac cones and generates chirality. For a small density of defects, Neehus et al. [Phys. Rev. Lett. 135, 126604 (2025)] found that the system's chirality reverses at a critical ℎ 𝑐 ≈ 0.95 associated with an unexpected tricritical point of Dirac fermions at zero defect density. We investigate this zero-density limit by analyzing a single defect and computing two experimentally relevant measures of chirality: (1) orbital magnetization via local Chern marker, a bulk probe of all occupied states; and (2) electronic currents of low-energy states. Both probes show a chirality reversal at a critical ℎ 𝑐 ≈ 0.9–1.0. Motivated by this consistency, we propose a defect-scale toy model whose low-energy states reverse their chirality at ℎ$^{'}_{c}$ ≈ 0.87. Remarkably, the same pair of zero-energy bound states also generates the critical point ℎ 𝑐 in the full impurity projected T-matrix. Our results show how the chirality reversal produced by an impurity can be observed either in local probes or in the global topology, and suggest a possible role of the microscopic defect structure at the critical point.

Chern insulators↗
DOE OSTI2025

Cation Crossover Limits Accessible Current Densities for Zero-Gap Alkaline CO2 Reduction to Ethylene

Traditional CO2 reduction systems often fail in an alkaline environment due to the interaction of CO2 with a high-pH electrolyte, where carbonate and bicarbonate ion formation results in potassium-containing salt precipitation. The presence of the salt crystals causes a reduction in the selectivity of the electrolyzer toward CO2 conversion. Here, the critical operational variables, which elicit the salting out process, are investigated (i.e., ion transport). When the electrolyzer exceeds a critical current density, H2 evolution dominates CO2 reduction due to salt formation, which is confirmed by postmortem cross-sectional SEM-EDS of the electrode. The critical current density decreases with an increasing membrane thickness or anolyte ionic strength. Cathode salt formation is mediated by the unmitigated crossover of cations from the anolyte to the cathode across an anion exchange membrane, through which cations are imperfectly excluded. It is likely that electric field-driven migration promotes an increase in concentration of potassium across the membrane, until, at the critical current density for that electrolyzer arrangement, the concentration of potassium and bicarbonate ions exceeds the solubility limit of KHCO3, leading to salt precipitation.

CO2 reduction↗
DOE OSTI2025

Pushing the Limits: Maximizing Energy Density in Silicon Sulfide Solid‐State Batteries

Here, for the first time, we demonstrate a silicon solid-state battery (SSB) architecture that achieves >400 Wh kg −1 , approaching the theoretical limit for silicon-based SSBs. This configuration features a 99.9 wt% micro-Si, a thin sulfide solid electrolyte (SSE), and a high-loading NMC811. Key to these results is strategically selecting and evaluating the processing techniques, whether wet or dry, for the negative electrode, positive electrode and thin sheet-type SSE. Excessive lithium incorporation into the silicon host, beyond the Li 3.75 +Si phase to form a LiSi composite, is essential to match the high capacity of the positive electrode. This SSB achieves over 1000 cycles for a 2 mAh cm −2 with ≈80% capacity retention and 94% capacity retention for 3 mAh cm −2 over 500 cycles at 25 °C. Post analysis identifies the primary capacity decay mechanisms as oxidation at the NMC/SSE interface and structural disruptions within NMC. Meanwhile, the Si electrode maintains a robust solid-electrolyte interphase layer, minimizing capacity decay. This study highlights the necessity for improved NMC coatings, lattice oxygen stabilization, and a durable positive electrode-electrolyte interface to improve the long-term stability of SSBs. Strategies leading to a single-layer pouch cell SSB exceeding 400 Wh kg −1 are developed.

25 ENERGY STORAGE↗
DOE OSTI2025

Extending the Mott–Gurney law to one-dimensional nonplanar diodes using point transformations

Recent studies have applied variational calculus, conformal mapping, and point transformations to generalize the one-dimensional (1D) space-charge limited current density (SCLCD) and electron emission mechanisms to nonplanar geometries; however, these assessments have focused on extending the Child–Langmuir law (CLL) for SCLCD in vacuum. Since the charge in the diode is independent of the coordinate system (i.e., covariant), we apply bijective point transformations to extend the Mott–Gurney law (MGL) for the SCLCD in a collisional or semiconductor gap to nonplanar 1D geometries. This yields a modified MGL that replaces the Cartesian gap distance with a canonical gap distance that may be written generally in terms of geometric scale factors that are known for multiple geometries. We tabulate results for common geometries. Such an approach may be applied to any current density, including non-space-charge limited gaps and SCLCD that may fall between the CLL and MGL.

