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DOE OSTI2020

Computationally Guided Investigation of the Optical Spectra of Pure β-UO 3

Single-phase β-UO 3 is synthesized by flash heating UO 2 (NO 3 )·6H 2 O in air to 450 °C and annealing for 60 h under the same conditions. For the first time, we report the Raman spectra of pure β-UO 3 . To facilitate the assignment of Raman and infrared vibrational modes, we use density functional theory with density functional perturbation theory. By employing a novel analysis scheme that includes the mode frequencies as well as a quantitative analysis of the mode eigenvectors, we assign the observed spectral features to individual chemical modes. In particular, the density functional theory optimized structure, observed Raman spectrum, and eigenvector analysis suggest the presence of four crystallographically distinct uranyl ions, one more than has previously been suggested.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Radiative Heat Transfer and 2D Transition Metal Dichalcogenide Materials

Here we study the radiative heat transfer power in the family of transition metal dichalcogenide monolayers in their H- and T-symmetries. For this purpose, the electronic and optical properties computed from first-principles are used in effective models to understand the emerging scaling laws for metals and semiconductors as well as specific material signatures as control knobs for radiative heat transfer. Our combined approach of analytical modeling with properties from ab initio simulations can be used for other materials families to build a materials database for radiative heat transfer.

36 MATERIALS SCIENCE↗

DOE OSTI2022

The Magnetic Genome of Two-Dimensional van der Waals Materials

Magnetism in two-dimensional (2D) van der Waals (vdW) materials has recently emerged as one of the most promising areas in condensed matter research, with many exciting emerging properties and significant potential for applications ranging from topological magnonics to low-power spintronics, quantum computing, and optical communications. In the brief time after their discovery, 2D magnets have blossomed into a rich area for investigation, where fundamental concepts in magnetism are challenged by the behavior of spins that can develop at the single layer limit. However, much effort is still needed in multiple fronts before 2D magnets can be routinely used for practical implementations. In this comprehensive review, prominent authors with expertise in complementary fields of 2D magnetism (i.e., synthesis, device engineering, magneto-optics, imaging, transport, mechanics, spin excitations, and theory and simulations) have joined together to provide a genome of current knowledge and a guideline for future developments in 2D magnetic materials research.

36 MATERIALS SCIENCE↗

DOE OSTI2026

High-Purity Quantum Emission from an Au 24 (S-CH 2 Ph- t Bu) 20 Nanocluster at Room Temperature

Atomically precise gold nanoclusters have garnered significant attention for their diverse applications, ranging from biological labeling to optoelectronics. Their potential in optical quantum computing, which calls for ideal single-photon sources, has recently become a key area of interest. In the current work, we use photon antibunching experiments to explore the single-photon emission efficiency of atomically precise Au 24 nanoclusters protected by 4-tert-butylbenzyl mercaptan ligands (Au 24 (TBBM) 20 ). This cluster exhibits quantum emission with good photostability and without any observable blinking or spectral drift at room temperature under an inert gas atmosphere, with antibunching dips (g 2 (0)) as low as 0.07 in the solid state or, equivalently, a single-photon purity of 93% under time-gated conditions. Transient absorption and time-gated antibunching studies reveal that the short emission lifetime of this cluster and its high photoluminescence quantum yield in the solid state play critical roles in enhancing the emitted single-photon purity. This research advances the understanding of single-emitter behavior in atomically precise gold nanoclusters, contributing to the development of stable quantum emitters that are essential for quantum computing and cryptography.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Enantioselective Se lattices for stable chiroptoelectronic processing media

Chiroptoelectronic devices are crucial for applications in quantum computing, spin optical communications, and magnetic recording. However, the limited efficiency and low stability of conventional circularly polarized light (CPL)-sensing materials have restricted their broader use. Here, we introduce atomic chiral Se nanorod (NRs) films as broadband CPL detectors, leveraging the intrinsic chirality and stability of Se nanocrystals. We also perform incident circular polarization (ICP)-Raman optical activity (ROA) to explore the chiroptical activity of the large-area films. The Se NRs thin films detected CPL across a broad range from ultraviolet (UV) to short-wavelength infrared (SWIR), with a responsivity dissymmetry factor of up to 0.4, maintaining high stability under ambient conditions for longer than 13 months. CPL-sensitive Se NRs with intrinsic chirality have potential applications in chiral photonic synapses, chiral spin devices, and CPL-sensitive photocatalysts. ICP-ROA mapping also advances the analysis of 2D chiral materials.

