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At least 631 records · Page 35

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DOE OSTI2017

Understanding trends in electrochemical carbon dioxide reduction rates

Electrochemical carbon dioxide reduction to fuels presents one of the great challenges in chemistry. Herein we present an understanding of trends in electrocatalytic activity for carbon dioxide reduction over different metal catalysts that rationalize a number of experimental observations including the selectivity with respect to the competing hydrogen evolution reaction. We also identify two design criteria for more active catalysts. The understanding is based on density functional theory calculations of activation energies for electrochemical carbon monoxide reduction as a basis for an electrochemical kinetic model of the process. Furthermore, we develop scaling relations relating transition state energies to the carbon monoxide adsorption energy and determine the optimal value of this descriptor to be very close to that of copper.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

A quantum processor based on coherent transport of entangled atom arrays

The ability to engineer parallel, programmable operations between desired qubits within a quantum processor is key for building scalable quantum information systems. In most state-of-the-art approaches, qubits interact locally, constrained by the connectivity associated with their fixed spatial layout. Here we demonstrate a quantum processor with dynamic, non-local connectivity, in which entangled qubits are coherently transported in a highly parallel manner across two spatial dimensions, between layers of single- and two-qubit operations. Our approach makes use of neutral atom arrays trapped and transported by optical tweezers; hyperfine states are used for robust quantum information storage, and excitation into Rydberg states is used for entanglement generation. We use this architecture to realize programmable generation of entangled graph states, such as cluster states and a seven-qubit Steane code state. Furthermore, we shuttle entangled ancilla arrays to realize a surface code state with thirteen data and six ancillary qubits and a toric code state on a torus with sixteen data and eight ancillary qubits. Finally, we use this architecture to realize a hybrid analogue–digital evolution and use it for measuring entanglement entropy in quantum simulations, experimentally observing non-monotonic entanglement dynamics associated with quantum many-body scars. Realizing a long-standing goal, these results provide a route towards scalable quantum processing and enable applications ranging from simulation to metrology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Active learning across intermetallics to guide discovery of electrocatalysts for CO2 reduction and H2 evolution

The electrochemical reduction of CO2 and H2 evolution from water can be used to store renewable energy that is produced intermittently. Scale-up of these reactions requires the discovery of effective electrocatalysts, but the electrocatalyst search space is too large to explore exhaustively. Here we present a theoretical, fully automated screening method that uses a combination of machine learning and optimization to guide density functional theory calculations, which are then used to predict electrocatalyst performance. We demonstrate the feasibility of this method by screening various alloys of 31 different elements, and thereby perform a screening that encompasses 50% of the d-block elements and 33% of the p-block elements. This method has thus far identified 131 candidate surfaces across 54 alloys for CO2 reduction and 258 surfaces across 102 alloys for H2 evolution. We use qualitative analyses to prioritize the top candidates for experimental validation.

Chemistry↗

DOE OSTI2017

Characterization of chemical contaminants and their spectral properties from an atmospheric pressure ns-pulsed microdischarge in neon

Portable applications of microdischarges will mandate operation in the presence of contaminant species. This paper examines the temporal evolution of microdischarge optical and ultraviolet emissions during pulsed operation by experimental methods. By varying the pulse length of a microdischarge initiated in a 4-hole silicon microcavity array operating in a 655 Torr ambient primarily composed of Ne, we were able to measure the emission growth rates for different contaminant species native to the discharge environment as a function of pulse length. It was found that emission from hydrogen and oxygen impurities demonstrated similar rates of change, while emissions from molecular and atomic nitrogen, measured at 337.1 and 120 nm’s respectively, exhibited the lowest rate of change. We conclude that it is likely that O 2 undergoes the same resonant energy transfer process between rare gas excimers that has been shown for H 2 . Further, efficient resonant processes were found to be favored during ignition and extinction phases of the pulse, while emission at the 337.1 nm line from N 2 was favored during the intermediate stage of the plasma. In addition to experimental results, a zero-dimensional analysis is also presented to further understand the nature of the microdischarge.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Observation of extremely strong shock waves in solids launched by petawatt laser heating

Understanding hydrodynamic phenomena driven by fast electron heating is important for a range of applications including fast electron collimation schemes for fast ignition and the production and study of hot, dense matter. In this work, detailed numerical simulations modelling the heating, hydrodynamic evolution, and extreme ultra-violet (XUV) emission in combination with experimental XUV images indicate shock waves of exceptional strength (200 Mbar) launched due to rapid heating of materials via a petawatt laser. In conclusion, we discuss in detail the production of synthetic XUV images and how they assist us in interpreting experimental XUV images captured at 256 eV using a multi-layer spherical mirror.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

