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DOE OSTI2026

Task Sharing of Proton Incorporation in Vertically Aligned Nanocomposite Triple Conductors: Growth, Structure, and Surface Exchange Kinetics

As protonic ceramic electrolysis cells emerge for efficient H 2 production, there is a need to develop air electrode materials enabling fast, durable steam splitting and proton incorporation. Single-phase triple conductors may fail to satisfy the myriad performance/stability requirements, and their critical charge-carriers (holes, oxygen vacancies, and protons) are in competition, limiting their concentrations. Instead, we propose task-sharing, vertically aligned nanocomposites (VANs), comprising a proton conductor (BaZr 0.9 Y 0.1 O 3-δ ) and a redox-active mixed ionic electronic conductor (Ce 0.9 Pr 0.1 O 2-δ ), that may enable rapid proton surface exchange at the solid–gas interface and transport along the solid–solid heterointerfaces. We grew VANs by pulsed laser deposition and investigated the interplay between their processing conditions, structure, and proton and oxygen surface exchange kinetics. We varied the substrate temperature, laser repetition rate, laser fluence, and processing oxygen pressure. The crystallinity and phases were characterized by grazing-incidence X-ray diffraction, and the strain and structural order as a function of depth were evaluated by angle-dependent synchrotron X-ray pair distribution function analysis. To evaluate the potential for interdiffusion, the formation energies of substitutional defects were simulated with density functional theory. Corresponding structural analysis and elemental mapping were performed by scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, and electron energy-loss spectroscopy, indicating distinct nanoscale compositional regions with a hierarchical structure embedded in individual VANs columns and minimal interdiffusion across a bilayer film. Proton and oxygen surface exchange coefficients (k H , k O ) and polarization resistances were evaluated by electrical and optical relaxations and impedance spectroscopy of VAN-incorporated protonic ceramic electrochemical cells, respectively, at 400–500 °C, demonstrating values comparable to some of the best-known triple and mixed conductors.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Epitaxial nanotwinned metals and alloys: synthesis-twin structure–property relations

Extensive studies have been performed to understand the structure–property relationship in nanotwinned (NT) metals, where the average twin thickness or twin spacing is less than 100 nm. NT metals may have high strength, ductility, good electrical conductivity and corrosion resistance and have promising applications in microelectronics, structural materials and coatings for gas and oil industry. Most prior studies focus on the computational and experimental investigations of NT metals with low stacking fault energy (SFE) and often in polycrystalline forms. In this highlight, we review recent findings on epitaxial growth of NT metals and alloys with low and high SFEs deposited on single crystal substrates, and focus primarily on advancing our comprehension towards tailoring the microstructures and properties of NT metals via extrinsic factors, including the synthesis technique, parametric control and growth template, and intrinsic factors, such as SFE and thermodynamic, kinetic alloying effects. The review intends to illuminate how to synthesize and design epitaxial NT structures to achieve desirable properties.

36 MATERIALS SCIENCE↗

DOE OSTI2022

An energy-dependent electro-thermal response model of CUORE cryogenic calorimeter

The Cryogenic Underground Observatory for Rare Events (CUORE) is the most sensitive experiment searching for neutrinoless double-beta decay (0νββ) in 130 Te. CUORE uses a cryogenic array of 988 TeO 2 calorimeters operated at ~10 mK with a total mass of 741 kg. To further increase the sensitivity, the detector response must be well understood. Here, we present a non-linear thermal model for the CUORE experiment on a detector-by-detector basis. We have examined both equilibrium and dynamic electro-thermal models of detectors by numerically fitting non-linear differential equations to the detector data of a subset of CUORE channels which are well characterized and representative of all channels. Further, we demonstrate that the hot-electron effect and electric-field dependence of resistance in NTD-Ge thermistors alone are inadequate to describe our detectors' energy-dependent pulse shapes. We introduce an empirical second-order correction factor in the exponential temperature dependence of the thermistor, which produces excellent agreement with energy-dependent pulse shape data up to 6 MeV. We also present a noise analysis using the fitted thermal parameters and show that the intrinsic thermal noise is negligible compared to the observed noise for our detectors.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Determining the oxidation stability of SnSe under atmospheric exposure