Nanophotonics and plasmonics↗

DOE OSTI2026

Milliwatt-level UV generation using sidewall poled lithium niobate

Integrated coherent sources of ultra-violet (UV) light are essential for a wide range of applications, from ion-based quantum computing and optical clocks to gas sensing and microscopy. Recently, approaches that use frequency upconversion have received considerable attention. Among these, the integrated thin-film lithium niobate (TFLN) photonic platform shows particular promise. However, to date, the high propagation losses and lack of reliable techniques for consistent poling of cm-long waveguides with small poling periods have impeded progress. Here, we present a sidewall poled lithium niobate (SPLN) waveguide approach that overcomes these obstacles and results in a two-orders-of-magnitude increase in generated UV power. We demonstrate SPLN waveguides featuring record-low propagation losses of 2.3 dB/cm, complete domain inversion across the waveguide cross-section, and an optimum 50% duty cycle, resulting in a record-high normalized conversion efficiency of 5050%W$^{−1}$cm$^{−2}$, and 4.2 mW of generated on-chip power at 390 nm wavelength. This advancement makes the TFLN platform a viable option for high-quality on-chip UV generation, benefiting emerging applications.

Franken, C. A.A. [Harvard U.; Twente U., Enschede]↗

DOE OSTI2025

Inverse design of photonic surfaces via multi fidelity ensemble framework and femtosecond laser processing

We demonstrate a multi-fidelity (MF) machine learning ensemble framework for the inverse design of photonic surfaces, trained on a dataset of 11,759 samples that we fabricate using high throughput femtosecond laser processing. The MF ensemble combines an initial low fidelity model for generating design solutions, with a high fidelity model that refines these solutions through local optimization. The combined MF ensemble can generate multiple disparate sets of laser-processing parameters that can each produce the same target input spectral emissivity with high accuracy (root mean squared errors < 2%). SHapley Additive exPlanations analysis shows transparent model interpretability of the complex relationship between laser parameters and spectral emissivity. Finally, the MF ensemble is experimentally validated by fabricating and evaluating photonic surface designs that it generates for improved efficiency energy harvesting devices. Our approach provides a powerful tool for advancing the inverse design of photonic surfaces in energy harvesting applications.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2025

Intrinsic optical bistability of photon avalanching nanocrystals

Optically bistable materials respond to a single input with two possible optical outputs, contingent on excitation history. Such materials would be ideal for optical switching and memory, but the limited understanding of intrinsic optical bistability (IOB) prevents the development of nanoscale IOB materials suitable for devices. Here we demonstrate IOB in Nd 3+ -doped KPb 2 Cl 5 avalanching nanoparticles, which switch with high contrast between luminescent and non-luminescent states, with hysteresis characteristic of bistability. Here we elucidate a non-thermal mechanism in which IOB originates from suppressed non-radiative relaxation in Nd 3+ ions and from the positive feedback of photon avalanching, resulting in extreme, >200th-order optical nonlinearities. The modulation of laser pulsing tunes the hysteresis widths, and dual-laser excitation enables transistor-like optical switching. This control over nanoscale IOB establishes avalanching nanoparticles for photonic devices in which light is used to manipulate light.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Tunable coherent mixed-dimensional perovskite heterojunctions and quantum wells grown from solution

