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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Elucidating ion capture and transport mechanisms of Preyssler anions in aqueous solutions using biased MACE-accelerated MD simulations

Equilibrium and biased multi-atomic cluster expansion (MACE) accelerated molecular dynamics (MD) simulations in aqueous solutions are performed to investigate the ion capture and transport mechanisms of the {P 5 W 30 } Preyssler anion (PA) as the smallest representative member of the extended polyoxometalate (POM) family with an internal cavity. The unique interatomic interactions present in the internal cavity vs the exterior of PA are carefully investigated using equilibrium MACE MD simulations for two representative Na(H 2 O)@PA and Na@PA complexes in aqueous solutions. Our careful analyses of radial distribution functions and coordination numbers show that the presence of confined water in Na(H 2 O)@PA has profound modulating effects on the nature of the interactions of the encapsulated ion with the oxygens of the PA cavity. Using well-converged MACE-accelerated multiple walker well-tempered metadynamics simulations with nanosecond timescales, two different associative (ion exchange) and dissociative (ion ejection) ion transport mechanisms were carefully investigated for Na + as one of the most abundant and representative ions present in seawater and saline solutions. By comparing systems with and without confined water, it was found that the presence of only one pre-encapsulated confined water in Na(H 2 O)@PA dramatically changes the free energy landscape of ion transport processes. It was also found that the contraction and dilation of the two windows present in PA directly influence the Na + and H 2 O transport. Furthermore, the results from this work are helpful, as they show a viable path toward tuning the ion exchange and transport phenomena in aqueous solutions of POM molecular clusters and frameworks.

25 ENERGY STORAGE↗
DOE OSTI2021

Probing Quantum Speed Limits with Ultracold Gases

Here, quantum speed limits (QSLs) rule the minimum time for a quantum state to evolve into a distinguishable state in an arbitrary physical process. These fundamental results constrain a notion of distance traveled by the quantum state, known as the Bures angle, in terms of the speed of evolution set by nonadiabatic energy fluctuations. I theoretically propose how to measure QSLs in an ultracold quantum gas confined in a time-dependent harmonic trap. In this highly-dimensional system of continuous variables, quantum tomography is prohibited. Yet, QSLs can be probed whenever the dynamics is self-similar by measuring as a function of time the cloud size of the ultracold gas. This makes it possible to determine the Bures angle and energy fluctuations, as I discuss for various ultracold atomic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

A sub-5 ps jitter time-to-digital converter ASIC with back-gate delay tuning in 22 nm CMOS

We present the design of a Time-to-Digital Converter (TDC) ASIC together with performance characterization results at cryogenic temperature (6-8 K), and at room temperature using emulated Low-Gain Avalanche Detector (LGAD) signals. The TDC design uses a two-step architecture with a ring-oscillator based counter and a Vernier delay line fine TDC. The TDC is implemented in an FD-SOI process, and back-gate tuning is used not only to correct threshold variation due to cryogenic operation, but also as a novel way to tune TDC delay elements with very little overhead. Using this technique, we demonstrate a design with very low power (0.5 mW) and area (0.003 mm 2 ). We present test results using the Fermilab Constant Fraction Discriminator (FCFD) ASIC to produce discriminated signals from an internal charge injection mechanism that mimics the waveform and signal amplitude of minimum ionizing particles impinging on LGAD sensors. We characterize the time precision of the full system and verify that the TDC ASIC contributes a negligible amount to the total system time precision, fully consistent with the expected jitter contribution of less than 5 ps. In conclusion, the results presented here demonstrate the utility of our TDC for applications in physics and quantum communications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

eReaxFF force field development for BaZr 0.8 Y 0.2 O 3-δ solid oxide electrolysis cells applications

