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DOE OSTI2026

Assessing metal nitrides and metal carbides as supports for thermally stable single-atom catalysts

Single-atom catalysts supported on metal oxides have been demonstrated to exhibit exceptional activity while also maintaining single-atom stability. However, alternative supports such as metal nitrides and carbides have received far less attention. Herein, we use density functional theory to systematically investigate the relative thermal stability of single-atom catalysts over a host of transition metal nitride and carbide supports. By considering the binding and dimerization energies of isolated transition metal atoms across various surface facets, we identify transition metal/support pairs that show the most promise for high-density single-atom catalysts. We find that transition metal atoms can be stabilized on both defect sites and pristine surfaces over transition metal nitrides and carbides. Furthermore, we identify promising metal/support pairings that may be suitable for achieving both stable and high-density single-atom catalysts. Furthermore, these results provide valuable insights to guide synthesis efforts towards achieving stable single-atom transition metal catalysts.

Density functional theory↗

DOE OSTI2013

The enhanced ASDEX Upgrade pellet centrifuge launcher

Pellets played an important role in the program of ASDEX Upgrade serving both for investigations on efficient particle fuelling and high density scenarios but also for pioneering work on Edge Localised Mode (ELM) pacing and mitigation. Initially designed for launching fuelling pellets from the magnetic low field side, the system was converted already some time ago to inject pellets from the magnetic high field side as much higher fuelling efficiency was found using this configuration. In operation for more than 20 years, the pellet launching system had to undergo a major revision and upgrading, in particular of its control system. Furthermore, the control system installed adjacent to the launcher had to be transferred to a more distant location enforcing a complete galvanic separation from torus potential and a fully remote control solution. Changing from a hybrid system consisting of PLC S5/S7 and some hard wired relay control to a state of the art PLC system allowed the introduction of several new operational options enabling more flexibility in the pellet experiments. This article describes the new system architecture of control hardware and software, the operating procedure, and the extended operational window. First successful applications for ELM pacing and triggering studies are presented as well as utilization for the development of high density scenarios.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2016

NH{sub 3}(3,3) AND CH{sub 3}OH NEAR SUPERNOVA REMNANTS: GBT AND VLA OBSERVATIONS

We report on Green Bank Telescope 23.87 GHz NH{sub 3}(3,3) emission observations in five supernova remnants (SNRs) interacting with molecular clouds (G1.4−0.1, IC 443, W44, W51C, and G5.7−0.0). The observations show a clumpy gas density distribution, and in most cases the narrow line widths of ∼3–4 km s{sup −1} are suggestive of maser emission. Very Large Array observations reveal 36 and/or 44 GHz CH{sub 3}OH maser emission in a majority (72%) of the NH{sub 3} peak positions toward three of these SNRs. This good positional correlation is in agreement with the high densities required for the excitation of each line. Through these observations we have shown that CH{sub 3}OH and NH{sub 3} maser emission can be used as indicators of high-density clumps of gas shocked by SNRs, and provide density estimates thereof. Modeling of the optical depth of the NH{sub 3}(3,3) emission is compared to that of CH{sub 3}OH, constraining the densities of the clumps to a typical density of the order of 10{sup 5} cm{sup −3} for cospatial masers. Regions of gas with this density are found to exist in the post-shocked gas quite close to the SNR shock front, and may be associated with sites where cosmic rays produce gamma-ray emission via neutral pion decay.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Optical and Plasmonic Properties of High-Electron-Density Epitaxial and Oxidative Controlled Titanium Nitride Thin Films

The present paper reports on the fabrication, detailed structural characterizations, and theoretical modeling of titanium nitride (TiN) and its isostructural oxide derivative, titanium oxynitride (TiNO) thin films that have excellent plasmonic properties and that also have the potential to overcome the limitation of noble metal and refractory metals. The TiNO films deposited at 700 °C in high vacuum conditions have the highest reflectance (R = ~ 95%), largest negative dielectric constant (ε 1 = –161), and maximal plasmonic figure of merit (FoM = –ε 1 /ε 2 ) of 1.2, followed by the 600 °C samples deposited in a vacuum (R = ~ 85%, ε 1 = –145, FoM = 0.8) and 700 °C–5 mTorr sample (R = ~ 82%, ε 1 = –8, FoM = 0.3). To corroborate our experimental observations, we calculated the phonon dispersions and Raman active modes of TiNO by using the virtual crystal approximation. From the experimental and theoretical studies, a multilayer optical model has been proposed for the TiN/TiNO epitaxial thin films for obtaining individual complex dielectric functions from which many other optical parameters can be calculated. The advantages of oxide derivatives of TiN are the continuation of similar free electron density as in TiN and the acquisition of additional features such as oxygen-dependent semiconductivity with a tunable bandgap.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2013