Coherent heterojunctions, quantum wells and multiple quantum wells are needed for high-performance devices; these are generally grown via a dedicated vapour phase epitaxy process. Here we demonstrate the growth of coherent perovskite heterojunctions and quantum wells made of mixed-dimensional perovskites using a solution process. By exploiting the solubility difference of methylammonium (MA + ) and 4-(aminomethyl)piperidinium (4AMP 2+ ), we assemble layered perovskites with different layer numbers. The resulting 4AMP-MA n–1 Pb n I 3n+1 materials each with different layer numbers or bandgaps form quantum wells. Heterojunctions and quantum wells made of 4AMP-MA 2 Pb 3 I 10 (n = 3) and 4AMP-MAPb 2 I 7 (n = 2) with various barrier thickness are tailored by the solution temperature profile during crystal growth. Multiple quantum wells have been formed by cycling temperature profiles. The planar heterojunction and quantum wells have lattice matching without interfacial defects, and exhibit strong thermal stability. Type I band alignment at the n = 2/n = 3 heterojunction is confirmed by both computation and optical studies. In conclusion, this study opens a new direction for the development of sophisticated perovskite heterojunction and quantum well devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

Deterministic fabrication of highly reproducible monochromatic quantum emitters in hexagonal boron nitride

Quantum emitters in hexagonal boron nitride are important room temperature single-photon sources. However, conventional fabrication methods yield quantum emitters with dispersed and inconsistent spectral profiles, limiting their potential for practical quantum applications, which demand reproducible high quality single-photon sources. Here, we report the deterministic creation of highly reproducible monochromatic quantum emitters by applying carbon-ion implantation on freestanding hexagonal boron nitride flakes, while a carbon mask with suitable thickness was adapted to optimize the implantation results. Quantum emitters fabricated using this approach exhibited thermally limited monochromaticity, with an emission center wavelength of 590.7 ± 2.7 nm, a narrow full width at half maximum of 7.1 ± 1.7 nm, an emission rate of 1 MHz without optical engineering, and exceptional stability under ambient conditions. Density functional theory calculations and scanning transmission electron microscopy suggest that these emitters are comprised of boron centered carbon tetramers. This method provides a reliable single-photon source for optical quantum computing and potential future industry-scale applications.

Hua, Muchuan [Argonne National Laboratory (ANL), A↗

DOE OSTI2016

Preliminary results concerning the simulation of beam profiles from extracted ion current distributions for mini-STRIKE

The Radio Frequency (RF) negative hydrogen ion source prototype has been chosen for the ITER neutral beam injectors due to its optimal performances and easier maintenance demonstrated at Max-Planck-Institut für Plasmaphysik, Garching in hydrogen and deuterium. One of the key information to better understand the operating behavior of the RF ion sources is the extracted negative ion current density distribution. This distribution—influenced by several factors like source geometry, particle drifts inside the source, cesium distribution, and layout of cesium ovens—is not straightforward to be evaluated. The main outcome of the present contribution is the development of a minimization method to estimate the extracted current distribution using the footprint of the beam recorded with mini-STRIKE (Short-Time Retractable Instrumented Kalorimeter). To accomplish this, a series of four computational models have been set up, where the output of a model is the input of the following one. These models compute the optics of the ion beam, evaluate the distribution of the heat deposited on the mini-STRIKE diagnostic calorimeter, and finally give an estimate of the temperature distribution on the back of mini-STRIKE. Several iterations with different extracted current profiles are necessary to give an estimate of the profile most compatible with the experimental data. A first test of the application of the method to the BAvarian Test Machine for Negative ions beam is given.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

RAY-UI: A powerful and extensible user interface for RAY

The RAY-UI project started as a proof-of-concept for an interactive and graphical user interface (UI) for the well-known ray tracing software RAY [1]. In the meantime, it has evolved into a powerful enhanced version of RAY that will serve as the platform for future development and improvement of associated tools. The software as of today supports nearly all sophisticated simulation features of RAY. Furthermore, it delivers very significant usability and work efficiency improvements. Beamline elements can be quickly added or removed in the interactive sequence view. Parameters of any selected element can be accessed directly and in arbitrary order. With a single click, parameter changes can be tested and new simulation results can be obtained. All analysis results can be explored interactively right after ray tracing by means of powerful integrated image viewing and graphing tools. Unlimited image planes can be positioned anywhere in the beamline, and bundles of image planes can be created for moving the plane along the beam to identify the focus position with live updates of the simulated results. In addition to showing the features and workflow of RAY-UI, we will give an overview of the underlying software architecture as well as examples for use and an outlook for future developments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

