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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 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Strong spin–orbit quenching via the product Jahn–Teller effect in neutral group IV qubits in diamond

Abstract Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn, and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers remains elusive. In this context, we predict the ground-state and excited-state properties of the neutral group IV color centers from first principles. We capture the product Jahn–Teller effect found in the excited state manifold to second order in electron–phonon coupling, and present a nonperturbative treatment of the effect of spin–orbit coupling. Importantly, we find that spin–orbit splitting is strongly quenched due to the dominant Jahn–Teller effect, with the lowest optically-active 3 E u state weakly split into m s -resolved states. The predicted complex vibronic spectra of the neutral group IV color centers are essential for their experimental identification and have key implications for use of these systems in quantum information science.

Materials Science↗
DOE OSTI2022

In situ electrochemical recomposition of decomposed redox-active species in aqueous organic flow batteries

Aqueous organic redox flow batteries (AORFBs) offer a safe and potentially inexpensive solution to the problem of storing massive amounts of electricity produced from intermittent renewables. However, molecular decomposition is the major barrier preventing AORFBs from being commercialized. Structural modifications can improve molecular stability at the expense of increased synthetic cost and molecular weight. Utilizing 2,6-dihydroxy-anthraquinone (DHAQ), without further structural modification, we demonstrate that electrochemical regeneration could be a viable route to achieve low-cost, long-lifetime AORFBs. In situ (online) NMR and EPR and complementary electrochemical analyses reveal that decomposition compounds i.e., 2,6-dihydroxy-anthrone (DHA) and its tautomer, 2,6-dihydroxy-anthranol (DHAL), can be converted back to DHAQ in two steps: first DHA(L) 2- are oxidized to the dimer (DHA) 2 4- at - 0.32 V vs. SHE by one-electron transfer; subsequently, the (DHA) 2 4- is oxidized to DHAQ 2- at +0.57 V vs. SHE by three-electron transfer. Electrochemical regeneration rejuvenates not only DHAQ 2- , but also the positive electrolyte – rebalancing the states of charge of both electrolytes without introducing extra ions. We demonstrate the repeated capacity recovery with DHAQ | potassium ferro-/ferricyanide flow battery in basic conditions, and show the approach is also effective for anthraquinone-2,7-disulfonate in acid. Electrochemical regeneration strategies may extend the useful lifetime of many water-soluble organic molecules with anthraquinone core structures in electrochemical cells.

25 ENERGY STORAGE↗
DOE OSTI2023

Nature-inspired methylated polyhydroxybutyrates from C1 and C4 feedstocks

Polyolefin plastics are widely used due to their low cost and outstanding properties, but their environmental persistence presents a major societal challenge. Polyhydroxyalkanoates (PHA) are biodegradable substitutes for polyolefins, but their high cost and thermal instability are impediments to their widespread application. Here we report a series of methylated polyhydroxybutyrates, poly(3-hydroxy-2-methylbutyrate)s, which are structurally inspired by natural PHAs. The cis homopolymers exhibit tacticity-independent crystallinity, which allows for the discovery of high-melting, thermally stable and mechanically tough copolymers, and a full range of polyolefin-like properties can be further achieved by tailoring the cis/trans ratio of the repeating units. Moreover, these materials can be synthesized from inexpensive carbon monoxide and 2-butene feedstocks, and they can be chemically recycled or upcycled at their end of life. As a result, the versatile properties, abundant feedstocks and end-of-life utility of this family of polyesters will enable a powerful platform for the discovery of sustainable alternatives to polyolefin plastics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Stable single-site organonickel catalyst preferentially hydrogenolyses branched polyolefin C–C bonds

Current methods of processing accumulated polyolefin waste typically require harsh conditions, precious metals or high metal loadings to achieve appreciable activities. Here, in this work, we examined supported, single-site organonickel catalysts for polyolefin upcycling. Chemisorption of Ni(COD) 2 (COD, 1,5-cyclooctadiene) onto Brønsted acidic sulfated alumina (AlS) yields a highly electrophilic Ni(I) precatalyst, AlS/Ni(COD) 2 , which is converted under H 2 to the active AlS/Ni II H catalyst. This single-site system exhibits unique hydrogenolysis selectivity that favours cleaving branched polyolefin C–C linkages, enabling the hydrogenolytic separation of polyethylene and isotactic polypropylene (iPP) mixtures. Moreover, AlS/Ni II H remains highly selective and active for hydrogenolysis of iPP admixed with polyvinyl chloride, and the spent catalyst can be repeatedly regenerated by AlEt3 treatment. Experimental mechanistic analysis and density functional theory modelling reveal a turnover-limiting C–C scission pathway featuring β-alkyl transfer and strong olefin binding. These results highlight the potential of nickel-based systems for the selective upcycling of complex plastic waste streams.