Influence of thermal agitation on the electric field induced precessional magnetization reversal with perpendicular easy axis

We investigated the influence of thermal agitation on the electric field induced precessional magnetization switching probability with perpendicular easy axis by solving the Fokker-Planck equation numerically with finite difference method. The calculated results show that the thermal agitation during the reversal process crucially influences the switching probability. The switching probability can be achieved is only determined by the thermal stability factor Δ of the free layer, it is independent on the device dimension, which is important for the high density device application. Ultra-low error rate down to the order of 10{sup −9} can be achieved for the device of thermal stability factor Δ of 40. Low damping factor α material should be used for the free layer for high reliability device applications. These results exhibit potential of electric field induced precessional magnetization switching with perpendicular easy axis for ultra-low power, high speed and high density magnetic random access memory (MRAM) applications.

36 MATERIALS SCIENCE↗

NASA NTRS2019

A Dissection of Spatially Resolved AGN Feedback across the Electromagnetic Spectrum

We present optical SuperNova Integral Field Spectrograph integral field spectroscopy, Hubble Space Telescope optical imaging, Chandra X-ray imaging, and Very Large Array radio interferometry of the merging galaxy 2MASX J04234080+0408017, which hosts a Seyfert 2 active galactic nucleus (AGN) at z = 0.046. Our observations reveal that radiatively driven, ionized gas outflows are successful to distances >10 kpc due to the low mass of the host system, encompassing the entirety of the observed optical emission. We also find that at large radii, where observed velocities cannot be reproduced by radiative driving models, high-velocity kinematics are likely due to mechanical driving from AGN winds impacting high-density host material. This impacting deposits sufficient energy to shock the host material, producing thermal X-ray emission and cosmic rays, which in turn promote the formation of in situ radio structure in a pseudo-jet morphology along the high-density lanes.

Travis Fischer↗

DOE OSTI2018

Increasing stagnation pressure and thermonuclear performance of inertial confinement fusion capsules by the introduction of a high-Z dopant

Inertial confinement fusion requires the inertia of the imploding mass to provide the necessary confinement such that the core reaches adequate high density, temperature, and pressure. Studies utilize low-Z capsules filled with hydrogenic fuel, which are subject to multiple instabilities at the interfaces during the implosion. To improve the stability of the fuel:capsule interface and narrow the imploding shell profile, capsules are doped with a small atomic percentage of a high-Z material. A series of recent indirect-drive experiments executed at the National Ignition Facility with tungsten-doped high density carbon capsules has demonstrated that the presence of this dopant serves to increase the in-flight aspect ratio of the shell and increase the compression and neutron yield performance of both gas-filled and deuterium-tritium cryogenically layered targets. These experiments definitively show that benefits accrued by the introduction of a high-Z dopant into the capsule can outweigh the detrimentally reduced stability of the ablation front, avoiding shell breakup or significant radiative cooling of the hot spot. Future experiments will utilize these types of capsules to additionally increase nuclear performance.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Modes of strain accommodation in Cu-Nb multilayered thin film on indentation and cyclic shear

Two-phase layered thin films with a high density of semi-coherent interfaces exhibit excellent mechanical properties and thermal stability. Here, in this study, a magnetron-sputtered Cu-Nb dual-layered thin film (~500 nm for Cu and ~150 nm for Nb) having an amorphous interface between Cu and Nb with a high density of aligned growth twins in Cu is subjected to severe surface deformation. The material is loaded using indentation and cyclic shear under tribological testing. The strain accommodation in the subsurface microstructure after deformation varies based on the local structure and deformation mode. Grain refinement and crack formations in the stressed region of the Nb layer and localized crystallization of the amorphous interface are observed after indentation and scratch testing. Pronounced detwinning of growth twins in the Cu layer under the cyclic shear strain leaves large dislocations sites and loops which are observed both by high-resolution transmission electron microscopy and experiment-guided molecular dynamic (MD) simulations. Our simulations provided insights into understanding the pathway for the detwinning process under cyclic shear loading.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Electromagnetic effects on dynamics of high-beta filamentary structures

The impacts of the electromagnetic effects on blob dynamics are considered. Electromagnetic BOUT++ simulations on seeded high-beta blobs demonstrate that inhomogeneity of magnetic curvature or plasma pressure along the filament leads to bending of the blob filaments and the magnetic field lines due to increased propagation time of plasma current (Alfvén time). The bending motion can enhance heat exchange between the plasma facing materials and the inner scrape-off layer (SOL) region. The effects of sheath boundary conditions on the part of the blob away from the boundary are also diminished by the increased Alfvén time. Using linear analysis and BOUT++ simulations, it is found that electromagnetic effects in high temperature and high density plasmas reduce the growth rate of resistive drift wave instability when resistivity drops below a certain value. The blobs temperature decreases in the course of its motion through the SOL and so the blob can switch from the electromagnetic to the electrostatic regime where resistive drift waves become important again.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Microstructure and high temperature properties of tungsten processed via electron beam melting additive manufacturing