A gas dynamic perspective on particle lifting in electrostatic discharge-like devices using multiphase particle-in-cell approach

Although particle–laden electrostatic discharges are widely used in laboratories as well as in industrial applications, the mechanism of particle lifting for particles initially at rest in such highly unsteady systems is not well understood. A multiphase gas–particle solver is developed using the multiphase particle-in-cell (MP-PIC) approach to emulate the interaction of a compressible shock-dominated gas phase with the dense particle phase. First, the two-way coupled solver is initially used to study the interaction of a planar traveling shock with a vertical curtain of particulates. The gas and particle phase evolution was found to be in good agreement with a similar experimental study in Ling et al. [Phys. Fluids 24, 113301 (2012)]. Second, the MP-PIC code is used to study the interaction of an expanding blast wave with a thick bed of particles. The simulation considered forces such as quasi-steady drag, pressure-gradient, added-mass, Saffman, and Magnus forces. We observe that the vertical liftoff particles close to the shock impingement point in this configuration are associated with the quasi-steady drag, pressure gradient, and added-mass forces. Also, the Saffman lift and Magnus forces contribute to lifting particles located radially farther away from the shock impingement point. In addition, the study finds a decrease in particle lifting efficiency with decreasing plasma kernel length and shock strength.

42 ENGINEERING↗

DOE OSTI2024

Guided Mode Evolution and Ionization Injection in Meter-Scale Multi-GeV Laser Wakefield Accelerators

Here, we show that multi-GeV laser wakefield electron accelerators in meter-scale, low density hydrodynamic plasma waveguides operate in a new nonlinear propagation regime dominated by sustained beating of lowest order modes of the ponderomotively modified channel; this occurs whether or not the injected pulse is linearly matched to the guide. For a continuously doped gas jet, this emergent mode beating effect leads to axially modulated enhancement of ionization injection and a multi-GeV energy spectrum of multiple quasimonoenergetic peaks; the same process in a locally doped jet produces single multi-GeV peaks with <10% energy spread. A three-stage model of drive laser pulse evolution and ionization injection characterizes the beating effect and explains our experimental results.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

In-cylinder spray evolution in a motored central-injection gasoline engine: Imaging and simulating the effects of flash-boiling and intake crossflow

Accurate predictions of fuel spray behavior and mixture formation in simulations of direct-injection spark-ignition (DISI) engines are fundamental to ensure proper description of all subsequent processes including ignition, combustion, and emissions. In this work, the spray evolution in a single-cylinder optical DISI engine was studied experimentally and numerically with the goal of enabling predictive computational fluid dynamics (CFD) modeling of in-cylinder sprays. The authors explored a wide range of operating conditions characterized by several fuel injection temperatures and engine speeds, using a well-characterized nine-component gasoline surrogate known as PACE-20. The effect of flash boiling and intake crossflow on the spray is discussed, with a focus on evaluating the ability of the spray models to capture highly transient spray behavior. In the experiments, the fuel temperature was varied between 20°C and 80°C, allowing for non-flash- to flash-boiling transition to emerge with enhanced flashing intensity at the highest temperatures. Spray collapse resulted in vapor-rich regions, owing to the locally lower inertia of the fluid. Varying the engine speed from 650 to 1950 rpm promoted increasingly more turbulent in-cylinder crossflow which interacted with the spray during the injection event and resulted in enhanced spray dispersion. The CFD model was able to capture the spray morphology transition at different fuel temperatures and engine speeds adequately. Further, it is shown that the spray breakup model could capture the transitional spray behavior induced by flash boiling atomization and intake flow via proper initialization of the spray cone angle and calibration of the spray models’ constants.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2020

Atomic electron tomography in three and four dimensions

Atomic electron tomography (AET) has become a powerful tool for atomic-scale structural characterization in three and four dimensions. It provides the ability to correlate structures and properties of materials at the single-atom level. With recent advances in data acquisition methods, iterative three-dimensional (3D) reconstruction algorithms, and post-processing methods, AET can now determine 3D atomic coordinates and chemical species with sub-Angstrom precision, and reveal their atomic-scale time evolution during dynamical processes. In this work, we review the recent experimental and algorithmic developments of AET and highlight several groundbreaking experiments, which include pinpointing the 3D atom positions and chemical order/disorder in technologically relevant materials and capturing how atoms rearrange during early nucleation at four-dimensional atomic resolution.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2023