green chemistry↗
DOE OSTI2025

Machine learning-accelerated discovery of heat-resistant polysulfates for electrostatic energy storage

The development of heat-resistant dielectric polymers that withstand intense electric fields at high temperatures is critical for electrification. Balancing thermal stability and electrical insulation, however, is exceptionally challenging as these properties are often inversely correlated. A traditional intuition-driven polymer design approach results in a slow discovery loop that limits breakthroughs. Here we present a machine learning-driven strategy to rapidly identify high-performance, heat-resistant polymers. A trustworthy feed-forward neural network is trained to predict key proxy parameters and down select polymer candidates from a library of nearly 50,000 polysulfates. The highly efficient and modular sulfur fluoride exchange click chemistry enables successful synthesis and validation of selected candidates. A polysulfate featuring a 9,9-di(naphthalene)-fluorene repeat unit exhibits excellent thermal resilience and achieves ultrahigh discharged energy density with over 90% efficiency at 200 °C. Its exceptional cycling stability underscores its promise for applications in demanding electrified environments.

Li, He↗
DOE OSTI2021

Fictitious phase separation in Li layered oxides driven by electro-autocatalysis

Layered oxides widely used as lithium-ion battery electrodes are designed to be cycled under conditions that avoid phase transitions. Although the desired single-phase composition ranges are well established near equilibrium, operando diffraction studies on many-particle porous electrodes have suggested phase separation during delithiation. Notably, the separation is not always observed, and never during lithiation. These anomalies have been attributed to irreversible processes during the first delithiation or reversible concentration-dependent diffusion. However, these explanations are not consistent with all experimental observations such as rate and path dependencies and particle-by-particle lithium concentration changes. Here, we show that the apparent phase separation is a dynamical artefact occurring in a many-particle system driven by autocatalytic electrochemical reactions, that is, an interfacial exchange current that increases with the extent of delithiation. We experimentally validate this population-dynamics model using the single-phase material L ix (Ni 1/3 Mn 1/3 Co 1/3 )O 2 (0.5 < x < 1) and demonstrate generality with other transition-metal compositions. Operando diffraction and nanoscale oxidation-state mapping unambiguously prove that this fictitious phase separation is a repeatable non-equilibrium effect. We quantitatively confirm the theory with multiple-datastream-driven model extraction. More generally, our study experimentally demonstrates the control of ensemble stability by electro-autocatalysis, highlighting the importance of population dynamics in battery electrodes (even non-phase-separating ones).

36 MATERIALS SCIENCE↗
DOE OSTI2022

Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries

Intercalation-type metal oxides are promising negative electrode materials for safe rechargeable lithium-ion batteries due to the reduced risk of Li plating at low voltages. Nevertheless, their lower energy and power density along with cycling instability remain bottlenecks for their implementation, especially for fast-charging applications. Here, we report a nanostructured rock-salt Nb 2 O 5 electrode formed through an amorphous-to-crystalline transformation during repeated electrochemical cycling with Li + . This electrode can reversibly cycle three lithiums per Nb 2 O 5 , corresponding to a capacity of 269 mAh g –1 at 20 mA g –1 , and retains a capacity of 191 mAh g –1 at a high rate of 1 A g –1 . Further, it exhibits superb cycling stability with a capacity of 225 mAh g –1 at 200 mA g –1 for 400 cycles, and a Coulombic efficiency of 99.93%. We attribute the enhanced performance to the cubic rock-salt framework, which promotes low-energy migration paths. Our work suggests that inducing crystallization of amorphous nanomaterials through electrochemical cycling is a promising avenue for creating unconventional high-performance metal oxide electrode materials.