The use of solid-oxide materials in electrocatalysis applications, especially in hydrogen-evolution reactions, is promising. However, further improvements are warranted to overcome the fundamental bottlenecks to enhancing the performance of solid-oxide electrolysis cells (SOECs), which is directly linked to the more-refined fundamental understanding of complex physical and chemical phenomena and mass exchanges that take place at the surfaces and in the bulk of electrocatalysis materials. Here, we developed an eReaxFF force field for barium zirconate doped with 20 mol% of yttrium, BaZr 0.8 Y 0.2 O 3-δ (BZY20) to enable a systematic, large-length-scale, and longer-timescale atomistic simulation of solid-oxide electrocatalysis for hydrogen generation. All parameters for the eReaxFF were optimized to reproduce quantum-mechanical (QM) calculations on relevant condensed phase and cluster systems describing oxygen vacancies, vacancy migrations, electron localization, water adsorption, water splitting, and hydrogen generation on the surfaces of the BZY20 solid oxide. Using the developed force field, we performed both zero-voltage (excess electrons absent) and non-zero-voltage (excess electrons present) molecular dynamics simulations to observe water adsorption, water splitting, proton migration, oxygen-vacancy migrations, and eventual hydrogen-production reactions. Based on investigations offered in the present study, we conclude that the eReaxFF force field-based approach can enable computationally efficient simulations for electron conductivity, electron leakage, and other non-zero-voltage effects on the solid oxide materials using the explicit-electron concept. Moreover, we demonstrate how the eReaxFF force field-based atomistic-simulation approach can enhance our understanding of processes in SOEC applications and potentially other renewable-energy applications.

08 HYDROGEN↗
DOE OSTI2021

Ultrafast time-resolved x-ray absorption spectroscopy of ionized urea and its dimer through ab initio nonadiabatic dynamics

Investigating the early dynamics of chemical systems following ionization is essential for our understanding of radiation damage. However, experimental as well as theoretical investigations are very challenging due to the complex nature of these processes. Time-resolved x-ray absorption spectroscopy on a femtosecond timescale, in combination with appropriate simulations, is able to provide crucial insights into the ultrafast processes that occur upon ionization due to its element-specific probing nature. In this theoretical study, we investigate the ultrafast dynamics of valence-ionized states of urea and its dimer employing Tully's fewest switches surface hopping approach using Koopmans' theorem to describe the ionized system. We demonstrate that following valence ionization through a pump pulse, the time-resolved x-ray absorption spectra at the carbon, nitrogen, and oxygen K-edges reveal rich insights into the dynamics. Excited states of the ionized system give rise to time-delayed blueshifts in the x-ray absorption spectra as a result of electronic relaxation dynamics through nonadiabatic transitions. Moreover, our statistical analysis reveals specific structural dynamics in the molecule that induce time-dependent changes in the spectra. For the urea monomer, we elucidate the possibility to trace effects of specific molecular vibrations in the time-resolved x-ray absorption spectra. For the urea dimer, where ionization triggers a proton transfer reaction, we show how the x-ray absorption spectra can reveal specific details on the progress of proton transfer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Signatures of Cooper pair dynamics and quantum-critical superconductivity in tunable carrier bands

Different superconducting pairing mechanisms are markedly distinct in the underlying Cooper pair kinematics. Quantum-critical soft modes drive pairing interactions in which the pair scattering processes are highly collinear and can be classified into two categories: forward scattering and backscattering. Conversely, in conventional phonon mechanisms, Cooper pair scattering is of a generic noncollinear character. In this study, we present a method to discern the kinematic type by observing the evolution of superconductivity while adjusting the Fermi surface geometry. To demonstrate our approach, we utilize the recently reported phase diagrams of untwisted graphene multilayers. Our analysis connects the emergence of superconductivity at “ghost crossings” of Fermi surfaces in distinct valleys to the pair kinematics of a backscattering type. Together with the observed nonmonotonic behavior of superconductivity near its onset (sharp rise followed by a drop), it lends strong support to a particular quantum-critical superconductivity scenario in which pairing is driven by intervalley coherence fluctuations. These findings offer direct insights into the genesis of pairing in these systems, providing compelling evidence for the electron–electron interactions driving superconductivity. More broadly, our work highlights the potential of tuning bands via ghost crossings as a promising means of boosting superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2003

