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All sources NASA NTRS DOE OSTI

DOE OSTI2018

Direct observation of dislocation structure evolution in SRF cavity niobium using electron channeling contrast imaging

Two major goals of superconducting radio frequency cavity research and development are achieving higher accelerating gradient and gaining the highest quality factor, a measure of efficiency. However, the consistent improvement of these performance metrics is restricted by many factors, one of which is microstructural defects, such as dislocation substructures within the material. In this work, dislocation evolution is compared in four samples extracted from a 2.8 mm thick large-grain niobium slice, with tensile axes chosen to generate specific dislocation structures during subsequent deformation. The four samples are (1) as-extracted, (2) extracted and annealed, (3) extracted and then deformed to 40% tensile strain, and (4) extracted, annealed at 800 °C 2 h, and then deformed to 40% strain. Electron channeling contrast imaging was performed on all samples to characterize initial dislocation density and dislocation structure evolution due to annealing and deformation, and related to the mechanical behavior observed in stress-strain curves. A fundamental understanding of dislocation evolution in niobium is necessary to develop computational models to simulate cavity forming, which could enable new processing methods for cavity fabrication to be identified that could lead to improved performance.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2012

Laser speckle-imaging of blood microcirculation in the brain cortex of laboratory rats in stress

The results of experimental approbation of the method of laser full-field speckle-imaging for monitoring the changes in blood microcirculation state of the brain cortex of laboratory rats under the conditions of developing stroke and administration of vasodilating and vasoconstrictive agents are presented. The studies aimed at the choice of the optimal conditions of speckle-image formation and recording were performed and the software implementing an adaptive algorithm for processing the data of measurements was created. The transfer of laser radiation to the probed region of the biotissue was implemented by means of a silica-polymer optical fibre. The problems and prospects of speckle-imaging of cerebral microcirculation of blood in laboratory and clinical conditions are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Photothermal alternative to device fabrication using atomic precision advanced manufacturing techniques

The attachment of dopant precursor molecules to depassivated areas of hydrogen-terminated silicon templated with a scanning tunneling microscope (STM) has been used to create electronic devices with subnanometer precision, typically for quantum physics experiments. This process, which we call atomic precision advanced manufacturing (APAM), dopes silicon beyond the solid-solubility limit and produces electrical and optical characteristics that may also be useful for microelectronic and plasmonic applications. However, scanned probe lithography lacks the throughput required to develop more sophisticated applications. In this work, we demonstrate and characterize an APAM device workflow where scanned probe lithography of the atomic layer resist has been replaced by photolithography. An ultraviolet laser is shown to locally and controllably heat silicon above the temperature required for hydrogen depassivation on a nanosecond timescale, a process resistant to under- and overexposure. STM images indicate a narrow range of energy density where the surface is both depassivated and undamaged. Modeling that accounts for photothermal heating and the subsequent hydrogen desorption kinetics suggests that the silicon surface temperatures reached in our patterning process exceed those required for hydrogen removal in temperature-programmed desorption experiments. A phosphorus-doped van der Pauw structure made by sequentially photodepassivating a predefined area and then exposing it to phosphine is found to have a similar mobility and higher carrier density compared with devices patterned by STM. Lastly, it is also demonstrated that photodepassivation and precursor exposure steps may be performed concomitantly, a potential route to enabling APAM outside of ultrahigh vacuum.

nanoscale devices↗

DOE OSTI2021

Mapping Conductance and Switching Behavior of Graphene Devices In Situ

Graphene is proposed for use in various nanodevice designs, many of which harness emergent quantum properties for device functionality. However, visualization, measurement, and manipulation become nontrivial at nanometer and atomic scales, representing a significant challenge for device fabrication, characterization, and optimization at length scales where quantum effects emerge. Herein, proof of principle results at the crossroads between 2D nanoelectronic devices, e-beam-induced modulation, and imaging with secondary electron e-beam induced currents (SEEBIC) is presented. A device platform compatible with scanning transmission electron microscopy investigations is introduced. Then how the SEEBIC imaging technique can be used to visualize conductance and connectivity in single layer graphene nanodevices, even while supported on a thicker substrate (conditions under which conventional imaging fails) is shown. Finally, it is shown that the SEEBIC imaging technique can detect subtle differences in charge transport through time in nonohmic graphene nanoconstrictions indicating the potential to reveal dynamic electronic processes.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Autonomous fabrication of tailored defect structures in 2D materials using machine learning-enabled scanning transmission electron microscopy