25 ENERGY STORAGE↗
DOE OSTI2025

Encoding hierarchical 3D architecture through inverse design of programmable bonds

The ability to fabricate materials and devices at small scales by design has resulted in tremendous technological progress. However, the need for engineered three-dimensional (3D) nanoscale materials requires new strategies for organizing nanocomponents. Here we demonstrate an inverse design approach for the assembly of nanoparticles into hierarchically ordered 3D organizations using DNA voxels with directional, addressable bonds. By identifying intrinsic symmetries in repeating mesoscale structural motifs, we prescribe a set of voxels, termed a mesovoxel, that are assembled into target 3D crystals. The relationship between different degrees of encoded information used for voxel bonds and the fidelity of assembly is investigated using experimental and computational methods. We apply this assembly strategy to create periodic 3D nanoparticle ordered organizations, including structures with low-dimensional elements, helical motifs, a nanoscale analogue of a face-centred perovskite crystal and a distributed Bragg reflector based on a crystal with plasmonic and photonic length-scale regimes.

36 MATERIALS SCIENCE↗
DOE OSTI2026

A nanoporous capacitive electrochemical ratchet for continuous ion separations

Directed ion transport in liquid electrolyte solutions underlies many phenomena in natural and industrial settings. While nature has evolved structures that drive continuous ion flow without Faradaic redox reactions, establishing this process in synthetic systems has been challenging. Here, in this study, we report an ion pump that drives aqueous ions against a force using a capacitive ratchet mechanism independent of redox reactions. Modulation of an electric potential between thin metallic layers on either face of a nanoporous alumina wafer immersed in solution results in persistent voltages and ionic currents. This occurs due to the nonlinear capacitive nature of electric double layers, whose repeated charging and discharging sustains a continuous ion flux. Using this approach, we demonstrate ratchet-driven electrodialysis that reaches a 50% decrease in the conductivity of the solution in a dilution cell. These ratchet-based ion pumps can enable continuous desalination and selective ion separation using an electrically powered device with no moving parts.

Kautz, Rylan [University of California, Irvine, CA↗
DOE OSTI2020

Electron acceleration in laboratory-produced turbulent collisionless shocks

Astrophysical collisionless shocks are among the most powerful particle accelerators in the Universe. Generated by violent interactions of supersonic plasma flows with the interstellar medium, supernova remnant shocks are observed to amplify magnetic fields and accelerate electrons and protons to highly relativistic speeds. In the well-established model of diffusive shock acceleration, relativistic particles are accelerated by repeated shock crossings. However, this requires a separate mechanism that pre-accelerates particles to enable shock crossing. This is known as the ‘injection problem’, which is particularly relevant for electrons, and remains one of the most important puzzles in shock acceleration. In most astrophysical shocks, the details of the shock structure cannot be directly resolved, making it challenging to identify the injection mechanism. In this letter we report results from laser-driven plasma flow experiments, and related simulations, that probe the formation of turbulent collisionless shocks in conditions relevant to young supernova remnants. We show that electrons can be effectively accelerated in a first-order Fermi process by small-scale turbulence produced within the shock transition to relativistic non-thermal energies, helping overcome the injection problem. Our observations provide new insight into electron injection at shocks and open the way for controlled laboratory studies of the physics underlying cosmic accelerators.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Assessment of the errors of high-fidelity two-qubit gates in silicon quantum dots

Achieving high-fidelity entangling operations between qubits consistently is essential for the performance of multi-qubit systems. Solid-state platforms are particularly exposed to errors arising from materials-induced variability between qubits, which leads to performance inconsistencies. Here we study the errors in a spin qubit processor, tying them to their physical origins. We use this knowledge to demonstrate consistent and repeatable operation with above 99% fidelity of two-qubit gates in the technologically important silicon metal-oxide-semiconductor quantum dot platform. Analysis of the physical errors and fidelities in multiple devices over extended periods allows us to ensure that we capture the variation and the most common error types. Physical error sources include the slow nuclear and electrical noise on single qubits and contextual noise that depends on the applied control sequence. Furthermore, we investigate the impact of qubit design, feedback systems and robust gate design to inform the design of future scalable, high-fidelity control strategies. Our results highlight both the capabilities and challenges for the scaling-up of silicon spin-based qubits into full-scale quantum processors.

Quantum dots↗
DOE OSTI2020

Demonstration of cooling by the Muon Ionization Cooling Experiment

The use of accelerated beams of electrons, protons or ions has furthered the development of nearly every scientific discipline. However, high-energy muon beams of equivalent quality have not yet been delivered. Muon beams can be created through the decay of pions produced by the interaction of a proton beam with a target. Such ‘tertiary’ beams have much lower brightness than those created by accelerating electrons, protons or ions. High-brightness muon beams comparable to those produced by state-of-the-art electron, proton and ion accelerators could facilitate the study of lepton–antilepton collisions at extremely high energies and provide well characterized neutrino beams. Such muon beams could be realized using ionization cooling, which has been proposed to increase muon-beam brightness. Here we report the realization of ionization cooling, which was confirmed by the observation of an increased number of low-amplitude muons after passage of the muon beam through an absorber, as well as an increase in the corresponding phase-space density. The simulated performance of the ionization cooling system is consistent with the measured data, validating designs of the ionization cooling channel in which the cooling process is repeated to produce a substantial cooling effect. The results presented here are an important step towards achieving the muon-beam quality required to search for phenomena at energy scales beyond the reach of the Large Hadron Collider at a facility of equivalent or reduced footprint.