Garner, Allen L. [Purdue Univ., West Lafayette, IN↗
DOE OSTI2024

Pathway to High Rate Capability in Interconnected Composite Electrolytes: A Case Study with a Single-Ion-Conducting Polymer

In a three-dimensional interconnected polymer/ceramic composite electrolyte (3D composite), both the polymer and ceramic electrolyte phases are individually connected with a polymer-rich surface layer to provide conformal contact with the electrodes. This work investigates how the transference number of the polymer phase affects the electrochemical properties of the 3D composite. Here, we fabricate a 3D composite using a “single-ion” conducting polymer electrolyte (PE), Li 1+x+y Al x Ti 2–x Si y P 3–y O 12 (LICGC) ceramic, and compare its electrochemical properties with the neat polymer, and with a 3D composite made with a dual-ion-conducting PE (we reported previously). Our results reveal that changing the polymer phase from a dual-ion-conducting PE to a single-ion-conducting PE results in a 9-fold increase in the limiting current density, although the interfacial impedance between the polymer and LICGC ceramic remains high (and contributes significantly to the total impedance of the 3D composite). Further, the limiting current density of the 3D composite is dictated by the PE and minimally affected by the ceramic scaffold. The ceramic scaffold, however, helps to ease the concentration gradient buildup within the PE and moderately improves the overall transference number. The LICGC scaffold does not provide any additional Li dendrite resistance due to its high reactivity with Li.

25 ENERGY STORAGE↗
DOE OSTI2026

Universal Relationship between Limiting Current and Electrochemical Transport Properties in Malonate-Based Polymer Electrolytes

There is considerable interest in developing high-performance electrolytes for rechargeable lithium batteries. For practical applications, the electrolyte must support large dc currents. However, the parameters most often reported in the literature, conductivity, κ, and current fraction, ρ + , reflect ion transport in the limit of infinitesimal currents. In this limit, the efficacy of an electrolyte is given by the product κρ + . The limiting current density, i lim , is the maximum current density that can be applied across an electrolyte; the cell voltage diverges if the applied current density exceeds ilim. This parameter reflects ion transport in the limit of large dc currents and is therefore of practical interest. It would therefore be convenient if i lim could be predicted from measurements of κρ + . In order to explore this possibility, we studied six malonate-based polymers and PEO at a fixed salt concentration (r = 0.08) and temperature (90°C) using symmetric cells with planar electrodes. Unfortunately, there is no correlation between ilim and κρ + . When the applied current density, i, is less than ilim, the cell voltage approaches a stable plateau, ϕ plateau . Here, we found a linear dependence between i and thickness-normalized plateau potential, ϕ plateau L –1 , irrespective of the magnitude of the applied current. In all seven polymer electrolytes, we found a linear correlation between ilim and the slopes of these lines, σ. In other words, measurements of σ can be used to predict the limiting current.

Jana, Rounak [Lawrence Berkeley National Laborator↗
DOE OSTI2025

Porous and Amorphous Mn x Mo 3 S 13 Chalcogel Electrode for High-Capacity Conversion-Based Lithium-Ion Batteries