Photoinduced modification of optical properties of ferroelectric PZT thin films

This study investigates ultrafast photoinduced changes in optical properties of ferroelectrics (PZT) on femtosecond to nanosecond timescales, using broadband transient reflectivity studies. Surprisingly, spectral features were observed below the bandgap, which could not be attributed to ground state bleaching, excited state absorption, and/or stimulated emission. A model based on probe energy independent changes in refractive index and extinction coefficient showed good agreement with experimental results. Three relaxation processes were phenomenologically considered for the temporal evolution. Laser-induced heating was ruled out as the cause of short timescale behavior and photorefractive effect was suggested as a potential mechanism for changes in the optical properties.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Peridynamic Theory as a New Paradigm for Multiscale Modeling of Sintering

Sintering is a component fabrication process in which powder is compacted by pressing or some other means and then held at elevated temperature for a period of hours. The powder grains bond with each other, leading to the formation of a solid component with much lower porosity, and therefore higher density and higher strength, than the original powder compact. In this project, we investigated a new way of computationally modeling sintering at the length scale of grains. The model uses a high-fidelity, three-dimensional representation with a few hundred nodes per grain. The numerical model solves the peridynamic equations, in which nonlocal forces allow representation of the attraction, adhesion, and mass diffusion between grains. The deformation of the grains is represented through a viscoelastic material model. The project successfully demonstrated the use of this method to reproduce experimentally observed features of material behavior in sintering, including densification, the evolution of microstructure, and the occurrence of random defects in the sintered solid.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Novel additive manufacturing for plasma facing materials ‐ creating a research pathway for minority students

This project addresses two critical and intertwined challenges in fusion energy, namely the shortage of a broadly trained scientific workforce and the lack of scalable manufacturing solutions for plasma-facing components (PFCs). Through a collaboration among Florida International University (FIU), Miami Dade College (MDC), and Purdue University, the project established structured, reproducible educational and research pathways that recruit and advance students from institutions historically outside the fusion energy enterprise, building the human capital that this field urgently needs. The project integrates the complementary research strengths of FIU and Purdue to investigate flash sintering as a transformative processing route for tungsten-based PFCs. Unlike conventional sintering approaches, flash sintering offers rapid densification at significantly reduced thermal budgets, making it a compelling candidate for fabricating complex tungsten geometries that must withstand extreme plasma-facing environments. Systematic experimental and modeling efforts will elucidate the fundamental mechanisms governing microstructure evolution, grain boundary chemistry, and thermomechanical response during flash sintering — knowledge that is presently lacking but essential for translating this technology into reliable manufacturing practice. The convergence of workforce development and cutting-edge manufacturing research positions this project to deliver measurable, durable impact: a pipeline of fusion-ready researchers cultivated through expanded institutional partnerships, and a validated materials processing framework that accelerates domestic readiness for next-generation fusion reactor construction.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Interference Control of Fano Resonances and Dynamical Imaging of an Electron Wave Packet

The Fano line shape, arising from the interference of pathways for the excitation of discrete and continuum states, plays a fundamental role in many branches of physics, chemistry, and materials science. Exciting the resonance with a high harmonic provides naturally a phase delay between the pathways leading to a complex asymmetry parameter. We demonstrate that its amplitude and phase can be controlled on the femtosecond and attosecond time scales, respectively. With our high-energy-resolution (10-meV) experiment, we dynamically image a resonance-enhanced electron wave packet during its temporal evolution, extracting both the amplitude and the phase. Calculations reproduce our experimental results. Our approach constitutes a method for measuring the photoionization delays of a resonance and enables the reconstruction of the electron wave packet in the time domain. This concept of an interference-controlled Fano line shape is a step toward attosecond quantum optics with potential ramifications into nanoscience and next-generation optical materials.

Han, Meng [ETH Zürich (Switzerland); Kansas State ↗

NASA NTRS1988

A self-injection locked, Q-switched, line-narrowed Ti:Al2O3 laser

Line-narrowing, Q-switched, and self-injection locking are studied independently and as a system. Line narrowing is shown both theoretically and experimentally to depend on the inverse square root of the pulse evolution time interval. Q switching of the Ti:Al2O3 laser is demonstrated and the laser output energy as a function of the Q-switch delay is investigated. Self-injection is demonstrated and the operation of the laser is explored as a function of loss and the Q-switch delay. Self-injection locking is demonstrated and the performance as a function of the Q-switch delay is determined.