Materials with tailored quantum properties can be engineered from atomic-scale assembly techniques, but existing methods often lack the agility and accuracy to precisely and intelligently control the manufacturing process. Here, we demonstrate a fully autonomous approach for fabricating atomic-level defects using electron beams in scanning transmission electron microscopy (STEM) that combines advanced machine learning and automated beam control. As a proof of concept, we achieved controlled fabrication of MoS-nanowire (MoS-NW) edge structures by iterative and targeted exposure of MoS 2 monolayer to a focused electron beam to selectively eject sulfur atoms, utilizing high-angle annular dark-field (HAADF) imaging for feedback-controlled monitoring of structural evolution of defects. A machine learning framework combining a random forest model and a convolutional neural network (CNN) was developed to decode the HAADF image and accurately identify atomic positions and species. This atomic-level information was then integrated into an autonomous decision-making platform, which applied predefined fabrication strategies to instruct beam control about atomic sites to be ejected. The selected sites were subsequently exposed to a localized electron beam using an FPGA-controlled scan routine with precise control over beam positioning and duration. While the MoS-NW edge structures produced exhibit promising mechanical and electronic properties, the proposed methods to build the autonomous fabrication framework is material-agnostic and can be extended to other 2D materials for the creation of diverse defect structures and heterostructures beyond Mo S2 .

Engineering↗

DOE OSTI2011

Magnetization reversal processes of epitaxial Fe{sub 3}Si films on GaAs(001)

We report magneto-optical Kerr microscopy study of the magnetic reversal behavior of Fe{sub 3}Si/GaAs(100) epitaxial thin films grown by molecular beam epitaxy. Results are described in the context of superconducting quantum interference device and Kerr effect vector magnetometry to study the magnetic switching behavior. By tuning the Fe concentration of the samples from 75% to 83%, we found that the ratio of uniaxial to cubic anisotropy constants {gamma} (=|K{sub u}/K{sub 1}|) would tremendously vary from 0.06 to 0.3. When the field was applied along the easy axis of Fe{sub 3}Si samples, a step feature was observed in the M-H loops. This feature has been resolved in the domain image by Kerr microscopy, in which we observed a two-switching behavior at the field where the step feature occurred. These can be qualitatively understood by considering the ratio {gamma}.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Robust frequency diversity based algorithm for clutter noise reduction of ultrasonic signals using multiple sub-spectrum phase coherence

This paper presents a robust frequency diversity based algorithm for clutter reduction in ultrasonic A-scan waveforms. The performance of conventional spectral-temporal techniques like Split Spectrum Processing (SSP) is highly dependent on the parameter selection, especially when the signal to noise ratio (SNR) is low. Although spatial beamforming offers noise reduction with less sensitivity to parameter variation, phased array techniques are not always available. The proposed algorithm first selects an ascending series of frequency bands. A signal is reconstructed for each selected band in which a defect is present when all frequency components are in uniform sign. Combining all reconstructed signals through averaging gives a probability profile of potential defect position. To facilitate data collection and validate the proposed algorithm, Full Matrix Capture is applied on the austenitic steel and high nickel alloy (HNA) samples with 5MHz transducer arrays. When processing A-scan signals with unrefined parameters, the proposed algorithm enhances SNR by 20dB for both samples and consequently, defects are more visible in B-scan images created from the large amount of A-scan traces. Importantly, the proposed algorithm is considered robust, while SSP is shown to fail on the austenitic steel data and achieves less SNR enhancement on the HNA data.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2026

Laser absorption measurements of temperature, pressure, CO, and CO 2 at near-MHz rates in post-detonation fireballs with comparison to synthetic measurements

