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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Laser-Induced Cooperative Transition in Molecular Electronic Crystal

The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm -2 , 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge–spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge–spin–lattice decoupling to activate and subsequently stabilize nonequilibrium phase. Finally, the cooperativity triggered by ultrahigh-strain-rate (above 10 6 s -1 ) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Direct Chemical Vapor Deposition Synthesis of Porous Single-Layer Graphene Membranes with High Gas Permeances and Selectivities

Single-layer graphene containing molecular-sized in-plane pores is regarded as a promising membrane material for high-performance gas separations due to its atomic thickness and low gas transport resistance. However, typical etching-based pore generation methods cannot decouple pore nucleation and pore growth, resulting in a trade-off between high areal pore density and high selectivity. In contrast, intrinsic pores in graphene formed during chemical vapor deposition are not created by etching. Therefore, intrinsically porous graphene can exhibit high pore density while maintaining its gas selectivity. Here in this work, the density of intrinsic graphene pores is systematically controlled for the first time, while appropriate pore sizes for gas sieving are precisely maintained. As a result, single-layer graphene membranes with the highest H 2 /CH 4 separation performances recorded to date (H 2 permeance > 4000 GPU and H 2 /CH 4 selectivity > 2000) are fabricated by manipulating growth temperature, precursor concentration, and non-covalent decoration of the graphene surface. Moreover, it is identified that nanoscale molecular fouling of the graphene surface during gas separation where graphene pores are partially blocked by hydrocarbon contaminants under experimental conditions, controls both selectivity and temperature dependent permeance. Overall, the direct synthesis of porous single-layer graphene exploits its tremendous potential as high-performance gas-sieving membranes.

chemical vapor deposition↗
DOE OSTI2022

Unraveling Thermodynamic and Kinetic Contributions to the Stability of Doped Nanocrystalline Alloys using Nanometallic Multilayers

Abstract Targeted doping of grain boundaries is widely pursued as a pathway for combating thermal instabilities in nanocrystalline metals. However, certain dopants predicted to produce grain‐boundary‐segregated nanocrystalline configurations instead form small nanoprecipitates at elevated temperatures that act to kinetically inhibit grain growth. Here, thermodynamic modeling is implemented to select the Mo–Au system for exploring the interplay between thermodynamic and kinetic contributions to nanostructure stability. Using nanoscale multilayers and in situ transmission electron microscopy thermal aging, evolving segregation states and the corresponding phase transitions are mapped with temperature. The microstructure is shown to evolve through a transformation at lower homologous temperatures (<600 °C) where solute atoms cluster and segregate to the grain boundaries, consistent with predictions from thermodynamic models. An increase in temperature to 800 °C is accompanied by coarsening of the grain structure via grain boundary migration but with multiple pinning events uncovered between migrating segments of the grain boundary and local solute clustering. Direct comparison between the thermodynamic predictions and experimental observations of microstructure evolution thus demonstrates a transition from thermodynamically preferred to kinetically inhibited nanocrystalline stability and provides a general framework for decoupling contributions to complex stability transitions while simultaneously targeting a dominant thermal stability regime.

25 ENERGY STORAGE↗
DOE OSTI2022

Tuning Organic Electrochemical Transistor Threshold Voltage using Chemically Doped Polymer Gates

Organic electrochemical transistors (OECTs) have shown promise as transducers and amplifiers of minute electronic potentials due to their large transconductances. Tuning the OECT threshold voltage is important to achieve low-powered devices with amplification properties within the desired operational voltage range. However, traditional design approaches have struggled to decouple channel and materials properties from threshold voltage, thereby compromising on several other OECT performance metrics, such as electrochemical stability, transconductance, and dynamic range. In this work, simple solution-processing methods are utilized to chemically dope polymer gate electrodes, thereby controlling their work function, which in turn tunes the operation voltage range of the OECTs without perturbing their channel properties. Chemical doping of initially air-sensitive polymer electrodes further improves their electrochemical stability in ambient conditions. Thus, OECTs that are simultaneously low-powered and electrochemically resistant to oxidative side reactions under ambient conditions are demonstrated. Furthermore, this approach shows that threshold voltage, which is once interwoven with other OECT properties, can in fact be an independent design parameter, expanding the design space of OECTs.

