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At least 433 records · Page 24

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DOE OSTI2025

Low-energy electron driven reactions in 2-bromo-5-nitrothiazole

Thiazole derivatives are biologically relevant molecules, used also in pharmaceutical applications. Herein, we report results for electron attachment to 2-bromo-5-nitrothiazole (BNT) in the gas phase. Employing two crossed electron–molecule beam experiments, we determined the efficiency curves of various fragment anions as a function of the initial electron energy between about 0 and 10 eV as well as the emission angle and kinetic energy distributions of Br− and NO2− ions formed from a resonance near 4 eV. The experiments were supported by quantum chemical calculations, exploring possible dissociation pathways along with their reaction energies. We also compared the electron attachment characteristics of BNT with those of the native thiazole molecule by performing electron attachment experiments and calculations for this molecule as well. Compared to thiazole, which is primarily degraded only by electrons with kinetic energies between about 5 and 10 eV, BNT is susceptible to low-energy electrons near 0 eV with enhanced cross section for (dissociative) electron attachment. However, although BNT offers two localization sites with high electron affinity (Br and NO2 moieties), we do not find the corresponding anions as the dominant negatively charged species formed upon electron attachment. Instead, the reaction channels with an abstraction of Br and NO2 as neutral radicals prevail, accompanied by the opening of the thiazole ring due to the relatively weak C–S bond.

Chen, Jiakuan (ORCID:0009000729608641)↗

DOE OSTI2021

Single-crystalline epitaxial TiO film: A metal and superconductor, similar to Ti metal

Titanium monoxide (TiO), an important member of the rock salt 3d transition-metal monoxides, has not been studied in the stoichiometric single-crystal form. It has been challenging to prepare stoichiometric TiO due to the highly reactive Ti 2+ . We adapt a closely lattice-matched MgO(001) substrate and report the successful growth of single-crystalline TiO(001) film using molecular beam epitaxy. This enables a first-time study of stoichiometric TiO thin films, showing that TiO is metal but in proximity to Mott insulating state. We observe a transition to the superconducting phase below 0.5 K close to that of Ti metal. Density functional theory (DFT) and a DFT-based tight-binding model demonstrate the extreme importance of direct Ti–Ti bonding in TiO, suggesting that similar superconductivity exists in TiO and Ti metal. Our work introduces the new concept that TiO behaves more similar to its metal counterpart, distinguishing it from other 3d transition-metal monoxides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Intentional Uranium Tagging for Material Provenance and Pathway Forensics (LA19-Intentional-Forensics-NDD3Bb) (Annual Report for FY21)

This report describes the outcomes of the third and final year of a project to research the feasibility of tagging uranium materials, especially nuclear fuels. The experimental focus remained on metallic uranium forms under prospective surface and bulk tagging scenarios. Overall, the results showed that the tags could be successfully imparted and characterized in both as-built and degraded conditions. This was in line with expectations coming into this project, indicating promise for both surface and bulk tagging of metallic forms of uranium. Multiple surface tagging techniques and detection strategies were explored in FY21, with an emphasis on improving tag quality, readability, and detection in the field. Non-radioactive materials were used as a testbed. Selective deposition via laser beam was determined to be successful in imparting a readable titanium deposit on a stainless steel base plate, and can be read with high resolution characterization techniques (e.g., scanning electron microscopy) and field capable tools (e.g., eddy current testing). Other deposition techniques, such as selective deposition via electron beam and photoluminescent tags, were explored in FY21, and while success for these techniques would be dependent on additional work, these techniques showed potential for surface tagging applications. To survey bulk taggant elements for bulk uranium metal, 16 tagging elements were spread among 18 depleted uranium castings (4 baseline, 3 mix, 1 dilution, and 10 recycle). Most of these were made and characterized in FY21. Taggant acceptability was based upon manufacturability, detectability, and persistence from the standpoint of two detection options: bulk chemical analysis (for “chemical taggants”) and microstructural analysis (for “second phase taggants”). Taggant detection in both up-front manufacturing and in the face of “degradations” such as dilution, mixing, and recycling was generally good. Two independent laboratories carried out chemical analysis on most of the castings, and often at several locations within a casting, and the results are discussed. Scanning electron microscopy+EDS microanalysis revealed the second phases mostly contained the expected tagging elements. The shapes and 2 spatial distributions of these micron-sized carbides, oxides, and intermetallic particles offers opportunities for further science-based investigation and tagging optimization. Overall, V and Co currently appear as the best choices for chemical taggants while Al, Ti, Mn, Co, Pd, and Tb all look good as second phase taggants. The other elements considered here – Sc, Ni, Ge, Nb, Ce, Ta, W, Ir, and Au – while not being ruled out, require more study to become viable options. It is of special note that in the recycling study only one of the 12 elements fell out of detection even after 10 meltings, demonstrating their persistence. An Appendix tabulates all chemical analysis results to enable more quantitative and statistical studies of detection opportunities and limitations, as a part of a related project.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Self-assembled nanocolumns in Bi 2 Se 3 grown by molecular beam epitaxy