Barnes, Norman P.↗

NASA NTRS1991

A study of hydrogen diffusion flames using PDF turbulence model

The application of probability density function (pdf) turbulence models is addressed in this work. For the purpose of accurate prediction of turbulent combustion, an algorithm that combines a conventional CFD flow solver with the Monte Carlo simulation of the pdf evolution equation has been developed. The algorithm has been validated using experimental data for a heated turbulent plane jet. The study of H2-F2 diffusion flames has been carried out using this algorithm. Numerical results compared favorably with experimental data. The computuations show that the flame center shifts as the equivalence ratio changes, and that for the same equivalence ratio, similarity solutions for flames exist.

Hsu, Andrew T.↗

NASA NTRS1994

The solid surface combustion experiment aboard the USML-1 mission

AA Experimental results from the five experiments indicate that flame spread rate increases with increasing ambient oxygen content and pressure. An experiment was conducted aboard STS-50/USML-1 in the solid Surface Combustion Experiment (SSCE) hardware for flame spread over a thin cellulosic fuel in a quiescent oxidizer of 35% oxygen/65% nitrogen at 1.0 atm. pressure in microgravity. The USML-1 test was the fourth of five planned experiments for thin fuels, one performed during each of five Space Shuttle Orbiter flights. Data that were gathered include gas- and solid-phase temperatures and motion picture flame images. Observations of the flame are described and compared to theoretical predictions from steady and unsteady models that include flame radiation from CO2 and H2O. Experimental results from the five esperiments indicate that flame spread rate increases with increasing ambient oxygen content and pressure. The brightness of the flame and the visible soot radiation also increase with increasing spread rate. Steady-state numerical predictions of temperature and spread rate and flame structure trends compare well with experimental results near the flame's leading edge while gradual flame evolution is captured through the unsteady model.

Altenkirch, Robert A.↗

NASA NTRS2003

Step Bunch Evolution on Vicinal Faces of KDP

For in-situ studies of the formation and evolution of step patterns in solution growth, we have assembled an experimental setup based on Michelson interferometry with the growing crystal surface as one of the reflective surfaces. The device allows data collection over a relatively large area (approximately 4 sq. mm) in situ and in real time during growth. The depth resolution is improved over traditional interferometry using phase-shifted images combining by a suitable algorithm. We achieve a depth resolution of approximately 50 Angstroms. Lateral resolution, dependent on the degree of magnification, is around 0.3 to 5 microns. The crystal chosen as a model in this work is potassium dihydrogen phosphate (KDP), the optically non-linear material widely used in frequency doubling applications. Kinetics of KDP crystallization is well studied so that KDP can serve as a benchmark for our investigations. We present quantitative results on the onset, initial stages and development of instabilities in moving step trains on vicinal crystal surfaces at varying supersaturation, flow rate, and flow direction. The kinetics data suggest that at low supersaturations, step bunching is caused by impurity retardation of the steps, while at higher supersaturations, we link the non-linearity during growth to interdependence of the velocity and density of the steps evidenced in independent experiments. The behavior on the surface is very dynamic, small bunches both merge and split from larger bunches as they travel across the facet. We present evidence that despite these dynamics, under steady conditions there exists a limiting value to step bunch height. This height is reached at distances between 600 and 1000 microns from the step source. In our experiments, we observed the retention of this step bunch height limit up to the path of 1500 microns.

Booth, N. A.↗

NASA NTRS2003

Intrinsic Hardware Evolution for the Design and Reconfiguration of Analog Speed Controllers for a DC Motor

Evolvable hardware provides the capability to evolve analog circuits to produce amplifier and filter functions. Conventional analog controller designs employ these same functions. Analog controllers for the control of the shaft speed of a DC motor are evolved on an evolvable hardware platform utilizing a second generation Field Programmable Transistor Array (FPTA2). The performance of an evolved controller is compared to that of a conventional proportional-integral (PI) controller. It is shown that hardware evolution is able to create a compact design that provides good performance, while using considerably less functional electronic components than the conventional design. Additionally, the use of hardware evolution to provide fault tolerance by reconfiguring the design is explored. Experimental results are presented showing that significant recovery of capability can be made in the face of damaging induced faults.

Gwaltney, David A.↗