chemical doping↗
DOE OSTI2022

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi 2 Te 4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi 2 Te 4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. Here, by quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2022

ECRAM Materials, Devices, Circuits and Architectures: A Perspective

Abstract Non‐von‐Neumann computing using neuromorphic systems based on two‐terminal resistive nonvolatile memory elements has emerged as a promising approach, but its full potential has not been realized due to the lack of materials and devices with the appropriate attributes. Unlike memristors, which require large write currents to drive phase transformations or filament growth, electrochemical random access memory (ECRAM) decouples the “write” and “read” operations using a “gate” electrode to tune the conductance state through charge‐transfer reactions, and every electron transferred through the external circuit in ECRAM corresponds to the migration of ≈1 ion used to store analogue information. Like static dopants in traditional semiconductors, electrochemically inserted ions modulate the conductivity by locally perturbing a host's electronic structure; however, ECRAM does so in a dynamic and reversible manner. The resulting change in conductance can span orders of magnitude, from gradual increments needed for analog elements, to large, abrupt changes for dynamically reconfigurable adaptive architectures. In this in‐depth perspective, the history of ECRAM, the recent progress in devices spanning organic, inorganic, and 2D materials, circuits, architectures, the rich portfolio of challenging, fundamental questions, and how ECRAM can be harnessed to realize a new paradigm for low‐power neuromorphic computing are discussed.

Talin, A. Alec↗
DOE OSTI2024

Redox Gating for Colossal Carrier Modulation and Unique Phase Control

Redox gating, a novel approach distinct from conventional electrolyte gating, combines reversible redox functionalities with common ionic electrolyte moieties to engineer charge transport, enabling power-efficient electronic phase control. This study achieves a colossal sheet carrier density modulation beyond 10 16 cm -2 , sustainable over thousands of cycles, all within the sub-volt regime for functional oxide thin films. The key advantage of this method lies in the controlled injection of a large quantity of carriers from the electrolyte into the channel material without the deleterious effects associated with traditional electrolyte gating processes such as the production of ionic defects or intercalated species. The redox gating approach offers a simple and practical means of decoupling electrical and structural phase transitions, enabling the isostructural metal-insulator transition and improved device endurance. The versatility of redox gating extends across multiple materials, irrespective of their crystallinity, crystallographic orientation, or carrier type (n- or p-type). This inclusivity encompasses functional heterostructures and low-dimensional quantum materials composed of sustainable elements, highlighting the broad applicability and potential of the technique in electronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Beyond Conventional Charge Density Wave for Strongly Enhanced 2D Superconductivity in 1H‐TaS 2 Superlattices

Noncentrosymmetric transition metal dichalcogenide (TMD) monolayers offer a fertile platform for exploring unconventional Ising superconductivity (SC) and charge density waves (CDWs). However, the vulnerability of isolated monolayers to structural disorder and environmental oxidation often degrade their electronic coherence. Herein, an alternative approach is reported for fabricating stable and intrinsic monolayers of 1H-TaS2 sandwiched between SnS blocks in a (SnS) 1.15 TaS 2 van der Waals (vdW) superlattice. The SnS block layers not only decouple individual 1H-TaS 2 sublayers to endow them with monolayer-like electronic characteristics, but also protect the 1H-TaS 2 layers from electronic degradation. The results reveal the characteristic 3 × 3 CDW order in 1H-TaS 2 sublayers associated with electronic rearrangement in the low-lying sulfur p band, which uncovers a previously undiscovered CDW mechanism rather than the conventional Fermi surface-related framework. Additionally, the (SnS) 1.15 TaS 2 superlattice exhibits a strongly enhanced Ising-like SC with a layer-independent T c of ≈3.0 K, comparable to that of the isolated monolayer 1H-TaS 2 sample, presumably attributed to their monolayer-like characteristics and retained Fermi states. These results provide new insights into the long-debated CDW order and enhanced SC of monolayer 1H-TaS 2 , establishing bulk vdW superlattices as promising platforms for investigating exotic collective quantum phases in the 2D limit.