Alloy Design Data Generated for B2-Ordered Compounds

Developing alloys based on ordered compounds is significantly more complicated than developing designs based on disordered materials. In ordered compounds, the major constituent elements reside on particular sublattices. Therefore, the addition of a ternary element to a binary-ordered compound is complicated by the manner in which the ternary addition is made (at the expense of which binary component). When ternary additions are substituted for the wrong constituent, the physical and mechanical properties usually degrade. In some cases the resulting degradation in properties can be quite severe. For example, adding alloying additions to NiAl in the wrong combination (i.e., alloying additions that prefer the Al sublattice but are added at the expense of Ni) will severely embrittle the alloy to the point that it can literally fall apart during processing on cooling from the molten state. Consequently, alloying additions that strongly prefer one sublattice over another should always be added at the expense of that component during alloy development. Elements that have a very weak preference for a sublattice can usually be safely added at the expense of either element and will accommodate any deviation from stoichiometry by filling in for the deficient component. Unfortunately, this type of information is not known beforehand for most ordered systems. Therefore, a computational survey study, using a recently developed quantum approximate method, was undertaken at the NASA Glenn Research Center to determine the preferred site occupancy of ternary alloying additions to 12 different B2-ordered compounds including NiAl, FeAl, CoAl, CoFe, CoHf, CoTi, FeTi, RuAl, RuSi, RuHf, RuTi, and RuZr. Some of these compounds are potential high temperature structural alloys; others are used in thin-film magnetic and other electronic applications. The results are summarized. The italicized elements represent the previous sum total alloying information known and verify the computational method used to establish the table. Details of the computational procedures used to determine the preferred site occupancy can be found in reference 2. As further substantiation of the validity of the technique, and its extension to even more complicated systems, it was applied to two simultaneous alloying additions in an ordered alloy.

Noebe, Ronald D.↗
DOE OSTI2021

Toward alcohol synthesis from CO hydrogenation on Cu(111)-supported MoS 2 – predictions from DFT+KMC

In the quest for cheap and efficient catalysts for alcohol synthesis from syngas, a material of interest is single-layer MoS2 owing to its low cost, abundancy, and flexible structure. Because of the inertness of its basal plane, however, it is essential to find ways that make it catalytically active. Herein, by means of density functional theory based calculations of reaction pathways and activation energy barriers and accompanying kinetic Monte Carlo simulations, we show that while S vacancy row structures activate the MoS 2 basal plane, further enhancement of chemical activity and selectivity can be achieved by interfacing the MoS 2 layer with a metallic support. When defect-laden MoS2 is grown on Cu(111), there is not only an increase in the active region (surface area of active sites) but also charge transfer from Cu to MoS 2 , resulting in a shift of the Fermi level such that the frontier states (d orbitals of the exposed Mo atoms) appear close to it, making the MoS 2 /Cu(111) system ready for catalytic activity. Finally, our calculated thermodynamics of reaction pathways lead to the conclusion that the Cu(111) substrate promotes both methanol and ethanol as the products, while kinetic Monte Carlo simulations suggest a high selectivity toward the formation of ethanol.

2D materials↗
DOE OSTI2023

Scrambling and quantum chaos indicators from long-time properties of operator distributions

Scrambling is a key concept in the analysis of nonequilibrium properties of quantum many-body systems. Most studies focus on its characterization via out-of-time-ordered correlation (OTOC) functions, particularly through the early-time decay of the OTOC. However, scrambling is a complex process which involves operator spreading and operator entanglement, and a full characterization requires one to access more refined information on the operator dynamics at several timescales. In this work we analyze operator scrambling by expanding the target operator in a complete basis and studying the structure of the expansion coefficients treated as a coarse-grained probability distribution in the space of operators. Here we study different features of this distribution, such as its mean, variance, and participation ratio, for the Ising model with longitudinal and transverse fields, kicked collective spin models, and random circuit models. We show that the long-time properties of the operator distribution display common features across these cases and discuss how these properties can be used as a proxy for the onset of quantum chaos. Finally, we discuss the connection with OTOCs and analyze the cost of probing the operator distribution experimentally using these correlation functions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Observation of Topological Chirality Switching Induced Freezing of a Skyrmion Crystal