While Li-ion batteries (LIBs) are a leading energy storage technology, their energy densities are limited by the low capacity of conventional intercalation cathodes, driving interest in high energy-density Li–S batteries that make use of conversion chemistry. Achieving high capacity, reversibility, and cycle stability, and controlling volume changes in conversion batteries during the charge–discharge process, however, remains challenging. Here, in this study, we present a porous, amorphous, sulfide-based Mn x Mo 3 S 13 chalcogel, which concurrently offers high capacity and cycle stability. The solution-processable room temperature synthesized Mn x Mo 3 S 13 (x = 0.25) chalcogel exhibits a local structure that resembles the Mo 3 S 13 cluster with Mn 2+ distributed across the Mo 3 S 13 matrix, as determined by synchrotron X-ray pair distribution function (PDF) and extended X-ray absorption fine structure (EXAFS). Ab initio molecular dynamics (AIMD) simulations reveal that Mn 2+ incorporation shortens the polysulfide chain in the gel matrix compared to the Mo 3 S 13 chalcogel, while forming a coordination environment with disulfide groups, analogous to the experimental findings. A Li/Mn 0.25 Mo 3 S 13 half-cell delivers 897 mAh g –1 capacity during the first discharge and retains 571 mAh g –1 capacity after 100 cycles at a C/3 rate. Distribution of relaxation time (DRT) unveils a stable solid–electrolyte interphase (SEI) formation upon cycling that enables charge–discharge reversibility. Here, the enhanced capacity retention and cycle stability compared to those of the Li/Mo 3 S 13 cell are attributed to the reduced dissolution of active mass into the electrolyte, facilitated by the formation of shorter polysulfide chains within the Mn 0.25 Mo 3 S 13 structure and the strong affinity of Lewis-acidic Mn 2+ for polysulfide anions generated during the charge–discharge process of the Li/Mn 0.25 Mo 3 S 13 cell. Thus, this work illustrates a design principle of material for high-capacity and cycle-stable Li-metal sulfide batteries.

25 ENERGY STORAGE↗
DOE OSTI2026

Ferroelectric Fractals: Switching Mechanism of Wurtzite AlN

The advent of wurtzite ferroelectrics is enabling new ferroelectric devices for computer memory that have the potential to bypass the von Neumann bottleneck due to their robust polarization and silicon compatibility. However, the atomistic switching mechanism of wurtzites is still undetermined due to the limitations of density functional theory simulation size and experimental temporal and spatial resolution. Thus, physics-informed materials engineering to reduce coercive field and breakdown in these devices has been limited. In this work, the atomistic mechanism of domain wall migration and domain growth in aluminum nitride-based wurtzites is uncovered using molecular dynamics and Monte Carlo simulations. We reveal the anomalous switching mechanism of fast 1D single columns of atoms propagating from a slow-moving 2D fractallike domain wall. We find that the critical nucleus is a single aluminum ion that breaks its bond with one nitrogen and bonds to another nitrogen; this creates a cascade that flips atoms directly only in the same column, due to the extreme locality (sharpness) of the domain walls in wurtzites. We further show how the fractallike shape of the domain wall in the 2D plane breaks assumptions in the Kolmogorov, Avrami, and Ishibashi (KAI) model and leads to the anomalously fast switching in wurtzite structured ferroelectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Viability of Additively Manufactured Electrodes for Lithium-Ion Batteries

As the global economy becomes increasingly electrified, the demand for batteries and energy storage is expected to rise significantly, particularly in the transportation and electricity sectors. Lithium-ion batteries (LIBs) are currently the most advanced and widely used technology in this field. Traditionally, LIBs are manufactured using simple 2D planar geometries to maximize production efficiency and minimize costs. However, this approach limits energy density due to the restricted design flexibility of the electrodes. Additive manufacturing (AM) offers a promising solution to enhance the energy density and efficiency of LIBs by enabling the design of architectures that reduce diffusive losses and allow for a greater amount of active material to be incorporated within the same device footprint, thereby minimizing the use of inactive materials. Different AM techniques come with their own set of limitations, including printing speed, material compatibility, and scale, which must be considered when designing electrodes. Scalable and cost-effective methods are particularly important for electric vehicle batteries, while achieving higher energy densities in microbatteries is crucial for the miniaturization of wearable electronics and medical devices. Here, in this study, we simulate various 3D porous electrode designs for LIBs using graphite and nickel manganese cobalt oxide (NMC) electrodes. These designs are selected to represent structures that could be produced using different AM techniques, such as direct ink writing, fused deposition modeling, and stereolithography. Our results indicate that at higher charging rates and increased areal mass loading, 3D structures can outperform traditional 2D electrodes, although the benefits may diminish with more complex designs that are harder to manufacture. The observed gains in energy density are attributed to improved electrode utilization and reduced diffusive energy losses. This comprehensive analysis of structure–performance relationships will provide valuable insights to guide future research on 3D designs, material selection, and AM techniques for additively manufactured battery electrodes.