Abstract Understanding surface stability becomes critical as 2D materials like SnSe are developed for piezoelectric and optical applications. SnSe thin films deposited by molecular beam epitaxy showed no structural changes after a two-year exposure to atmosphere, as confirmed by X-ray diffraction and Raman spectroscopy. X-ray photoelectron spectroscopy and reflectivity show a stable 3.5 nm surface oxide layer, indicating a self-arresting oxidative process. Resistivity measurements show an electrical response dominated by SnSe post-exposure. This work shows that SnSe films can be used in ambient conditions with minimal risk of long-term degradation, which is critical for the development of piezoelectric or photovoltaic devices. Graphical Abstract

Chin, Jonathan R. (ORCID:0000000273205678)↗

DOE OSTI2024

UHT-CAMANCHE: Ultra-High Temperature Ceramic Additively Manufactured Compact Heat Exchangers

The conceptual basis for this project is the convergence of advanced ultra-high temperature ceramic materials and additive manufacturing technologies to produce compact ceramic heat exchangers with complex internal flow path geometries. Task areas were broadly divided into materials and manufacturing development, heat exchanger design, component testing, and techno-economic analysis. Technical challenges included the design and commissioning of new test facilities, improving feature resolution and deposition rate of ceramic additive manufacturing techniques, establishing process-structure-property relationships in additively manufactured ultra-high temperature ceramics, and assessing high temperature materials compatibility in CO 2 environments. The primary candidate material evaluated in this work is a composite comprising zirconium diboride (ZrB2) with 30 vol. % silicon carbide (SiC) which was selected based on its desirable combination of high temperature mechanical properties, high thermal and electrical conductivities, and oxidation resistance. High solids loaded ZrB2-SiC pastes suitable for extrusion-based additive manufacturing were developed for the first time as part of this work. Materials compatibility studies indicate this material oxidizes in CO 2 to form a protective borosilicate scale which transforms to pure silica above 1000°C. Parts made by additive manufacturing displayed enlarged grain sizes produced by pressureless sintering as compared to hot-press sintering. Increases in microstructural coarseness have outsized effect on oxidation performance up to 1400°C due to incomplete oxidation of coarse large diameter SiC particles resulting in lower amounts of silica that apparently inhibit protective scale formation. Additive manufacturing as a forming technique did not appear to significantly affect thermal conductivity, hardness, or elastic modulus, though flexural strength was reduced by half or more as compared to traditionally hot-pressed materials. This effect was attributed to the presence of strength-limiting flaws (ca. 40 microns in size) originating from extrudate inhomogeneities that could potentially be eliminated with further process improvements. Attempts to attain economies of scale for production of multi-kilowatt scale heat exchangers by ceramic additive manufacturing proved difficult. Lack of automation and a modest extrusion rate while retaining fine feature resolution made the overall process labor intensive and limited experimental throughput. A number of full-scale components were taken through post-process heat treatments including drying, binder burnout, and sintering; however, none survived without significant flaws or cracks. Therefore, no operational data from a newly installed heat exchanger test loop were able to be obtained during the performance period. Continued research and development is recommended to improve economic feasibility of ceramic additive manufacturing by standardizing the use of advanced sensors, artificial intelligence, and automation tools to reduce associated labor costs and accelerate production rates. The materials and manufacturing techniques demonstrated in this work are likely to find applications in defense and energy applications.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

Ultraefficient resistance switching between charge ordered phases in 1 T -TaS 2 with a single picosecond electrical pulse

Progress in high-performance computing demands significant advances in memory technology. Among novel memory technologies that promise efficient device operation on a sub-ns timescale, resistance switching between charge ordered phases of 1T-TaS 2 has shown to be potentially useful for development of high-speed, energy efficient nonvolatile memory devices. Measurement of the electrical operation of such devices in the picosecond regime is technically challenging and hitherto still largely unexplored. Here, we use an optoelectronic “laboratory-on-a-chip” experiment for measurement of ultrafast memory switching, enabling accurate measurement of electrical switching parameters with 100 fs temporal resolution. Photoexcitation and electro-optic sampling on a (Cd,Mn)Te substrate are used to generate and, subsequently, measure electrical pulse propagation with intra-band excitation and sub-gap probing, respectively. We demonstrate high contrast nonvolatile resistance switching from high to low resistance states of a 1T-TaS 2 device using single sub-2ps electrical pulses. Using detailed modeling, we find that the switching energy density per unit area is exceptionally small, E A =9.4 fJ/μm 2 . Finally, the speed and energy efficiency of an electronic “write” process place the 1T-TaS 2 devices into a category of their own among new generation nonvolatile memory devices.