Layered van der Waals (vdW) materials grown by physical vapor deposition techniques are generally assumed to have a weak interaction with the substrate during growth. This leads to films with relatively small domains that are usually triangular and a terraced morphology. In this paper, we demonstrate that Bi 2 Se 3 , a prototypical vdW material, will form a nano-column morphology when grown on GaAs(001) substrates. This morphology is explained by a relatively strong film/substrate interaction, long adatom diffusion lengths, and a high reactive selenium flux. In conclusion, this discovery paves the way toward growth of self-assembled vdW structures even in the absence of strain.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Nanoscale decoupling of electronic nematicity and structural anisotropy in FeSe thin films

In a material prone to a nematic instability, anisotropic strain in principle provides a preferred symmetry-breaking direction for the electronic nematic state to follow. This is consistent with experimental observations, where electronic nematicity and structural anisotropy typically appear hand-in-hand. In this work, we discover that electronic nematicity can be locally decoupled from the underlying structural anisotropy in strain-engineered iron-selenide (FeSe) thin films. We use heteroepitaxial molecular beam epitaxy to grow FeSe with a nanoscale network of modulations that give rise to spatially varying strain. We map local anisotropic strain by analyzing scanning tunneling microscopy topographs, and visualize electronic nematic domains from concomitant spectroscopic maps. While the domains form so that the energy of nemato-elastic coupling is minimized, we observe distinct regions where electronic nematic ordering fails to flip direction, even though the underlying structural anisotropy is locally reversed. The findings point towards a nanometer-scale stiffness of the nematic order parameter.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Magnetic undulator shim

A magnetic undulator shim having three interconnected sections arranged one after the other in a direction substantially parallel to the beam axis. The first section is adapted to magnetically engage a magnet having a horizontal surface and configured to extend partially onto the horizontal surface of the magnet. The magnet is adjacent to a pole and the magnet and the pole form a boundary. The second third sections are interconnected to form a shape. The shape corresponds to the boundary. The third section is adapted to magnetically engage a surface of the pole.

Xu, Joseph Z.↗

DOE OSTI2023

Neutron Magnetic Form Factor GNM Measurement at High Q2 with CLAS12

The neutron magnetic form factor, GnM , is a fundamental quantity that describes how magnetic properties are distributed within a neutron. This measurement provides insights into the internal structure of the neutron. Furthermore, by measuring GnM alongside three other form factors (GnE , GpE , GpM ), we can test the predictions of Quantum Chromodynamics (QCD), which is the fundamental theory governing the strong force that binds quarks and gluons. Additionally, these measurements play a significant role in constraining Generalized Parton Distributions (GPDs) and contribute to determining the angular momentum of the quarks within nucleons. The GnM was measured using the ratio of quasi-elastic e ? n to e ? p scattering from a deuteron target. The measurement covered a range of four-momentum transfer squared, Q2, from 5 to 12 GeV2, using three different beam energies (10.2, 10.4, and 10.6 GeV). The data is compared with previous measurements and several theoretical models. The preliminary results reveal that Gn M exceeds the predictions of the standard dipole parametrization by 12-20%, based on RG-B pass1 data. It is expected that this deviation from the standard dipole parametrization will diminish as we transition to using RG-B pass2 data, aligning GnM more closely with the dipole form factor. The ongoing RG-B pass2 analysis in CLAS12 holds considerable promise for significant improvement. This enhancement is achievable through collaborative efforts aimed at refining tracking efficiency, momentum correction, calibration, and alignment.

Baashen, Lamya↗

DOE OSTI2023

Systems and methods of electron beam induced processing

Embodiments of the present disclosure provide for methods and systems for making structures using an electrospray system while under vacuum. In particular, embodiments of the present disclosure provide for methods and systems for ultra-fast growth of high aspect ratio nano/meso/micro-structures with three dimensional topological complexity and control of phase and composition of the structure formed.