Magnetic skyrmions are topologically protected quasi-particles with a well-defined chirality. Control over their chirality is proposed as an additional feature for encoding data bits or as qubits in quantum computing due to their high efficiency and stability against achiral magnetic textures. Here it is shown that an in-plane magnetic field can be utilized to reshape the energy barriers between different skyrmionic bubbles (e.g., Bloch type, type-II) enabling spontaneous chirality fluctuations with a frequency that increases with the strength of the in-plane field. The insulating van der Waals ferromagnet CrBr3 is used as an archetypal system for low damping, reduced energy dissipation and a high number of magnetic phases to capture the chirality dynamics in real time through cryo-Lorentz transmission electron microscopy. It is observed that the interplay between the intrinsic Dzyaloshinskii–Moriya interaction and out-of-plane field biased the chirality dynamics, favoring one handedness over the other. A remarkable consequence of the spontaneous chirality switching mechanism is that it induces a freezing (or crystallization) process in the skyrmion lattice. As the bubbles fluctuate between Bloch and type-II they elongate and shrink parallel to the in-plane field. Subsequently, the overall lattice crystallizes along the in-plane field direction, inducing a phase transition from a disordered liquid state to a hexatic phase where skyrmions are highly ordered resembling that of a solid. The results indicate chirality as an active element in the creation of topologically protected skyrmion crystals unveiling pathways toward chiral spintronic device platforms with tunable embedded configuration.

2D Phase Transition↗
DOE OSTI2020

System and method for high power diode based additive manufacturing

A system is disclosed for performing an Additive Manufacturing (AM) fabrication process on a powdered material forming a substrate. The system may make use of a diode array for generating an optical signal sufficient to melt a powdered material of the substrate. A mask may be used for preventing a first predetermined portion of the optical signal from reaching the substrate, while allowing a second predetermined portion to reach the substrate. At least one processor may be used for controlling an output of the diode array.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Subnanometer Scale Mapping of Hydrogen Doping in Vanadium Dioxide

Hydrogen donor doping of correlated electron systems such as vanadium dioxide (VO 2 ) profoundly modifies the ground state properties. The electrical behavior of H x VO 2 is strongly dependent on the hydrogen concentration; hence, atomic scale control of the doping process is necessary. It is however a nontrivial problem to quantitatively probe the hydrogen distribution in a solid matrix. As hydrogen transfers its sole electron to the material, the ionization mechanism is suppressed. Here in this study, a methodology mapping the doping distribution at subnanometer length scale is demonstrated across a H x VO 2 thin film focusing on the oxygen-hydrogen bonds using electron energy loss spectroscopy (EELS) coupled with first-principles EELS calculations. The hydrogen distribution was revealed to be nonuniform along the growth direction and between different VO 2 grains, calling for intricate hydrogenation mechanisms. Our study points to a powerful approach to quantitatively map dopant distribution in quantum materials relevant to energy and information science

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validation

Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These calculations often involve a significant amount of manual input and expertise, although most of this effort could be automated, which would alleviate the need for expertise in software and hardware accessibility. Here, we present the AutoRXN workflow, an automated workflow for exploratory high-throughput electronic structure calculations of molecular systems, in which (i) density functional theory methods are exploited to deliver minimum and transition-state structures and corresponding energies and properties, (ii) coupled cluster calculations are then launched for optimized structures to provide more accurate energy and property estimates, and (iii) multi-reference diagnostics are evaluated to back check the coupled cluster results and subject them to automated multi-configurational calculations for potential multi-configurational cases. All calculations are carried out in a cloud environment and support massive computational campaigns. Key features of all components of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow with the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Attosecond XUV probing of vibronic quantum superpositions in Br 2 +

Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on a few femtosecond timescale. While recent attosecond experiments have addressed real-time observation of these primary photochemical processes, the underlying roles of simultaneous nuclear motions and how they modify and disturb the valence electronic motion remain uncertain. In this work, we investigate coherent electronic-vibrational dynamics induced among multiple vibronic levels of ionic bromine (Br 2 + ), including both spin-orbit (X 2 Π 3/2,g – X 2 Π 1/2,g ) and valence (A 2 Π 3/2,u – 4 Σ 3/2,u ) electronic superpositions, using attosecond transient absorption spectroscopy. Decay, revival, and apparent frequency shifts of electronic coherences are measured via characteristic quantum beats on the Br-3d core-level absorption signals. Quantum-mechanical simulations attribute the observed electronic decoherence to broadened phase distributions of nuclear wave packets on anharmonic potentials. Molecular vibronic structure is further revealed to be imprinted as discrete progressions in electronic beat frequencies. These results provide a future basis to interpret complex charge-migration dynamics in polyatomic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Solvated Nuclear–Electronic Orbital Structure and Dynamics