42 ENGINEERING↗

DOE OSTI2024

Low-Power Characterization and Integration of Carbon Black Resistive Ink for Aerosol Jet-Printed RF Components

Aerosol jet printing (AJP) is gaining attention in additive manufacturing research, especially in the discipline of microwave engineering. Currently, no reliable AJP method exists to fabricate resistors that are both electrically small and with a resistance compatible with waveguide impedances for use in microwave components. In this work, the commercially available Metalon JR-038 is characterized and used to fabricate a resistor that is 100 μ m long by 250 μ m wide for the first time to the best of our knowledge. Furthermore, this resistor was then used to fabricate a Ka-band Wilkinson power divider using only the AJP process.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Electrical edge effect induced photocurrent overestimation in low-light organic photovoltaics

In many literatures, the short-circuit current (J SC ) of indoor organic photovoltaics is overestimated, leading to severely wrong device performance evaluation and analysis. In this work, based on the equivalent circuit model, we demonstrate that electrical edge effect is sensitive to both transverse surface resistance and light intensity. At low light intensity, the electrical edge effect could lead to J SC being significantly overestimated, i.e., by 100% and even more. We show that for a PM6:Y6 device capped with a MoOX layer, when measured under 0.01 sun, the usually overlooked interface doping mechanism would lead to J SC and PCE overestimation by 51% and 15%, respectively. Besides, we show that the magnitude of J SC overestimation drastically increases with high photoactive-layer surface roughness. This work emphasized the significant electrical edge effect on J SC evaluations for low-light solar cells and is conducive to understanding the intrinsic mechanism of edge effect, promoting a healthier development of organic photovoltaics.

14 SOLAR ENERGY↗

DOE OSTI2022

The Third Dimension of Ferroelectric Domain Walls

Abstract Ferroelectric domain walls are quasi‐2D systems that show great promise for the development of nonvolatile memory, memristor technology, and electronic components with ultrasmall feature size. Electric fields, for example, can change the domain wall orientation relative to the spontaneous polarization and switch between resistive and conductive states, controlling the electrical current. Being embedded in a 3D material, however, the domain walls are not perfectly flat and can form networks, which leads to complex physical structures. In this work, the importance of the nanoscale structure for the emergent transport properties is demonstrated, studying electronic conduction in the 3D network of neutral and charged domain walls in ErMnO 3 . By combining tomographic microscopy techniques and finite element modeling, the contribution of domain walls within the bulk is clarified and the significance of curvature effects for the local conduction is shown down to the nanoscale. The findings provide insights into the propagation of electrical currents in domain wall networks, reveal additional degrees of freedom for their control, and provide quantitative guidelines for the design of domain‐wall‐based technology.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Medium- and heavy-duty value of technology improvement

Improvements in vehicle technology impact the purchase price of a vehicle and its operating cost. In this study, the monetary benefit of a technology improvement includes the potential reduction in vehicle price from using cheaper or smaller components, as well as the discounted value of the fuel cost savings. As technology progresses over time, the value and benefit of improving technology varies as well. In this study, the value of improving a few selected technologies (battery energy density, electric drive efficiency, tire rolling resistance, aerodynamics, light weighting) is studied and the value of the associated cost saving is quantified. The change in saving as a function of time, powertrain selection and vehicle type is also quantified. For example, a 10% reduction in aerodynamic losses is worth $24,222 today but only $8,810 in 2030 in an electric long haul truck. The decrease in value is primarily due to expected battery cost reduction over time. The same loss reduction in a 2030 conventional long haul truck is worth $5,117 and is primarily driven by a reduction in diesel expenditure. For conventional vehicles, the value of technology improvement is likely to increase over time as diesel price is expected to increase over the next decades while for electric vehicles, the value of technology improvement is likely to decrease as battery energy density increases and cost decreases. The study focuses on medium- and heavy-duty applications where cost of driving is of paramount importance. The savings realized from each technology improvement serve as an upper limit for how much can be spent to acquire that improvement in technology.