There is considerable interest in the adoption of additive manufacturing for processing refractory metals. The layer-wise fabrication approach enables opportunities for producing complex geometries which cannot be otherwise be achieved via powder metallurgy. However, the processing science is still in its nascent stages and structure–property relations are relatively unexplored. Fundamental research is needed to further develop the technology and enable the fabrication of refractory metals for high temperature applications. Here we focus on the processing of pure tungsten using electron beam melting additive manufacturing. Experimentally we develop a suitable processing window for achieving high density crack free material. Microstructural analysis reveals that the microstructure generally consists of a columnar structure with a (111) build direction fiber preference, although, fiber switching was observed. Process induced deformation is believed to drive the formation of subgrains whose boundaries exhibit a high dislocation density. Additionally, high temperature tensile testing reveals that the material exhibits excellent properties closer to that of annealed tungsten. Significant mechanical anisotropy was observed to be present which is likely driven by strong crystallographic texture.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Supernova remnant KESTEVEN 27: Interaction with a neighbor Hi cloud viewed by Fermi

We report on the likely detection of γ-ray emission from the supernova remnant (SNR) Kesteven 27 (Kes 27). We analyze 5.7 yr Fermi Large Area Telescope data of the SNR region and find an unresolved source at a position consistent with the radio brightness peak and the X-ray knot of Kes 27, which is located in the eastern region of the SNR and caused by its interaction with a nearby Hi cloud. The source’s emission is best fit with a power-law spectrum with a photon index of 2.5 ± 0.1 and a >0.2 GeV luminosity of 5.8×10{sup 34} erg s{sup −1} assuming a distance of 4.3 kpc, as derived from radio observations of the nearby Hi cloud. Comparing the properties of the source with that of other SNRs that are known to be interacting with nearby high-density clouds, we discuss the origin of the source’s emission. The spectral energy distribution of the source can be described by a hadronic model that considers the interaction of energetic protons escaping from the shock front of Kes 27 with a high-density cloud.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Relativistic Hybrid Stars with Sequential First-order Phase Transitions in Light of Multimessenger Constraints

In this work, we consider the properties of compact stars in which quark matter has low- and high-density phases that are separated by a first-order phase transition. Thus, unlike the commonly considered case of a single phase transition from hadronic to quark matter, our models of hybrid stars contain sequential phase transitions from hadronic matter to low- and then to high-density quark matter phases. We extend our previous study of the parameter space of hybrid stars with a single phase transition to those with sequential phase transitions, taking into account the constraints on the mass and radius of neutron stars from the NICER experiment, the experimental inferences of the neutron skin thickness of the lead nucleus by the PREX-II experiment, and constraints on the tidal deformability from the gravitational-wave event GW170817. We determine the range of the masses for which both twin and triplet configurations, i.e., identical-mass stars with two and three different values of radii, arise.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2014

LHCD and ICRF heating experiments in H-mode plasmas on EAST

An ICRF system with power up to 6.0 MW and a LHCD system up to 4MW have been applied for heating and current drive experiments on EAST. Intensive lithium wall coating was intensively used to reduce particle recycling and Hydrogen concentration in Deuterium plasma, which is needed for effective ICRF and LHCD power absorption in high density plasmas. Significant progress has been made with ICRF heating and LHW current drive for realizing the H-mode plasma operation in EAST. In 2010, H-mode was generated and sustained by LHCD alone, where lithium coating and gas puffing launcher mouth were applied to improve the LHCD power coupling and penetration into the core plasmas at high density of H-modes. During the last two experimental campaigns, ICRF Heating experiments were carried out at the fixed frequency of 27MHz, achieving effective ions and electrons heating with the H Minority Heating (H-MH) mode, where electrons are predominantly heated by collisions with high energy minority ions. The H-MH mode gave the best plasma performance, and realized H-mode alone in 2012. Combination of ICRF and LHW power injection generated the H-mode plasmas with various ELMy characteristics. The first successful application of the ICRF Heating in the D (He3) plasma was also achieved. The progress on ICRF heating, LHCD experiments and their application in achieving H-mode operation from last two years will be discussed in this report.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

A finite element procedure for radio-frequency sheath–plasma interactions based on a sheath impedance model