2D superconductivity↗
DOE OSTI2024

A Fluoride-Rich Solid-Like Electrolyte Stabilizing Lithium Metal Batteries

To address the problems associated with Li metal anodes, a fluoride-rich solid-like electrolyte (SLE) that combines the benefits of solid-state and liquid electrolytes is presented. Its unique triflate-group-enhanced frame channels facilitate the formation of a functional inorganic-rich solid electrolyte interphase (SEI), which not only improves the reversibility and interfacial charge transfer of Li anodes but also ensures uniform and compact Li deposition. Furthermore, these triflate groups contribute to the decoupling of Li + and provide hopping sites for rapid Li + transport, enabling a high room-temperature ionic conductivity of 1.1 mS cm -1 and a low activation energy of 0.17 eV, making it comparable to conventional liquid electrolytes. Consequently, Li symmetric cells using such SLE achieve extremely stable plating/stripping cycling over 3500 h at 0.5 mA cm -2 and support a high critical current up to 2 mA cm -2 . Here, the assembled Li||LiFePO 4 solid-like batteries exhibit exceptional cyclability for over 1 year and a half, even outperforming liquid cells. Additionally, high-voltage cylindrical cells and high-capacity pouch cells are demonstrated, corroborating much simpler processibility in battery assembly compared to all-solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2026

Adsorption-Engineered Hydrocarbon Ionomers for Durable Proton-Exchange Membrane Fuel Cells

Reducing reliance on perfluoroalkyl substances (PFAS) in proton-exchange membrane fuel cells requires hydrocarbon ionomers that combine high performance with long-term durability, a persistent challenge in catalyst-layer design. Here, we identify oxidation-driven ionomer-catalyst interfacial degradation as a dominant failure pathway in hydrocarbon ionomer-bonded cathodes and introduce an adsorption-engineering strategy to overcome this limitation. The comparison of a commercial sulfonated poly(phenylene) (Pemion) with structurally engineered sulfonated poly(fluorene)s demonstrated that electrode durability is governed by the interplay between ionomer adsorption strength and resistance to oxidative degradation on carbon-supported Pt catalysts. A poly(fluorene) ionomer with mobile alkyl sulfonic acid groups forms resilient interfaces, delivering 1.28 A cm−2 at 0.65 V under fully humidified H2/air conditions (80°C and 150 kPaabs), comparable to Pemion. After 90,000 accelerated potential cycles, the poly(fluorene)-bonded cathode exhibits significantly improved durability, with only 29% performance loss compared to 58% for Pemion; further molecular refinement reduces the loss to 17%, approaching that of Nafion-bonded cathodes (14%). These findings establish adsorption-engineered ionomer design that decouples interfacial anchoring from oxidative degradation as a general strategy for achieving durable, high-performance PFAS-free PEM fuel cell electrodes.

08 HYDROGEN↗
DOE OSTI2026

Lewis Acid‐Activated Charge Trapping in Dielectric Polymers for Superior High‐Temperature Electrostatic Energy Storage

Dielectric polymer capacitors are essential for electrostatic energy storage but suffer from charge transport-induced energy losses, particularly at elevated temperatures where thermally activated charge carriers exacerbate conduction. Conventional mitigation strategies rely on introducing heterogeneous interfaces to create charge traps, complicating scalable film fabrication. A homogeneous molecular trapping mechanism would circumvent these complexities, yet remains underexplored. Herein, a charge trapping strategy is devised by modifying the lowest occupied molecular orbitals of dielectric polymers through Lewis acid-base adduct formation. The use of tris(pentafluorophenyl)boron (BCF) as a Lewis acidic molecular additive introduces deeper charge traps in commercial polyetherimide (PEI) while retaining homogeneity. With only 0.5 wt.% loading, the PEI-BCF film exhibits greatly improved breakdown strength, achieving an ultrahigh discharged energy density of 7.3 J cm-3 with excellent cycle stability at 200 °C. This work establishes a facile molecular approach to decoupling charge trapping from heterogeneous interfaces, enabling high-energy-density polymer capacitors operable under extreme thermal conditions.