A laser absorption spectroscopy (LAS) diagnostic was used to obtain measurements of temperature, pressure, CO, and CO 2 at 500 kHz or 1 MHz in post-detonation fireballs produced by hemispherical samples of pentaerythritol tetranitrate (PETN). A quantum-cascade laser was scanned over multiple CO absorption transitions near 2008.5 cm −1 at 1 MHz, while an interband-cascade laser was scanned over a CO 2 absorption transition near 2394.8 cm −1 at 500 kHz. Light from each laser was combined onto a single path and passed through a detonation chamber approximately 83 mm above the 12-mm diameter hemispherical PETN charge. The CO and CO 2 absorption signals were post-processed to obtain time histories of temperature, pressure, species column pressures (P CO L, P CO2 L), and species column mole fractions (X CO L, X CO2 L). Additionally, schlieren imaging was performed simultaneously at 500 kHz to aid interpretation of the LAS measurements. Experimental and synthetic (i.e., CFD based) LAS measurements were compared to evaluate the accuracy of the CFD model and its ability to model the turbulent afterburning of the detonation products in air. In general, the experimental measurements exhibit reasonable agreement with the synthetic measurements at early times; thereby supporting the accuracy of the CFD model. Periods of disagreement between experimental and synthetic measurements at later times are most likely due to a reflected shock and detonator cavity jetting, which are not accounted for in the CFD model.

Schwartz, Charles J. [Purdue Univ., West Lafayette↗

DOE OSTI2020

Attosecond light science and its application for probing quantum materials

In this paper, we review the development and application of coherent short wavelength light sources implemented using the high harmonic generation (HHG) process. The physics underlying HHG brought quantum physics into the domain of attosecond time-scales for the first time. Here, the observation and manipulation of electron dynamics on such short time-scales—a capability not conceived—of just a few decades ago—is becoming both more-and-more sophisticated and useful as a route to achieve exquisite control over short wavelength light. New experimental techniques are enabling HHG light sources to provide new insights into fundamental quantum interactions in materials, making it possible for the first time to capture the fastest charge, spin, photon and phonon interactions and to achieve diffraction-limited imaging at short wavelengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2018

Generalized, Energy-conserving Numerical Simulations of Particles in General Relativity. I. Time-like and Null Geodesics

The numerical integration of particle trajectories in curved spacetimes is fundamental for obtaining realistic models of the particle dynamics around massive compact objects such as black holes and neutron stars. Generalized algorithms capable of handling generic metrics are needed for studies of both standard (Schwarzschild and Kerr metrics) and nonstandard (e.g., Schwarzschild metric plus nonclassical perturbations or multiple black hole metrics) spacetimes. The most commonly employed explicit numerical schemes (e.g., Runge–Kutta) are incapable of producing highly accurate results at critical points, e.g., in the regions close to the event horizon where gravity causes extreme curvature of the spacetime, at an acceptable computational cost. In this work we describe a generalized algorithm for the numerical integration of time-like (massive particles) and null (photons) geodesics in any given 3 + 1 split spacetime. We introduce a new, exactly energy-conserving implicit integration scheme based on the preservation of the underlying Hamiltonian, and we compare its properties with a standard fourth-order Runge–Kutta explicit scheme and an implicit midpoint scheme. We test the numerical performance of the three schemes against analytic solutions of particle and photon orbits in Schwarzschild and Kerr spacetimes. We additionally prove the versatility of our framework in handling more exotic metrics, such as Morris–Thorne wormholes and quantum-perturbed Schwarzschild black holes. The generalized method is also discussed in the perspective of future extensions to more complex particle dynamics, e.g., the addition of the Lorentz force acting on charged particles, which allows for test particle diagnostics in GRMHD simulations.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

On the turbulent flow in piston engines: Coupling of statistical theory quantities and instantaneous turbulence

Planar particle image velocimetry (PIV) and tomographic PIV (TPIV) measurements are utilized to analyze turbulent statistical theory quantities and the instantaneous turbulence within a single-cylinder optical engine. Measurements are performed during the intake and mid-compression stroke at 800 and 1500 RPM. TPIV facilitates the evaluation of spatially resolved Reynolds stress tensor (RST) distributions, anisotropic Reynolds stress invariants, and instantaneous turbulent vortical structures. The RST analysis describes distributions of individual velocity fluctuation components that arise from unsteady turbulent flow behavior as well as cycle-to-cycle variability (CCV). A conditional analysis, for which instantaneous PIV images are sampled by their tumble center location, reveals that CCV and turbulence have similar contributions to RST distributions at the mean tumble center, but turbulence is dominant in regions peripheral to the tumble center. Analysis of the anisotropic Reynolds stress invariants reveals the spatial distribution of axisymmetric expansion, axisymmetric contraction, and 3D isotropy within the cylinder. Findings indicate that the mid-compression flow exhibits a higher tendency toward 3D isotropy than the intake flow. A novel post-processing algorithm is utilized to classify the geometry of instantaneous turbulent vortical structures and evaluate their frequency of occurrence within the cylinder. Findings are coupled with statistical theory quantities to provide a comprehensive understanding of the distribution of turbulent velocity components, the distribution of anisotropic states of turbulence, and compare the turbulent vortical flow distribution that is theoretically expected to what is experimentally observed. The analyses reveal requisites of important turbulent flow quantities and discern their sensitivity to the local flow topography and engine operation.