A finite element code that solves self-consistent radio-frequency (RF) sheath-plasma interaction problems is improved by incorporating a generalized sheath boundary condition in the macroscopic solution scheme. This sheath boundary condition makes use of a complex sheath impedance including both the sheath capacitance and resistance, which enables evaluation of not only the RF voltage across the sheath but also the power dissipation in the sheath. The newly developed finite element procedure is applied to cases where the background magnetic field is perpendicular to the sheath surface in one- and two-dimensional domains filled by uniform low- and high-density plasmas. The numerical results are compared with those obtained by employing the previous capacitive sheath model at a typical frequency for ion cyclotron heating used in fusion experiments. It is shown that for sheaths on the order of 100 V in a high-density plasma, localized RF power deposition can reach a level which causes material damage. It is also shown that the sheath-plasma wave resonances predicted by the capacitive sheath model do not occur when parameters are such that the generalized sheath impedance model substantially modifies the capacitive character of the sheath. Here, possible explanations for the difference in the maximum RF sheath voltage depending on the plasma density are also discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2016

High-mass twins & resolution of the reconfinement, masquerade and hyperon puzzles of compact star interiors

We aim at contributing to the resolution of three of the fundamental puzzles related to the still unsolved problem of the structure of the dense core of compact stars (CS): (i) the hyperon puzzle: how to reconcile pulsar masses of 2 M{sub ⊙} with the hyperon softening of the equation of state (EoS); (ii) the masquerade problem: modern EoS for cold, high density hadronic and quark matter are almost identical; and (iii) the reconfinement puzzle: what to do when after a deconfinement transition the hadronic EoS becomes favorable again? We show that taking into account the compositeness of baryons (by excluded volume and/or quark Pauli blocking) on the hadronic side and confining and stiffening effects on the quark matter side results in an early phase transition to quark matter with sufficient stiffening at high densities which removes all three present-day puzzles of CS interiors. Moreover, in this new class of EoS for hybrid CS falls the interesting case of a strong first order phase transition which results in the observable high mass twin star phenomenon, an astrophysical observation of a critical endpoint in the QCD phase diagram.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Dual Passivation of Cathode and Anode through Electrode–Electrolyte Interface Engineering Enables Long-Lifespan Li Metal–SPAN Batteries

The reliability and durability of lithium metal (Li 0 )–sulfur batteries are largely limited by the undesired Li 0 plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. In this study, we report the stable operation of a Li 0 -SPAN (sulfurized polyacrylonitrile) battery via an anode–cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li 3 N-forming additive (TMS-N 3 ), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li 0 anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li 0 plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li 2 S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/g SPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode–electrolyte interphase engineering strategy has tackled the major limitations of Li–S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from –10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li 0 -S batteries.

25 ENERGY STORAGE↗

DOE OSTI2021

Cookoff of Powdered and Pressed Explosives using a Micromechanics Pressurization Model

Cookoff experiments of powdered and pressed TATB-based plastic bonded explosives (PBXs) have been modeled using a pressure-dependent universal cookoff model (UCM) in combination with a micromechanics pressurization (MMP) model described in a companion paper. The MMP model is based on the accumulation of decomposition gases at nucleation sites that load the surrounding TATB crystals and binder. This is the first cookoff model to use an analytical mechanics solution for compressibility and thermal expansion to describe internal pressurization caused by both temperature and decomposition occurring within closed-pore explosives. This approach produces more accurate predictions of ignition time and pressurization within high-density explosives than simple equation-of-state models. The current paper gives details of the reaction chemistry, model parameters, predicted uncertainty, and validation using experiments from multiple laboratories with errors less than 6 %. The UCM/MMP model framework gives more accurate thermal ignition predictions for high density explosives that are initially impermeable to decomposition gases.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2016

Enhancement of diffraction efficiency of laminar-type diffraction gratings overcoated with diamond-like carbon (DLC) in soft x-ray region

Boron is the critical trace element in the production of high quality steel, creating a great demand for an efficient detection method of the B-K emission band at around 6.76 nm. To meet this demand we made a simulation study and obtained a practical method to improve the diffraction efficiency of metal-coated laminar-type gratings for a grazing incidence flat-field spectrograph by overcoating a sufficiently transparent high-density material. In the simulation the diffraction efficiency in a spectral region of 3.5-8.5 nm was computed for several combinations of overcoating materials and coating metals, with various thicknesses of the overcoating layer. The result obtained are: (1) the best overcoating material is high-density diamond-like carbon (DLC) having a density of 3.1 g/cm{sup 3}, (2) its optimum thickness is 24 nm at an angle of incidence of 87.0°, and (3) with this thickness the first-order diffraction efficiency is expected to reach 29.7 %, which well exceeds 15.6 % for Ni-coated (or 14.1 % for Au-coated) grating.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