Fedorov, Andrei G.↗

DOE OSTI2024

Systems and methods of electron beam induced processing

Fedorov, Andrei G.↗

DOE OSTI2022

Production of high fluence laser beams using ion wave plasma optics

Optical components for laser beams with high peak and averaged powers are being developed worldwide using stimulated plasma scattering that occurs when plasmas interact with intense, coherent light. After decades of pursuit of pulse compressors, mirrors, and other plasma based components that can be created by stimulated scattering from electron density perturbations forming on ultra-short time scales (e.g., via Stimulated Raman Scattering), more recent work has produced optical components on longer time scales allowing ion motion as well [via Stimulated Brillouin Scattering (SBS)]. In the most recent work, ion wave plasma optics have had success in producing pulses of focusable coherent light with high energy and fluence by operating on ns time scales and now promise to enable numerous applications. Experiments have further shown that in some parameter regimes, even simple plasma response models can describe the output of such optics with sufficient accuracy that they can be used as engineering tools to design plasma optics for future applications, as is already being done to control power deposition in fusion targets. In addition, the development of more sophisticated models promises to enable still higher performance from SBS driven plasma optical components under a wider range of conditions. The present status and most promising directions for future development of ion wave plasma optic techniques are discussed here.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Curvilinear magnetic effects in helicoid nanotubes

We report the fabrication and characterization of ferromagnetic helicoid nanotubes with a tunable surface curvature and chirality. Through combining focused electron beam induced deposition and magnetron sputtering we realize these complex curvilinear magnetic architectures. Electron holography reveals two distinct states: a single domain remanent state, with a magnetic chirality governed by the geometric chirality, and a vortex-anti-vortex domain wall, preferentially forming at areas of lower curvature. Micromagnetic simulations reveal how the geometry, specifically pitch and local surface curvature, affects the stability and formation of magnetic domain walls. Furthermore, we show that the interplay between magnetic and geometric chirality has a strong impact on domain wall motion, whereby a right-handed geometric chirality leads to faster domain wall motion and a left-handed geometry hinders domain wall transport. The results shown here highlight the potential of 3D magnetic architectures in spintronic devices and offer insights into how geometry and curvature affect the magnetization, the distribution of magnetic solitons and the motion of domain walls.

3D Nanomagnetism↗

DOE OSTI2025

Characterization of uncertainties in electron-argon collision cross sections

Abstract The predictive capability of a plasma discharge model depends on accurate representations of electron-impact collision cross sections, which determine the corresponding reaction rates and electron transport properties. The values of cross sections can be known only approximately either through experiments or simulations and are thus subject to uncertainties. Quantifying the uncertainties in plasma simulations allows us to assess the reliability of simulations and to provide a basis for interpreting discrepancies between simulations and experiments. For such uncertainty quantification of plasma simulations, it is essential to quantify the uncertainties of the underlying cross sections. Although much effort has been committed to calibrate the cross section values, their uncertainties are not well investigated. We characterize uncertainties in electron-argon atom collision cross sections using a Bayesian framework. Six collision processes—elastic momentum transfer, ionization, and four excitations—are characterized with semi-empirical models, which effectively capture the features important to the macroscopic properties of the plasma. A probability model for the uncertain parameters of these semi-empirical models is developed. Specifically, a Gaussian-process likelihood model is proposed to capture discrepancies among data sets, as well as the model-form inadequacies of the semi-empirical models. Two other likelihood models are compared with the proposed Gaussian-process model, to illustrate the importance of the choice of the likelihood model. The cross section models are calibrated using the electron-beam experiments and ab-inito quantum simulations. The resulting calibrated uncertainties capture well the scattering among the data sets. The calibrated cross section models are further validated against swarm-parameter experiments and zero-dimensional Boltzmann equation simulations of widely used cross section datasets.