A 5 kA pulsed power supply for inductive and plasma loads in large volume plasma device

This paper describes 5 kA, 12 ms pulsed power supply for inductive load of Electron Energy Filter (EEF) in large volume plasma device. The power supply is based upon the principle of rapid sourcing of energy from the capacitor bank (2.8 F/200 V) by using a static switch, comprising of ten Insulated Gate Bipolar Transistors (IGBTs). A suitable mechanism is developed to ensure equal sharing of current and uniform power distribution during the operation of these IGBTs. Safe commutation of power to the EEF is ensured by the proper optimization of its components and by the introduction of over voltage protection (>6 kV) using an indigenously designed snubber circuit. Various time sequences relevant to different actions of power supply, viz., pulse width control and repetition rate, are realized through optically isolated computer controlled interface.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Forward modeling of Doppler velocity interferometer system for improved shockwave measurements

We report that when near-instantaneous shocks are recorded by using a Doppler velocity interferometer velocity interferometer system for any reflector (VISAR), they typically exceed the detector’s ability to react and “skipped fringes” result, where its visibility briefly reduces. Traditionally, replacing skipped fringes required guesswork in analysis, which increased arrival time errors. Second, the use of long but velocity-sensitive interferometer delays with fast detectors which can resolve the delay has traditionally been avoided because of the fear of confusing the arrival time signal. However, shorter delays produce smaller fringe phase shifts per velocity and, thus, can decrease velocity precision. We realize that while some loss of fringe information occurs at shock events, this is often just a partial loss and the residual fringe information can still hold valuable information. We describe a forward model (FM) of the interferometer action and detector blurring that assists with VISAR fringe analysis at skipping events: (1) more precise shock arrival times, (2) arrival time precision not limited by long delays, and (3) improved ghost subtraction, which improves accuracy over a broad time region. Lastly, we demonstrate the utility of a FM on National Ignition Facility and Laboratory for Laser Energetics Omega shots and discuss data process methods to increase the high time resolution of VISAR systems despite their limitations and complexities.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

An updated technique to obtain explosive kinetics data on microsecond timescales

There are few techniques available for chemists to obtain time-to-explosion data with known temperature inputs at the early stages of the design and synthesis of new explosives. In the 1960s, a technique was developed to rapidly heat milligram-quantities of confined explosives to ~1000 K on microsecond timescales. Wenograd loaded explosives inside stainless steel hypodermic needles, connected them to a fireset and rapidly discharged a capacitor through the steel. He obtained the temperature by measuring the needle resistance in a Wheatstone bridge arrangement and the time to explosion from a needle rupture. However, owing to the narrow-gauge needles used in the original research, the experiment was only possible with melt-castable explosives; it was never replicated, and modern diagnostics are now available with advances beyond the 1960s. Here, we report the development of the High Explosives Initiation Time (HEIT) test, which utilizes a 250 J pulsed power system to heat the needles. This work extends the Wenograd approach by using optical diagnostics, computational modeling, and advanced techniques to measure needle resistance and needle rupture. Preliminary rate information for pentaerythritol tetranitrate (PETN) will be presented.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2013