Fan, Lu↗
DOE OSTI2023

Electronic Coupling of Metal–to–Insulator Transitions in Nickelate–Based Heterostructures

In rare earth nickelates, the metal-to-insulator transition observed as a function of temperature can be described using an electronic and a structural order parameter. The electronic one is linked to the electronic disproportionation observed below the transition temperature and the structural one characterizes the breathing mode that develops in the low temperature phase. Here SmNiO 3 /NdNiO 3 superlattices are grown with insulating LaAlO 3 spacer layers to study the unusual coupling of metal-to- insulator transitions observed at SmNiO 3 /NdNiO 3 interfaces and determine the role of the two order parameters. Temperature-dependent transport measurements reveal that a single unit cell of LaAlO 3 inserted between SmNiO 3 and NdNiO 3 leads to a complete decoupling of the metal-to-insulator transitions suggesting that the order parameter controlling the coupling is the electronic one.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electrically‐Driven Metal‐Insulator Transitions Emerging from Localizing Current Density and Temperature

Negative differential resistance (NDR) is a key electronic response enabling two‐terminal artificial neurons that can be achieved through different physical phenomena, including phase‐homogeneous current density and temperature (electro‐thermal) localizations and spatially‐localized metal‐insulator phase transitions (MITs). These two effects have been observed to occur sequentially in select electrically‐biased transition metal oxides. However, it is unknown why and under what conditions localizing behaviors precede MITs, particularly as a function of device length scale. To this end, the interplay between phase‐homogeneous electro‐thermal localizations and MITs is investigated in a 3D multiphysics simulation of a lateral thin film device, using the material properties of the prototype MIT material VO 2 . These findings demonstrate that the MIT is nucleated through dynamically localizing current density and temperature. A critical device width (≈0.7 µm in this study) is identified, below which both the electrically‐induced electro‐thermal and phase inhomogeneities cease to appear. It is demonstrated that the formation of spatial inhomogeneities directly relates to device dimensions, and demonstrate the decoupling of NDR from the MIT through device scaling relationships. These results provide insight into the material phenomena underlying the material's electrical responses, clarifying conditions under which spatial inhomogeneities form in electrically‐biased MIT materials.

artificial neuron↗
DOE OSTI2023

Grain Boundary Phases in NbFeSb Half‐Heusler Alloys: A New Avenue to Tune Transport Properties of Thermoelectric Materials

Abstract Many thermoelectric materials benefit from complex microstructures. Grain boundaries (GBs) in nanocrystalline thermoelectrics cause desirable reduction in the thermal conductivity by scattering phonons, but often lead to unwanted loss in the electrical conductivity by scattering charge carriers. Therefore, modifying GBs to suppress their electrical resistivity plays a pivotal role in the enhancement of thermoelectric performance, zT . In this work, different characteristics of GB phases in Ti‐doped NbFeSb half‐Heusler compounds are revealed using a combination of scanning transmission electron microscopy and atom probe tomography. The GB phases adopt a hexagonal close‐packed lattice, which is structurally distinct from the half‐Heusler grains. Enrichment of Fe is found at GBs in Nb 0.95 Ti 0.05 FeSb, but accumulation of Ti dopants at GBs in Nb 0.80 Ti 0.20 FeSb, correlating to the bad and good electrical conductivity of the respective GBs. Such resistive to conductive GB phase transition opens up new design space to decouple the intertwined electronic and phononic transport in thermoelectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Probing Electrode Transformation under Dynamic Operation for Alkaline Water Electrolysis