Chung, Seung Whan (ORCID:0000000302501549)↗

DOE OSTI2023

Subcomponent Validation of Composite Joints for the Marine Energy Advanced Materials Project

The Marine Energy Advanced Materials project is an ongoing multi-year, multi-lab project with the main goals of addressing barriers and uncertainties facing marine energy developers in adopting advanced materials for structural applications. NREL's goals of the project were to address subcomponents testing needs for marine energy materials, to improve understanding of design allowables at the full-scale and provide near net-scale static and fatigue data of composite subcomponents using materials applicable to the marine energy industry. In the long term, the test method development and data generated would be used to inform standards development. This report outlines perhaps one of the largest-scale studies conducted with regards to saltwater conditioning of various composite material subcomponents and their subsequent structural validation, specifically directed at the marine renewable energy industry. A variety of fiberglass composite panels with epoxy and vinyl ester epoxy resin systems were manufactured at Montana State University, which were then used to manufacture an array of different types of subcomponent test specimens at the National Renewable Energy Laboratory's Flatirons Campus. These subcomponents were in the form of T-bolt and double-ended-insert specimens, which were intended to represent bonded and mechanical bolted connections for thick composite laminates, metal-metal and composite lap shear specimens to evaluate adhesion of constituent materials, and adhesive beam-shear specimens as part of an effort to better evaluate the characteristics of thick adhesive bondlines. Overall, the materials used were fiberglass reinforced epoxy and vinyl ester matrix composites, epoxy and methacrylate adhesives, and 316 and 2507 stainless steels. Specimens were then conditioned in salt water at various temperatures and for various periods of time at Florida Atlantic University and Pacific Northwest National Laboratory. All specimens were then mechanically characterized and validated using various test methods under static and fatigue loading conditions at NREL's Structural Technology Laboratory. Throughout the conditioning and mechanical validation process, valuable experience was gained, which will help guide future test method development for marine energy materials. In many instances, the results indicated similar observations as to what had been observed during previous coupon scale characterization efforts that provided a vital understanding of the scale up process. However in some instances, unexpected phenomena were observed, such as interactions between the adhesives and 316 steel. Furthermore, some materials exhibited significant degradation due to the saltwater conditioning. Ultimately, this report provides a detailed summary of the specimens that were designed, the subcomponent test methods that were developed, and the results that were generated, which will serve as important guidance for marine renewable energy developers and researchers for future structural designs and validation.

16 TIDAL AND WAVE POWER↗

DOE OSTI2020

Gas phase formation of cyclopentanaphthalene (benzindene) isomers via reactions of 5- and 6-indenyl radicals with vinylacetylene

The tricyclic polycyclic aromatic hydrocarbons (PAHs) 3H-cyclopenta[a]naphthalene (C 13 H 10 ), 1H-cyclopenta[b]naphthalene (C 13 H 10 ) and 1H-cyclopenta[a]naphthalene (C 13 H 10 ) along with their indene-based bicyclic isomers (E)-5-(but-1-en-3-yn-1-yl)-1H-indene, (E)-6-(but-1-en-3-yn-1-yl)-1H-indene, 5-(but-3-ene-1-yn-1-yl)-1H-in-dene, and 6-(but-3-ene-1-yn-1-yl)-1H-indene were formed via a “directed synthesis” in a high-temperature chemical micro reactor at the temperature of 1300 ± 10 K through the reactions of the 5- and 6-indenyl radicals (C 9 H 7 ˙) with vinylacetylene (C 4 H 4 ). The isomer distributions were probed utilizing tunable vacuum ultraviolet light by recording the photoionization efficiency curves at mass-to-charge of m/z = 166 (C 13 H 10 ) and 167 ( 13 CC 12 H 10 ) of the products in a supersonic molecular beam. Here, the underlying reaction mechanisms involve the initial formation of van-der-Waals complexes followed by addition of the 5- and 6-indenyl radicals to vinylacetylene via submerged barriers, followed by isomerization (hydrogen shifts, ring closures), and termination via atomic hydrogen elimination accompanied by aromatization. All the barriers involved in the formation of 3H-cyclopenta[a]naphthalene, 1H-cyclopenta[b]naphthalene and 1H-cyclopenta[a]naphthalene are submerged with respect to the reactants indicating that the mechanisms are in fact barrierless, potentially forming PAHs via the hydrogen abstraction – vinylacetylene addition (HAVA) pathway in the cold molecular clouds such as Taurus Molecular Cloud-1 (TMC-1) at temperatures as low as 10 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Self‐Assembled Monolayer Templating for Engineered Nanopinholes in Passivated Contact Solar Cells