43 PARTICLE ACCELERATORS↗
DOE OSTI2020

The promise and challenge of therapeutic genome editing

Genome editing, which involves the precise manipulation of cellular DNA sequences to alter cell fates and organism traits, has the potential to both improve our understanding of human genetics and cure genetic disease. Here I discuss the scientific, technical and ethical aspects of using CRISPR (clustered regularly interspaced short palindromic repeats) technology for therapeutic applications in humans, focusing on specific examples that highlight both opportunities and challenges. Further, genome editing is—or will soon be—in the clinic for several diseases, with more applications under development. The rapid pace of the field demands active efforts to ensure that this breakthrough technology is used responsibly to treat, cure and prevent genetic disease.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Constraint on the matter–antimatter symmetry-violating phase in neutrino oscillations

The charge-conjugation and parity-reversal (CP) symmetry of fundamental particles is a symmetry between matter and antimatter. Violation of this CP symmetry was first observed in 1964, and CP violation in the weak interactions of quarks was soon established. Sakharov proposed that CP violation is necessary to explain the observed imbalance of matter and antimatter abundance in the Universe. Yet, CP violation in quarks is too small to support this explanation. So far, CP violation has not been observed in non-quark elementary particle systems. It has been shown that CP violation in leptons could generate the matter–antimatter disparity through a process called leptogenesis. Leptonic mixing, which appears in the standard model’s charged current interactions, provides a potential source of CP violation through a complex phase δ CP , which is required by some theoretical models of leptogenesis. This CP violation can be measured in muon neutrino to electron neutrino oscillations and the corresponding antineutrino oscillations, which are experimentally accessible using accelerator-produced beams as established by the Tokai-to-Kamioka (T2K) and NOvA experiments. Until now, the value of δ CP has not been substantially constrained by neutrino oscillation experiments. Here we report a measurement using long-baseline neutrino and antineutrino oscillations observed by the T2K experiment that shows a large increase in the neutrino oscillation probability, excluding values of δ CP that result in a large increase in the observed antineutrino oscillation probability at three standard deviations (3σ). The 3σ confidence interval for δ CP , which is cyclic and repeats every 2π, is [-3.41, -0.03] for the so-called normal mass ordering and [-2.54, -0.32] for the inverted mass ordering. Our findings indicate CP violation in leptons and our method enables sensitive searches for matter–antimatter asymmetry in neutrino oscillations using accelerator-produced neutrino beams. Future measurements with larger datasets will test whether leptonic CP violation is larger than the CP violation in quarks.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Large-scale integration of artificial atoms in hybrid photonic circuits

A central challenge in developing quantum computers and long-range quantum networks is the distribution of entanglement across many individually controllable qubits. Colour centres in diamond have emerged as leading solid-state ‘artificial atom’ qubits because they enable on-demand remote entanglement, coherent control of over ten ancillae qubits with minute-long coherence times and memory-enhanced quantum communication. A critical next step is to integrate large numbers of artificial atoms with photonic architectures to enable large-scale quantum information processing systems. So far, these efforts have been stymied by qubit inhomogeneities, low device yield and complex device requirements. Here we introduce a process for the high-yield heterogeneous integration of ‘quantum microchiplets’—diamond waveguide arrays containing highly coherent colour centres—on a photonic integrated circuit (PIC). We use this process to realize a 128-channel, defect-free array of germanium-vacancy and silicon-vacancy colour centres in an aluminium nitride PIC. Photoluminescence spectroscopy reveals long-term, stable and narrow average optical linewidths of 54 megahertz (146 megahertz) for germanium-vacancy (silicon-vacancy) emitters, close to the lifetime-limited linewidth of 32 megahertz (93 megahertz). We show that inhomogeneities of individual colour centre optical transitions can be compensated in situ by integrated tuning over 50 gigahertz without linewidth degradation. The ability to assemble large numbers of nearly indistinguishable and tunable artificial atoms into phase-stable PICs marks a key step towards multiplexed quantum repeaters and general-purpose quantum processors