Freyermuth, Vincent↗

DOE OSTI2023

Electrical conductivity of TaO x as function of composition and temperature

The ability to model the resistive switching devices depends on input material parameters and is particularly sensitive to values of electrical conductivity of the functional material as a function of composition and temperature. Here we report the results of conductivity measurements of TaO x with 0 AC ) changing from 0.34 eV at x=2.36 to 0.016 eV at x=1.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Mapping of the transient electric field causing spark suppression in Micromegas of the ATLAS New Small Wheels

Resistive strips Micromegas are employed in the ATLAS New Small Wheel project. They have already been installed and operate in the experimental cavern of the ATLAS experiment at CERN. This work attempts to describe the mechanism of the surface electric charge spread on a resistive strip of the Micromegas detector and the created transient electric field leading to the suppression of the spark rate in the amplification region. The electric field spatial mapping is calculated versus time by using the accurate 3-layer geometry as a function of the resistive layer thickness around its value used in Micromegas detectors. We also used the approximated method based on 2-layer geometry to investigate its discrepancy from the accurate one.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

A hybrid optoelectronic Mott insulator

The coupling of electronic degrees of freedom in materials to create “hybridized functionalities” is a holy grail of modern condensed matter physics that may produce versatile mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition (MIT) is technologically attractive due to the large changes in resistance, tunable by doping, strain, electric fields, and orbital occupancy but not, in and of itself, controllable with light. Here, an alternate approach is presented to produce optical functionalities using a properly engineered photoconductor/strongly correlated hybrid heterostructure. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the intimate proximity between the two materials, the heterostructure exhibits giant volatile and nonvolatile, photoinduced resistivity changes with substantial shifts in the MIT transition temperatures. This approach can be extended to other judicious combinations of strongly correlated materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Characterization of Annealing-Induced Phase Segregation in Composite Silicon Anodes for Li-ion Batteries

Silicon (Si) anodes present a promising alternative to graphite anodes for lithium-ion batteries (LIBs), as Si has a greater specific capacity. However, one major constraint is the volumetric change of Si during lithiation that results in an unstable solid-electrolyte interphase (SEI), so Si-containing electrodes require the use of various strategies to mitigate these effects and improve performance. One such solution is the use of Si nanoparticles (NPs) that maximize the surface area to volume ratio. Here, we discuss electrodes made with Si NPs treated with polyethylene oxide (PEO) (for improving dispersion during processing), conductive carbon NPs, and P84 polyimide binder which shows significant impacts of annealing treatment on improvements of active material utilization, first cycle efficiency, and capacity retention with extensive cycling . We used air-free argon ion polishing to create electrode cross sections and imaged through the electrode thickness using atomic force microscopy (AFM)-based nano-electrical characterization of scanning spreading resistance microscopy (SSRM), nano-mechanical characterizations of contact resonance and force volume (CR-FV), and scanning electron microscopy-based energy dispersive x-ray spectroscopy (SEM-EDS). Results show that the Si and conductive carbon segregate into phases with a distinctive carbon-rich banded morphology that surrounds the Si-rich phase during annealing. In pristine electrodes, the carbon- and SEI-rich bands exhibit a higher electronic conductivity and a lower elastic modulus than the Si active material phase. These structures, as well as distinct electronic and mechanical properties, remain during cycling, suggesting an improvement of electrical conduction pathways and a mechanical strain buffer for active Si material expansion during cycling. This phase separation may be a major factor in the improvement seen in electrochemical performance due to annealing. Additionally, our nm-scale and multi-mode characterizations provide a novel route for understanding and improving energy storage devices, which is advantageous due to the highly inhomogeneous of composite electrodes in nm-mm scales.