42 ENGINEERING↗

DOE OSTI2015

Phase-selective vanadium dioxide (VO{sub 2}) nanostructured thin films by pulsed laser deposition

Thin films of monoclinic nanostructured vanadium dioxide are notoriously difficult to produce in a selective manner. To date, post-annealing, after pulsed laser deposition (PLD), has been used to revert the crystal phase or to remove impurities, and non-glass substrates have been employed, thus reducing the efficacy of the transparency switching. Here, we overcome these limitations in PLD by optimizing a laser-ablation and deposition process through optical imaging of the laser-induced plasma. We report high quality monoclinic rutile-type vanadium dioxide (VO{sub 2}) (M1) nanoparticles without post-annealing, and on a glass substrate. Our samples demonstrate a reversible metal-to-insulator transition at ∼43 °C, without any doping, paving the way to switchable transparency in optical materials at room temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Characterizing Dynamic Structure in Battery Electrodes by Time-Resolved Cryo-TEM

In recent years, cryogenic transmission electron microscopy (cryo-TEM) has enabled high-resolution characterization of sensitive battery materials by minimizing electron beam-induced artifacts and damage. Success of this technique relies on the preparation of thin, rapidly frozen samples, generally by disassembling batteries under inert atmosphere, transferring materials of interest to a TEM grid, and finally plunge freezing into a cryogen. In material degradation studies, this extensive time between electrochemical cycling and cryo-TEM characterization leaves room for structural relaxation, diffusion, and other dynamic processes that make it difficult to precisely correlate the imaged structure with the native structure that evolves during battery cycling or aging. Here, we present a method to integrate battery cycling with fast preparation of electrode samples for cryo-TEM. This enables higher fidelity between the structures characterized and the electrochemical state of interest, which we use to study deformation in silicon nanoparticle anodes for lithium-ion batteries.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗

NASA NTRS2000

Recent Developments and Applications of Quantum Well Infrared Photodetector Focal Plane Arrays

There are many applications that require long wavelength, large, uniform, reproducible, low cost, stable, and radiation-hard infrared (IR) focal plane arrays (FPAs). For example, the absorption lines of many gas molecules, such as ozone, water, carbon monoxide, carbon dioxide, and nitrous oxide occur in the wavelength region from 3 to 18 micron. Thus, IR imaging systems that operate in the long wavelength IR (LWIR) region (6 - 18 micron) are required in many space borne applications such as monitoring the global atmospheric temperature profiles, relative humidity profiles, cloud characteristics, and the distribution of minor constituents in the atmosphere which are being planned for future NASA Earth and planetary remote sensing systems. Due to higher radiation hardness, lower 1/f noise, and larger array size the GaAs based Quantum Well Infrared Photodetector (QWIP) FPAs are very attractive for such space borne applications compared to intrinsic narrow band gap detector arrays. In this presentation we will discuss the optimization of the detector design, material growth and processing that has culminated in realization of large format long-wavelength QWIP FPAs, portable and miniature LWIR cameras, holding forth great promise for myriad applications in 6-18 micron wavelength range in science, medicine, defense and industry. In addition, we will present some system demonstrations using broadband, two-color, and high quantum efficiency long-wavelength QWIP FPAs.

Gunapala, S. D.↗

DOE OSTI2016

Magnetization reversal of the domain structure in the anti-perovskite nitride Co{sub 3}FeN investigated by high-resolution X-ray microscopy

We performed X-ray magnetic circular dichroism (XMCD) photoemission electron microscopy imaging to reveal the magnetic domain structure of anti-perovskite nitride Co{sub 3}FeN exhibiting a negative spin polarization. In square and disc patterns, we systematically and quantitatively determined the statistics of the stable states as a function of geometry. By direct imaging during the application of a magnetic field, we revealed the magnetic reversal process in a spatially resolved manner. We compared the hysteresis on the continuous area and the square patterns from the magnetic field-dependent XMCD ratio, which can be explained as resulting from the effect of the shape anisotropy, present in nanostructured thin films.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

State-to-State Molecular Reactions in the Ultracold Regime (Final Scientific Report)