Alkaline water electrolyzers (AWEs) play a pivotal role in the realm of large-scale hydrogen production. However, AWEs face significant challenges in electrode degradation particularly under dynamic operating conditions, induced by reverse current phenomenon during frequent startup/shutdown. Herein, this study aims to rationalize the degradation mechanisms of AWEs under these conditions. A three-electrode membrane electrode assembly (MEA) setup is first utilized to decouple polarization behaviors of anode and cathode in AWEs. Following a proposed accelerated stress testing protocol, the setup allows for tracking individual electrode performance transformations during frequent reverse current operation. Integrating operando cell studies with in situ and post-mortem characterizations, it is showed that continuous formation of highly active species, nickel (oxy)hydroxides, improves the anode performance for oxygen evolution reaction. On the contrary, irreversible oxidation of nickel to β-nickel hydroxide results in a severe degradation of cathode, leading to material dissolution, poor electrical conductivity and loss of catalytic activity for hydrogen evolution reaction. These results provide insights in nickel-based electrode transformation mechanisms for alkaline water electrolysis and indicate that cathode with higher redox reversibility can potentially improve durability of AWEs under dynamic conditions.

08 HYDROGEN↗
DOE OSTI2025

Challenges in Tracking Waste Reduction Performance Improvement in Manufacturing Plants

The recently released Circularity Gap Report 2023 by the Circle Economy Foundation states that the circularity score for the global economy is declining. The US Environmental Protection Agency (EPA) tracked municipal solid waste from 1960 to 2018 and found that 50% of the waste was destined for landfills. EPA estimates that US industry is responsible for 2.7 Gt of solid nonhazardous waste annually in the US mostly linear economy model. The circular economy framework aims to decouple economic value generation from the extraction of virgin materials from nature. The linear model of material extraction and disposal at the end of life is highly unsustainable. Manufacturing companies are adopting ambitious waste reduction targets to achieve sustainability. Through the Better Plants program, US DOE has established the Waste Reduction Network, which offers technical assistance to partners to achieve their ambitious waste reduction goals. Basic requirements of establishing a target include identifying a baseline, quantifying waste performance, and measuring progress over time. One problem faced by industry is unstandardized metrics for quantifying waste performance that may not be well suited to demonstrate progress. This paper studies traditional methods used to measure waste performance and highlights advantages, disadvantages, and limitations of each method. It also examines the suitability of applying the methods in different manufacturing circumstances. Finally, the paper presents a case study of a large manufacturer that faced inconsistencies in its tracked measurement metric. A solution was proposed and implemented to alter the methodology to enable more accurate waste performance tracking against a baseline.

circular economy↗
DOE OSTI2021

Promoting the Furan Ring‐Opening Reaction to Access New Donor–Acceptor Stenhouse Adducts with Hexafluoroisopropanol

Abstract Donor–acceptor Stenhouse adducts (DASAs) are visible‐light‐responsive photoswitches with a variety of emerging applications in photoresponsive materials. Their two‐step modular synthesis, centered on the nucleophilic ring opening of an activated furan, makes DASAs readily accessible. However, the use of less reactive donors or acceptors renders the process slow and low yielding, which has limited their development. We demonstrate here that 1,1,1,3,3,3‐hexafluoro‐2‐propanol (HFIP) promotes the ring‐opening reaction and stabilizes the open isomer, allowing greatly reduced reaction times and increased yields for known derivatives. In addition, it provides access to previously unattainable DASA‐based photoswitches and DASA–polymer conjugates. The role of HFIP and the photochromic properties of a set of new DASAs is probed using a combination of 1 H NMR and UV/Vis spectroscopy. The use of sterically hindered, electron‐poor amines enabled the dark equilibrium to be decoupled from closed‐isomer half‐lives for the first time.

Clerc, Michèle↗