25 ENERGY STORAGE↗
DOE OSTI2024

Frontiers in Magnetic Materials

Magnetism is crucial to many modern technologies, a driver for condensed matter physics research and one of the most remarkable and diverse properties of matter. We propose to develop understanding of novel magnetism and magnetic related behavior in materials and use this to accelerate the discovery of forefront magnetic materials. The approach is via the connection of magnetic properties to specific structures and materials. Topics that will be addressed are (1) Metallic magnetic materials with unusually low carrier concentrations and/or moments (2) Magnetism arising from unusual chemistry including 4d and 5d magnetism and (3) Materials with strong spin-fluctuations, which can lead to quantum criticality, spin-fluctuation induced superconductivity and other novel quantum behavior. These topics overlap, for example, the 4d ruthenates include ferromagnets (perovskite SrRuO 3 ), extremely high ordering temperature antiferromagnets (honeycomb lattice SrRu 2 O 6 ) and well as quantum materials with strong spin fluctuations (layered perovskite Sr 2 RuO 4 and Sr 3 Ru 2 O 7 ). We will use of density calculations to connect magnetic properties with chemistry and structure and employ phenomenological theories to extend these results to properties that are not directly given by direct first principles methods and we will conduct tests to explore the limitations of density functional approximations and new functionals.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Molecular Layer Deposited Aluminum‐Based Hybrid Resist for High‐Resolution Nanolithography and Direct Ultra‐High Aspect Ratio Pattern Transfer

Inorganic-containing hybrid photoresists are critical for next-generation extreme ultraviolet (EUV) lithography and angstrom-era semiconductor miniaturization. However, associated conventional solution processing struggles to achieve ultrathin, uniform films with high conformality and compositional control, limiting overall patterning performance. Here, this study reports the systematic lithographic patterning characterization of an Al-based hybrid resist synthesized via vapor-phase molecular layer deposition (MLD), using the trimethylaluminum (TMA) metal precursor and the hydroquinone (HQ) aromatic organic linker. The resist supports both sub-20 nm high-resolution nanolithography and virtually infinite silicon plasma etch selectivity. Lithographic performance studied using electron beam lithography (EBL) as a proxy for EUV shows that, under an optimized process adopting post-exposure bake, the resist achieves the best resolution of 15.4 nm linewidth under stringent 1:1 line-space high-density patterning—limited only by the minimum beam size of the EBL system. The resist also shows wide dose latitude and balanced performance in resolution, roughness, and sensitivity. The infinite silicon etch selectivity, stemming from spontaneous aluminum oxyfluoride passivation layer formation, enables fabrication of micrometer-tall, 40 nm-wide silicon nanofin structures using only a ≈30 nm-thick resist layer, without no hard mask. These results highlight the potential of MLD-based hybrid resists for developing next-generation resist materials for micro/nanoelectronics manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Theoretical Assessment of the Transition Between Electron Emission Mechanisms for Nonplanar Diodes

Theoretically and computationally describing the operation of nanodiodes requires characterizing the transitions between multiple electron emission mechanisms for nanodiodes with complicated geometries. This motivates our development of techniques to determine when simplified theories for individual mechanisms suffice compared to more complete, but more computationally expensive, models. Leveraging recent theories that define a canonical gap distance to translate planar theory to nonplanar diodes, we derive the conditions for the transitions among thermal emission, field emission, and space-charge-limited current density (SCLCD) in vacuum and with collisions for non-Cartesian coordinate systems, including spherical, cylindrical, and prolate spheroidal coordinate systems. Particle-in-cell (PIC) simulations of the current density as a function of applied voltage for a tip-to-plate geometry in vacuum agreed qualitatively with the asymptotes for thermal emission at low voltage and SCLCD at higher voltage using the canonical gap distance. As a result, this demonstrates the utility of this approach for guiding system design and suggests future extensions to save simulation time for more realistic geometries that are more computationally expensive.