We have achieved the proposed goal to experimentally probe the AB + CD and AB + C types of reactions with state-to-state resolution, which we also compared to advanced theoretical calculations to help elucidate the role of quantum mechanics in the processes of bond breakage and formation. Our approach uses reactants that are prepared at ultracold temperatures (< 1µK) such that the quantum effects of translational motion are an important factor. Specific example reactions, including the potassium-rubidium metathesis reaction KRb + KRb → K 2 + Rb 2 as well as the atom exchange reaction Rb + KRb → Rb2 + K, are chosen because the technology of quantum internal and motional state control of these types of molecules is particularly advanced. The results for the entire funding period are fruitful. For the majority of this grant, we have constructed a one-of-the-kind quantum degenerate gas apparatus that integrates ion detection and velocity map imaging capabilities, allowing us to explore the KRb + KRb → K 2 + Rb 2 bimolecular reaction in detail. Specifically, we first verified such a reaction indeed proceed at ultracold temperatures by direct detection of reaction products. We then mapped out the complete product state distribution, which was compared to a state-counting model based on statistical theory. Our results show an overall agreement with the statistical state counting model, but also reveal several deviating state-pairs. An exact quantum calculation for molecule-molecule collisions, that is needed to understand these deviations, is however beyond the current state-of-the-art. Beside scrutinizing the reaction products, we also directly observe the reaction intermediate complex, which was quite a surprise to us. The intermediate complexes are long-lived and can interact with the inferred light that we use to trap the ultracold gas. After molecule-molecule collisions, we then explored the more theoretically tractable Rb + KRb reaction, which is endothermic. Surprisingly, we observed an exceedingly long-lived KRb$^*_2$ collisional complexes, with our experimentally measured complex lifetime deviating from conventional theoretical calculations by five orders of magnitude. This discrepancy has motivated many explorations of possible underlying causes, though no model yet captures this phenomenon completely. In the final year and the work that continues today, we extend upon these atom-molecule collision experiments to explore the origin of the long-lived KRb$^*_2$ complex lifetime and develop means to control the outcome of the reaction complex. The 5-year funded work advanced our understanding of chemical reactions at the lowest possible temperatures and at the same time opened up many new questions that are beyond our initial imaginations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Microfluidic electrochemical device and process for chemical imaging and electrochemical analysis at the electrode-liquid interface in-situ

A microfluidic electrochemical device and process are detailed that provide chemical imaging and electrochemical analysis under vacuum at the surface of the electrode-sample or electrode-liquid interface in-situ. The electrochemical device allows investigation of various surface layers including diffuse layers at selected depths populated with, e.g., adsorbed molecules in which chemical transformation in electrolyte solutions occurs.

42 ENGINEERING↗

DOE OSTI2016

Insights on finite size effects in ab initio study of CO adsorption and dissociation on Fe 110 surface

Adsorption and dissociation of hydrocarbons on metallic surfaces represent crucial steps on the path to carburization, eventually leading to dusting corrosion. While adsorption of CO molecules on Fe surface is a barrier-less exothermic process, this is not the case for the dissociation of CO into C and O adatoms and the diffusion of C beneath the surface that are found to be associated with large energy barriers. In practice, these barriers can be affected by numerous factors that combine to favour the CO-Fe reaction such as the abundance of CO and other hydrocarbons as well as the presence of structural defects. From a numerical point of view, studying these factors is challenging and a step-by-step approach is necessary to assess, in particular, the influence of the finite box size on the reaction parameters for adsorption and dissociation of CO on metal surfaces. Here, we use density functional theory (DFT) total energy calculations with the climbing-image nudged elastic band method to estimate the adsorption energies and dissociation barriers for different CO coverages with surface supercells of different sizes. We further compute the effect of periodic boundary condition for DFT calculations and find that the contribution from van der Waals interaction in the computation of adsorption parameters is important as they contribute to correcting the finite-size error in small systems. The dissociation process involves carbon insertion into the Fe surface causing a lattice deformation that requires a larger surface system for unrestricted relaxation. We show that, in the larger surface systems associated with dilute CO-coverages, C-insertion is energetically more favourable, leading to a significant decrease in the dissociation barrier. This observation suggests that a large surface system with dilute coverage is necessary for all similar metal-hydrocarbon reactions in order to study their fundamental electronic mechanisms, as an isolated phenomenon, free from finite-size effects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