36 MATERIALS SCIENCE↗
DOE OSTI2021

Self-similar mesocrystals form via interface-driven nucleation and assembly

Crystallization by particle attachment (CPA) is a frequently occurring mechanism of colloidal crystallization that results in hierarchical morphologies. CPA has been exploited to create nanomaterials with unusual properties and is implicated in the development of complex mineral textures. Oriented attachment–a form of CPA in which particles align along specific crystallographic directions–produces mesocrystals that diffract as single crystals do, although the constituent particles are still discernible. The conventional view of CPA is that nucleation provides a supply of particles that aggregate via Brownian motion biased by attractive interparticle potentials. However, mesocrystals often exhibit regular morphologies and uniform sizes. Although many crystal systems form mesocrystals and individual attachment events have been directly visualized10, how random attachment events lead to well defined, self-similar morphologies remains unknown, as does the role of surface-bound ligands, which are ubiquitous in nanoparticle systems. Attempts to understand mesocrystal formation are further complicated in many systems by the presence of precursor nanoparticles with a phase distinct from that of the bulk. Some studies propose that such particles convert before attachment, whereas others attribute conversion to the attachment process itself and yet others conclude that transformation occurs after the mesocrystals exceed a characteristic size. Here we investigate mesocrystal formation by iron oxides, which are important colloidal phases in natural environments and classic examples of systems forming ubiquitous precursor phases and undergoing CPA accompanied by phase transformations. Combining in situ transmission electron microscopy (TEM) at 80 degrees Celsius with ‘freeze-and-look’ TEM, we tracked the formation of haematite (Hm) mesocrystals in the presence of oxalate (Ox), which is abundant in soils, where iron oxides are common. In this work, we find that isolated Hm particles rarely appear, but once formed, interfacial gradients at the Ox-covered surfaces drive Hm particles to nucleate repeatedly about two nanometres from the surfaces, to which they then attach, thereby generating mesocrystals. Comparison to natural and synthetic systems suggests that interface-driven pathways are widespread.

36 MATERIALS SCIENCE↗
DOE OSTI2023

High-fidelity parallel entangling gates on a neutral-atom quantum computer

The ability to perform entangling quantum operations with low error rates in a scalable fashion is a central element of useful quantum information processing. Neutral-atom arrays have recently emerged as a promising quantum computing platform, featuring coherent control over hundreds of qubits and any-to-any gate connectivity in a flexible, dynamically reconfigurable architecture. The main outstanding challenge has been to reduce errors in entangling operations mediated through Rydberg interactions. Here we report the realization of two-qubit entangling gates with 99.5% fidelity on up to 60 atoms in parallel, surpassing the surface-code threshold for error correction. Our method uses fast, single-pulse gates based on optimal control, atomic dark states to reduce scattering and improvements to Rydberg excitation and atom cooling. We benchmark fidelity using several methods based on repeated gate applications, characterize the physical error sources and outline future improvements. Finally, we generalize our method to design entangling gates involving a higher number of qubits, which we demonstrate by realizing low-error three-qubit gates. By enabling high-fidelity operation in a scalable, highly connected system, these advances lay the groundwork for large-scale implementation of quantum algorithms, error-corrected circuits and digital simulations.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Axon-like active signal transmission

Any electrical signal propagating in a metallic conductor loses amplitude due to the natural resistance of the metal. Compensating for such losses presently requires repeatedly breaking the conductor and interposing amplifiers that consume and regenerate the signal. This century-old primitive severely constrains the design and performance of modern interconnect-dense chips. Here we present a fundamentally different primitive based on semi-stable edge of chaos (EOC), a long-theorized but experimentally elusive regime that underlies active (self-amplifying) transmission in biological axons. By electrically accessing the spin crossover in LaCoO 3 , we isolate semi-stable EOC, characterized by small-signal negative resistance and amplification of perturbations. In a metallic line atop a medium biased at EOC, a signal input at one end exits the other end amplified, without passing through a separate amplifying component. While superficially resembling superconductivity, active transmission offers controllably amplified time-varying small-signal propagation at normal temperature and pressure, but requires an electrically energized EOC medium. Operando thermal mapping reveals the mechanism of amplification—bias energy of the EOC medium, instead of fully dissipating as heat, is partly used to amplify signals in the metallic line, thereby enabling spatially continuous active transmission, which could transform the design and performance of complex electronic chips.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