Conformal mapping↗
DOE OSTI2026

Hypochlorite Redox Chemistry Enables High-Voltage and High-Power Saltwater Batteries

Saltwater batteries (SWBs) are promising alternatives to lithium-ion batteries for large-scale stationary energy storage. However, the performance of conventional oxygen redox-based saltwater battery systems is often constrained by sluggish oxygen evolution and reduction reactions (OER/ORR) at the cathode, leading to low voltage efficiency and limited power density. Here, OER and ORR are replaced by hypochlorite-based redox reactions through the introduction of sodium hypochlorite into saltwater. Operando pH and dissolved oxygen measurements confirm that OER and ORR are minimized and that hypochlorite redox reactions dominate the cathode behavior. Owing to the higher operating potential and faster reaction kinetics, the hypochlorite-redox-based SWBs delivers a higher discharge voltage of 3.3 V and reduced charge-discharge voltage polarization to 0.66 V. Further improvement is achieved by adjusting the saltwater pH to near-neutral conditions, increasing the discharge voltage to 3.5 V and more than doubling the peak power. The hypochlorite redox environment also exhibits chemical stability with key cell components, including the solid electrolyte and cathode current collectors. Operation of series-connected cells and cells employing hard carbon anodes demonstrates scalability and compatibility with alternative anode materials. These results provide a strong foundation for next-generation SWBs targeting large-scale stationary energy storage applications.

Go, Wooseok [ORNL]↗
DOE OSTI2025

Liquid Metals for Advanced Batteries: Recent Progress and Future Perspective

ABSTRACT The shift toward sustainable energy has increased the demand for efficient energy storage systems to complement renewable sources like solar and wind. While lithium‐ion batteries dominate the market, challenges such as safety concerns and limited energy density drive the search for new solutions. Liquid metals (LMs) have emerged as promising materials for advanced batteries due to their unique properties, including low melting points, high electrical conductivity, tunable surface tension, and strong alloying tendency. Enabled by the unique properties of LMs, four key scientific functions of LMs in batteries are highlighted: active materials, self‐healing, interface stabilization, and conductivity enhancement. These applications can improve battery performance, safety, and lifespan. This review also discusses current challenges and future opportunities for using LMs in next‐generation energy storage systems. image

Zheng, Tianrui [Materials Science and Engineering ↗
DOE OSTI2025

Balmer emission measurements in JET-ILW hydrogen, deuterium, tritium and deuterium-tritium low-confinement mode plasmas

Measurements of Balmer-alpha (B-α) and Balmer-gamma (B-γ), where B = H, D, or T isotopes of hydrogen, emission across the low-field side (LFS) divertor in JET ITER-like Wall (ILW), low-confinement mode (L-mode) plasma indicate that the divertor plasma was more strongly detached in deuterium, tritium and deuterium–tritium than in hydrogen plasmas. These measurements are consistent with the lower degree of detachment in hydrogen versus tritium plasmas inferred from Langmuir probes (Groth et al., 2023). The ratio of B-γ to B-α is a suitable indicator of high density/low temperature conditions because B-α emission is dominated by electron impact excitation with a small electron–ion recombination component regardless of electron temperature and density (for conditions in tokamak plasmas) whilst for B-γ the recombination component increases and the excitation component decreases as the electron temperature decreases and the electron density increases. Within the uncertainty of the measurements, the electron density at the low-field side separatrix and the power crossing the separatrix are similar to permit these comparisons. The B-©/B-α ratio is well correlated with the onset of detachment as measured by Langmuir probes (McCracken et al., 1998; Groth et al., 2023). The ratios of B-γ and B-α varied between 0.005 and 0.035 for low-recycling, high-recycling and partially detached conditions, and were 60–70 % higher in partially detached hydrogen than in tritium plasmas. In contrast, the difference between deuterium, tritium and 40–60 % deuterium–tritium is within 10 % and thus within the uncertainties of the measurements. Profiles of the B-α and B-γ emission was measured with two filtered CCDs connected to the visible lost light leg of JET’s mirror link spectroscopy system (Meigs et al., 2010; Lomanowski et al., 2014). Spatially (radial) narrower B-α profiles were measured with increasing isotope mass, while similarly broadened B-γ profiles were measured.