Nonadiabatic dynamical processes such as proton-coupled electron transfer and excited state intramolecular proton transfer have been the subject of much research. One of the promising theoretical methods to describe these processes is the nuclear–electronic orbital (NEO) approach. This approach inherently accounts for nuclear quantum effects within quantum chemistry calculations, and it has recently been extended to directly simulate nonadiabatic processes with the development of real-time NEO methods. These processes can also be significantly dependent on the surrounding chemical environment, however, and capturing the effects of the environment is often necessary for analyzing experimentally relevant systems. This work couples the NEO density functional theory and real-time time-dependent density functional theory approaches with solvation through the polarizable continuum model. Here, the effects of this coupling are investigated for ground state properties, solvent-dependent vibrational frequencies, and direct excited state intramolecular proton transfer dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Holographic Kolmogorov-Sinai entropy and the quantum Lyapunov spectrum

In classical chaotic systems the entropy, averaged over initial phase space distributions, follows a universal behavior. While approaching thermal equilibrium it passes through a stage where it grows linearly, while the growth rate, the Kolmogorov-Sinai entropy (rate), is given by the sum over all positive Lyapunov exponents. A natural question is whether a similar relation is valid for quantum systems. We argue that the Maldacena-Shenker-Stanford bound on quantum Lyapunov exponents implies that the upper bound on the growth rate of the entropy, averaged over states in Hilbert space that evolve towards a thermal state with temperature T, should be given by πT times the thermal state’s von Neumann entropy. Strongly coupled, large N theories with black hole duals should saturate the bound. To test this we study a large number of isotropization processes of random, spatially homogeneous, far from equilibrium initial states in large N, $\mathcal{N}$ = 4 Super Yang Mills theory at strong coupling and compute the ensemble averaged growth rate of the dual black hole’s apparent horizon area. We find both an analogous behavior as in classical chaotic systems and numerical evidence that the conjectured bound on averaged entropy growth is saturated granted that the Lyapunov exponents are degenerate and given by λ i = ±2πT. This fits to the behavior of classical systems with plus/minus symmetric Lyapunov spectra, a symmetry which implies the validity of Liouville’s theorem.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Advances and opportunities in materials science for scalable quantum computing

We report that by harnessing unique quantum mechanical phenomena, such as superposition and entanglement, quantum computers offer the possibility to drastically outperform classical computers for certain classes of problems. The realization of this potential, however, presents a substantial challenge, because noise and imperfections associated with the materials used to fabricate devices can obscure the delicate quantum mechanical effects that enable quantum computing. Hence, progress in synthesis, characterization, and modeling of materials for quantum computing have driven many exciting advances in recent years and will become increasingly important in the years to come. As progressively more complex, multi-qubit systems come online, and as significant government and industrial investment drives research forward, new challenges and opportunities for materials science continue to emerge. The articles in this issue survey the current state of materials science progress and obstacles for some leading quantum computing platforms; opportunities for deeper involvement by materials scientists abound. Ultimate realization of the full potential of quantum computers will require a multidisciplinary effort spanning many traditional areas of expertise.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Development of electro-optical quantum transducers based on three-dimensional superconducting cavities

Quantum transducers enable the conversion of quantum information and signals between different physical platforms. Based on the pioneering works in three-dimensional superconducting cavity technology developed at Fermilab, we are advancing the development of three-dimensional microwave-optical transducers and exploring their applications in quantum information processing and sensing. We present our progress in the design, fabrication, and characterization of three-dimensional microwave cavities integrated with bulk lithium niobate resonators. The material characterization using three-dimensional cavities based on a resonant-type method allows for understanding of complex permittivity and loss mechanism of electro-optic materials at cryogenic temperatures. We also evaluate the potential of the high-efficiency quantum transducers in enhancing the performance of quantum sensors for applications such as dark matter detection, compared to conventional homodyne detection approaches. This manuscript has been authored by Fermi Research Alliance, LLC under Contract No. DE-AC0207CH11359 with the U.S. Department of Energy, Office of Science, Office of High Energy Physics. This work is funded by the DOE's Early Career Research Program. This research used resources of the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Superconducting Quantum Materials and Systems Center (SQMS) under Contract No. DE-AC02-07CH11359.

Zorzetti, Silvia↗