LINE PROFILES OF CORES WITHIN CLUSTERS. II. SIGNATURES OF DYNAMICAL COLLAPSE DURING HIGH-MASS STAR FORMATION

Observations of atomic or molecular lines can provide important information about the physical state of star-forming regions. In order to investigate the line profiles from dynamical collapsing massive star-forming regions (MSFRs), we model the emission from hydrodynamic simulations of a collapsing cloud in the absence of outflows. By performing radiative transfer calculations, we compute the optically thick HCO{sup +} and optically thin N{sub 2}H{sup +} line profiles from two collapsing regions at different epochs. Due to large-scale collapse, the MSFRs have large velocity gradients, reaching up to 20 km s{sup -1} pc{sup -1} across the central core. The optically thin lines typically contain multiple velocity components resulting from the superposition of numerous density peaks along the line of sight. The optically thick lines are only marginally shifted to the blue side of the optically thin line profiles, and frequently do not have a central depression in their profiles due to self-absorption. As the regions evolve, the lines become brighter and the optically thick lines become broader. The lower-order HCO{sup +} (1-0) transitions are better indicators of collapse than the higher-order (4-3) transitions. We also investigate how the beam sizes affect profile shapes. Smaller beams lead to brighter and narrower lines that are more skewed to the blue in HCO{sup +} relative to the true core velocity, but show multiple components in N{sub 2}H{sup +}. High-resolution observations (e.g., with Atacama Large Millimeter Array) can test these predictions and provide insights into the nature of MSFRs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2015

Binarity and the abundance discrepancy problem in planetary nebulae

The discrepancy between abundances computed using optical recombination lines and collisionally excited lines is a major unresolved problem in nebular astrophysics. Here, we show that the largest abundance discrepancies are reached in planetary nebulae with close binary central stars. We illustrate this using deep spectroscopy of three nebulae with a post common-envelope (CE) binary star. Abell 46 and Ou 5 have O{sup 2+}/H{sup +} abundance discrepancy factors larger than 50, and as high as 300 in the inner regions of Abell 46. Abell 63 has a smaller discrepancy factor around 10, which is still above the typical values in ionized nebulae. Our spectroscopic analysis supports previous conclusions that, in addition to “standard” hot (T{sub e} ∼ 10{sup 4} K) gas, there exists a colder (T{sub e} ∼ 10{sup 3} K), ionized component that is highly enriched in heavy elements. These nebulae have low ionized masses, between 10{sup −3} and 10{sup −1} M{sub ⊙} depending on the adopted electron densities and temperatures. Since the much more massive red giant envelope is expected to be entirely ejected in the CE phase, the currently observed nebulae would be produced much later, during post-CE mass loss episodes when the envelope has already dispersed. These observations add constraints to the abundance discrepancy problem. We revise possible explanations. Some explanations are naturally linked to binarity such as, for instance, high-metallicity nova ejecta, but it is difficult at this stage to depict an evolutionary scenario consistent with all of the observed properties. We also introduce the hypothesis that these nebulae are the result of tidal destruction, accretion, and ejection of Jupiter-like planets.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Plasma breakdown in bubbles passing between two pin electrodes

The ignition of plasmas in liquids has applications from medical instrumentation to manipulation of liquid chemistry. Formation of plasmas directly in a liquid often requires prohibitively large voltages to initiate breakdown. Producing plasma streamers in bubbles submerged in a liquid with higher permittivity can significantly lower the voltage needed to initiate a discharge by reducing the electric field required to produce breakdown. The proximity of the bubble to the electrodes and the shape of the bubbles play critical roles in the manner in which the plasma is produced in, and propagates through, the bubble. In this paper, we discuss results from a three-dimensional direct numerical simulation (DNS) used to investigate the shapes of bubbles formed by injection of air into water. Comparisons are made to results from a companion experiment. A two-dimensional plasma hydrodynamics model was then used to capture the plasma streamer propagation in the bubble using a static bubble geometry generated by the DNS The simulations showed two different modes for streamer formation depending on the bubble shape. In an elliptical bubble, a short electron avalanche triggered a surface ionization wave (SIWs) resulting in plasma propagating along the surface of the bubble. In a circular bubble, an electron avalanche first traveled through the middle of the bubble before two SIWs began to propagate from the point closest to the grounded electrode where a volumetric streamer intersected the surface. In an elliptical bubble approaching a powered electrode in a pin-to-pin configuration, we experimentally observed streamer behavior that qualitatively corresponds with computational results. Optical emission captured over the lifetime of the streamer curve along the path of deformed bubbles, suggesting propagation of the streamer along the liquid/gas boundary interface. Plasma generation supported by the local field enhancement of the deformed bubble surface boundaries is a mechanism that is likely responsible for initiating streamer formation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