We present a novel self-assembled monolayer (SAM)-based technique to make nanopinhole-enabled passivated contacts on silicon solar cells by tuning the SAM coverage area and etch selectivity. We deposit trimethyl-silyl Si(CH 3 ) 3 groups using hexamethyldisilazane (HMDS) as the precursor over passivating dielectric layers and their stacks (SiO 2 , SiN x , SiO 2 /SiN x ) and interrupt the HMDS attachment chemistry shortly before a full monolayer is formed on its surface. Subsequent etching in dilute HF produces pinholes through the dielectric layers due to the higher etch resistance of the SAM to HF etching. The pinhole areal density (10 4 –10 8 /cm 2 ) and size (10–1000 nm) can be tuned both by duration of HMDS attachment and HF etch time. Pinholes were characterized by atomic force microscopy, tetramethylammonium hydroxide (TMAH) selective etch, and Ag decoration by electroless plating. Polysilicon (poly-Si) passivated contacts enabled by pinholes were formed by subsequent deposition of doped amorphous silicon (a-Si:H) followed by thermal crystallization and dopant drive-in. At optimal areal pinhole density ≈10 7 /cm 2 , contacts exhibit both passivation and carrier transport via pinholes as evidenced by electron beam induced current, transmission line measurements, and carrier lifetime measurements. Solar cells based with these pinhole contacts show V oc = 723 mV and FF = 80.3%. The remaining SAM layer does not affect device performance.

14 SOLAR ENERGY↗

DOE OSTI2026

Mechanism of Vapor-Phase Infiltration of Organometallic Hf in Poly(Methyl Methacrylate) for Hybrid Resist Applications

Inorganic–organic hybrid thin films synthesized by vapor-phase infiltration (VPI) of metal oxides into organic photoresists, such as poly(methyl methacrylate) (PMMA), have recently demonstrated their utility in extreme ultraviolet lithography, critical for angstrom-era semiconductor device miniaturization. Hafnium oxide infiltration has been reported recently for this purpose, but its detailed VPI mechanism has remained largely unexplored. In this study, we investigated the VPI characteristics and mechanisms of tetrakis(dimethylamido)hafnium (TDMAHf)─the hafnium precursor predominantly used for VPI in the field─into PMMA and examined its impact on electron-beam lithography (EBL) exposure behavior. VPI was performed at temperatures ranging from 85 to 150 °C, with chemical interactions characterized using infrared reflection-absorption spectroscopy, and resist patterning performance was evaluated through EBL dose-sensitivity assessments. The results indicate that TDMAHf forms a reversible adduct with PMMA at temperatures up to 120 °C, whereas at 150 °C, covalent bond formation occurs, most likely via dealkylation that leads to acetate formation. EBL studies reveal that resist sensitivity is influenced by both infiltration temperature and developer selection, with aqueous isopropyl alcohol development demonstrating enhanced sensitivity compared to organic solvent-based development. The optimized infiltration protocol at 120 °C ensures a uniform inorganic distribution without compromising resist dissolution. These findings not only help refine hybrid resist patterning performance but also offer insights potentially applicable to the VPI of other homoleptic metal-amide organometallic VPI precursors that include TDMA ligands.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Light-Matter Interaction near the Schwinger Limit Using Tightly Focused Doppler-Boosted Lasers

Strong-field quantum electrodynamics (SF QED) is a burgeoning research topic dealing with electromagnetic fields comparable to the Schwinger field (≈1.32×10 18 V/m). While most past and proposed experiments rely on reaching this field in the rest frame of relativistic particles, the Schwinger limit could also be approached in the laboratory frame by focusing to its diffraction limit the light reflected by a plasma mirror irradiated by a multipetawatt laser. Here, we explore the interaction between such intense light and matter with particle-in-cell simulations. We find that the collision with a relativistic electron beam would enable the study of the nonperturbative regime of SF QED, while the interaction with a solid target leads to a profusion of SF QED effects that retroact on the interaction. In both cases, relativistic attosecond pair jets with high densities are formed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Dry etching of epitaxial InGaAs/InAlAs/InAlGaAs structures for fabrication of photonic integrated circuits

A dry etching process to transfer the pattern of a photonic integrated circuit design for high-speed laser communications is described. The laser stack under consideration is a 3.2-µm-thick InGaAs/InAlAs/InAlGaAs epitaxial structure grown by molecular beam epitaxy. The etching was performed using Cl2-based inductively-coupled-plasma and reactive-ion-etching (ICP-RIE) reactors. Four different recipes are presented in two similar ICP-RIE reactors, with special attention paid to the etched features formed with various hard mask compositions, in-situ passivations, and process temperatures. The results indicate that it is possible to produce high-aspect-ratio features with sub-micron separation on this multilayer structure. Additionally, the results of the etching highlight the tradeoffs involved with the corresponding recipes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