ENERGY STORAGE↗

DOE OSTI2020

Enhanced copper–carbon nanotube hybrid conductors with titanium adhesion layer

Cu–carbon nanotube (CNT) hybrids combine the advantages of the high electrical conductivity of Cu with the low temperature coefficient of resistance for CNTs, but require enhanced interfacing to improve the electrical performance when exposed to elevated temperatures. In this work, Ti and Ni were investigated as adhesion metals by thermally evaporating 10 nm layers onto a CNT conductor. SEM analysis shows Ni deposits as discrete nanoscale crystallites which coalesce after annealing to 400 °C in H 2 /Ar. Ti deposits uniformly along the CNT surface and is stable over such temperatures. A 100 nm deposition of Cu is shown to delaminate from the CNTs after annealing, and the resistance per length (R/L) increases by 40%. The Cu–Ni–CNT exhibits a 125% increase, while the Cu–Ti–CNT achieves a 12% decrease in R/L, for similar annealing conditions. Thus, Ti emerges as an effective adhesion metal, warranting its use in metal–CNT wire technologies for elevated temperature operation.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Voltage-controlled magnetic anisotropy enabled by resistive switching

The discovery of new mechanisms of controlling magnetic properties by electric fields or currents furthers the fundamental understanding of magnetism and has important implications for practical use. Here, we present an approach of utilizing resistive switching to control magnetic anisotropy. We study a ferromagnetic oxide that exhibits an electrically triggered metal-to-insulator phase transition producing a volatile resistive switching. The switching occurs in a characteristic spatial pattern, the formation of an insulating barrier perpendicular to the current flow, which results in an unusual ferromagnetic/paramagnetic/ferromagnetic configuration. Further, the formation of this voltage-driven paramagnetic insulating barrier is accompanied by the emergence of a strong uniaxial magnetic anisotropy that overpowers the intrinsic material anisotropy. Our results demonstrate that resistive switching is an effective tool for manipulating magnetic properties. Because resistive switching can be induced in a broad range of materials, our findings could enable a new class of voltage-controlled magnetism systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Mathematical modeling of novel porous transport layer architectures for proton exchange membrane electrolysis cells

Thin foil based porous transport layers (PTLs) that contain highly structured pore arrays have shown promise as anode PTLs in proton exchange membrane electrolysis cells. These novel PTLs, fabricated with advanced manufacturing techniques, produce thin, tunable, multifunctional layers with reduced flow and interfacial resistances and high thermal and electric conductivities. To further optimize their design, it is important to understand their fundamental impact on the transport of protons, electrons, and liquid/vapor mixtures in the electrode. In this work, we develop a two-dimensional multiphysics model to simulate the coupled electrochemistry and multiphase transport in an electrolysis cell operated with the novel PTL architecture. The results show that larger pores improve access of water to the anode catalyst layer, which is beneficial for both the oxygen evolution reaction and membrane hydration. Larger pore sizes also improve oxygen gas transport from the catalyst layer, because generated oxygen gas is forced to travel in-plane through the anode catalyst layer until it reaches a pore opening that is connected to a channel. The discussed results confirm that the proposed thin foil based PTLs are fundamentally different from conventional PTLs, such as felts or layered meshes. The model developed in this work also provides generalizable insight into fundamental PEMEC phenomena, such as the competition between liquid and gas phase transport, membrane hydration and water management, and nonuniform electrochemical reactions, which are processes relevant to all PEMEC designs.

25 ENERGY STORAGE↗

DOE OSTI2025

Methane pyrolysis by Joule heating for graphitic carbon and hydrogen production

The global energy transition toward sustainability requires technologies that can decarbonize energy carriers and fuels while producing valuable materials. Methane, a primary component of natural gas, is both a high-energy-density fuel and a significant greenhouse gas. This study reports an approach for methane pyrolysis utilizing Joule heating within the deposition substrate to drive the endothermic reaction. With electric current passing through a resistive porous carbon cloth, heat is generated to break C-H bonds of methane molecules. Here, the decomposition of methane as it flows through the cloth results in hydrogen production and the formation of conformally layered graphite around the carbon fibers. The effects of input power, chamber pressure, feedstock flow rate, and process duration on hydrogen and graphite production are characterized via in situ mass spectrometry and laser absorption spectroscopy, resulting in methane conversion rates up to 88%, with hydrogen and carbon yields of 82% and 72%, respectively. Material characterization verifies uniform high-quality graphite deposition, with a Raman I D /I G ratio of 0.1 and 3.38 Å d-spacing. This Joule heating method for catalyst-free methane pyrolysis offers the potential for advancing hydrogen production technology by simultaneously producing valuable materials such as solid graphite, thus enhancing the economic viability of the fuel decarbonization process.

Energy Resources↗