Balmer↗
DOE OSTI2025

High-Energy, High-Power Sodium-Ion Batteries from a Layered Organic Cathode

Sodium-ion batteries (SIBs) attract significant attention due to their potential as an alternative energy storage solution, yet challenges persist due to the limited energy density of existing cathode materials. In principle, redox-active organic materials can tackle this challenge because of their high theoretical energy densities. However, electrode-level energy densities of organic electrodes are compromised due to their poor electron/ion transport and severe dissolution. Here, we report the use of a low-bandgap, conductive, and highly insoluble layered metal-free cathode material for SIBs. It exhibits a high theoretical capacity of 355 mAh g –1 per formula unit, enabled by a four-electron redox process, and achieves an electrode-level energy density of 606 Wh kg –1 electrode (90 wt % active material) along with excellent cycling stability. It allows for facile two-dimensional Na+ diffusion, which enables a high intrinsic rate capability. Growth of the active cathode material in the presence of as little as 2 wt % carboxyl-functionalized carbon nanotubes improves charge transport and charge transfer kinetics and further enhances the power performance. Altogether, these allow the construction of SIB cells built from an affordable, sustainable organic small molecule, which provide a cathode energy density of 472 Wh kg –1 electrode when charging/discharging in 90 s and a top specific power of 31.6 kW kg –1 electrode .

36 MATERIALS SCIENCE↗
DOE OSTI2026

Carbon nanodot precursors enable ultrahigh-loading copper single-atom catalysts for oxygen reduction reaction

Single-atom catalysts (SACs) have attracted significant attention in electrocatalysis due to their high metal utilization and tunable electronic structures; however, their practical implementation is often limited by poor atomic dispersion, low metal loadings (typically < 1 wt%), and insufficient anchoring of single metal atoms on catalyst supports. Herein, we report a simple and versatile strategy to synthesize copper single-atom catalysts (Cu-SACs) with ultrahigh metal loading using citric-acid-derived carbon nanodots as metal-capturing precursors. Through hydrothermal treatment followed by pyrolysis in the presence of urea, atomically dispersed copper atoms coordinated with nitrogen are incorporated into a carbon framework, achieving a Cu loading of up to 20 wt% while maintaining atomic dispersion. Notably, a significant fraction of the copper single atoms exists as Cu+–N2 coordination, which provides under-coordinated and catalytically active sites. The resulting Cu-SAC exhibits promising oxygen reduction reaction (ORR) activity in alkaline media, delivering a limiting current density comparable to that of commercial 20 wt% Pt/C with a predominant four-electron reduction pathway. Despite this high intrinsic activity, durability tests reveal gradual performance degradation under prolonged electrochemical operation, which is attributed to demetallation and aggregation of copper single atoms into metallic nanoparticles. These results demonstrate the potential of carbon nanodot-based platforms for synthesizing high-loading SACs, while underscoring the critical need to simultaneously control carbon porosity and metal–nitrogen coordination to enhance active-site accessibility and durability.

Sharma, Prakhar [University of Kentucky]↗
DOE OSTI2025

Electrostatic limits on charge selectivity in ultrahigh charge density polymer membranes

Ion-exchange membranes (IEMs) with ultrahigh charge densities offer the promise of enhanced ion transport for electrochemical technologies, yet the fundamental limits of this membrane design strategy are not yet understood. In this work, we present a systematic study of bis(1-vinyl-3-imidazolium) cross-linked polymer membranes with fixed charge contents ranging from 6 to 9 mol/L[dry polymer], synthesized to isolate the effects of charge density at constant membrane water content. While ionic conductivity increases monotonically with increasing charge density, a sharp decline in charge selectivity is observed for the most densely charged membranes, defying conventional expectations. Structural, thermal, and mechanical analyses reveal a critical onset of network disruption and anomalous ion partitioning behavior in these densely charged membranes. With proper consideration of cross-linker geometry, these results are interpreted using Manning's counter-ion condensation theory, which suggests that closely packed charged cross-linkers amplify inter-chain electrostatic interactions and trigger excess counter-ion condensation. Our findings suggest that, beyond a threshold spacing between fixed charges, increased functionalization may harm rather than help charge selectivity of IEMs.

36 MATERIALS SCIENCE↗