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DOE OSTI2022

Advances in actinide thin films: synthesis, properties, and future directions

Actinide-based compounds exhibit unique physics due to the presence of 5f electrons, and serve in many cases as important technological materials. Targeted thin film synthesis of actinide materials has been successful in generating high-purity specimens in which to study individual physical phenomena. These films have enabled the study of the unique electron configuration, strong mass renormalization, and nuclear decay in actinide metals and compounds. The growth of these films, as well as their thermophysical, magnetic, and topological properties, have been studied in a range of chemistries, albeit far fewer than most classes of thin film systems. This relative scarcity is the result of limited source material availability and safety constraints associated with the handling of radioactive materials. Here, we review recent work on the synthesis and characterization of actinide-based thin films in detail, describing both synthesis methods and modeling techniques for these materials. Further, we review reports on pyrometallurgical, solution-based, and vapor deposition methods. We highlight the current state-of-the-art in order to construct a path forward to higher quality actinide thin films and heterostructure devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Role of sheared E × B flow in self-organized, improved confinement states in magnetized plasmas

A great scientific success story of magnetic fusion research in the past several decades is the theoretical development and experimental testing of the process of turbulence decorrelation and stabilization by sheared E×B flow which shows that E×B shear effects are ubiquitous in magnetized plasmas. This concept of turbulence decorrelation and stabilization has the universality needed to explain the H-mode edge transport barriers seen in limiter and divertor tokamaks, stellarators, and mirror machines; the broader edge transport barrier seen in VHmode plasmas; and the core transport barriers formed in tokamaks. Similar effects are seen in linear devices. These examples of confinement improvement are of considerable physical interest; it is not often that a system self-organizes to reduce transport when an additional source of free energy is applied to it. The transport decrease associated with E×B velocity shear is also of great practical benefit to fusion research, since it contributed to substantially increased fusion yield in all DT magnetic fusion experiments conducted to date. The fundamental physics involved in transport reduction is the effect of E×B shear on the growth, radial extent, and phase correlation of turbulent eddies in the plasma. The same basic transport reduction process can be operational in various portions of the plasma because there are a number of ways to change the radial electric field Er. An important secondary theme in this area is the synergistic effect of E×B velocity shear and magnetic shear. Although the E×B velocity shear appears to have an effect on broader classes of microturbulence, magnetic shear can mitigate some potentially harmful effects of E×B velocity shear and facilitate turbulence stabilization. Our present understanding in this area is the result of a multi-decade, intertwined effort in theory, modeling and diagnostic development combined with continuing experimental investigations. These experiments have clearly demonstrated that increased E×B shear causes reductions in turbulence and transport. Finally, the experimental findings are generally consistent with the basic theoretical models although considerable work remains to be done before we have a fully predictive theory of transport in magnetized plasmas including E×B shear effects.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Ultrafast local demagnetization in 𝑑 6 systems via driven Jahn-Teller distortions

Ultrafast control of spin orientations without relying on highly nonequilibrium electron distributions offers a new pathway for femtosecond spintronics. It is shown that excitation of specific vibronic modes can drive a substantial demagnetization of a local moment relative to the magnetization axis, while preserving its total spin quantum number. Using a fully quantum many-body treatment of a local 𝑆=2 (𝑑 6 ) many-body spin coupled to a driven Jahn-Teller mode with quantum dissipation, we find that the projected spin can be strongly reduced via a Jahn-Teller-induced 𝑥⁢𝑦↑→𝑦⁢𝑧/𝑧⁢𝑥↓ transition, which occurs without additional Coulomb exchange cost. The excited state subsequently relaxes back to its original electronic configuration with a rotated spin direction, enabling spin reorientation without generating a large net angular momentum in the electronic subsystem.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Oxygen Deficiency and Migration-Mediated Electric Polarization in Magnetic Fe,Co-Substituted SrTiO3−δ

We use density functional theory (DFT) calculations to show that oxygen vacancies (vO) and mobility induce noncentrosymmetric polar structures in SrTi1−x−yFexCoyO3−δ (STFC, x=y=0.125) with δ={0.125,0.25}, enhance the saturation magnetization, and give rise to large changes in the electric polarization |ΔP|. We present an intuitive set of rules to describe the properties of STFC, which are based on the interplay between (Co/Fe)-vO defects, magnetic cation coordination, and topological vacancy disorder. STFC structures consist of layered crystals with sheets of linearly organized O4,5,6-coordinated Fe–Co pairs, sandwiched with layers of O5-coordinated Ti. (Co/Fe)-vO defects are the source of crystal distortions, cation off-centering and bending of the oxygen octahedra which, considering the charge redistribution mediated by vO and the cations’ electronegativity and valence states, triggers an effective electric polarization. Oxygen migration for δ=0.125 leads to |ΔP|>∼10 µC/cm2 due to quantum-of-polarization differences between δ=0.125 structures. Increasing the oxygen deficiency to δ=0.25 yields |ΔP|, the O migration of which resolved polarization for δ=0.25 is >∼3 µC/cm2. Magnetism is dominated by the Fe,Co spin states for δ=0.125, and there is a contribution from Ti magnetic moments (∼1 μB) for δ=0.25. Magnetic and electric order parameters change for variations of δ or oxygen migration for a given oxygen deficiency. Our results capture characteristics observed in the end members of the series SrTi(Co,Fe)O3, and suggest the existence of a broader set of rules for oxygen-deficient multiferroic oxides.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Brightening of Dark States in CsPbBr 3 Quantum Dots Caused by Light–Induced Magnetism

Lead halide perovskite quantum dots (QDs) have shown great potential for optoelectronic and quantum photonic applications. Although controversy remains about the electronic fine structures of bulk perovskites due to the strong spin-orbit coupling affecting the conduction bands, compelling evidence indicates that the ground states of perovskite QDs remain dark, limiting their applications in optoelectronic devices. In this study, it is demonstrated that photoexcitation can induce large intrinsic magnetic fields in Mn-doped CsPbBr 3 perovskite QDs. Equivalent to applying an external magnetic field, the light-induced field causes giant Zeeman splitting to the bright triplet states and brightens the dark singlet ground state, thus effectively rendering a partially bright ground state in the doped QDs. These findings here may contribute to the understanding of the electronic fine structures in perovskite QDs and demonstrate a potential approach for creating semiconductor nanostructures that can serve as bright light sources.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Development of a portable high-T c spherical neutron polarimetry device at the Oak Ridge National Laboratory

Spherical neutron polarimetry is a powerful polarized neutron scattering technique used to determine complex magnetic structures which are only partly accessible by other methods. This technique measures the full neutron polarization change upon scattering from a sample by fully decoupling the incoming and outgoing neutron polarization with a zero-field chamber placed at the sample position. Recent advancements and testing are presented for a new spherical neutron polarimetry device utilizing high-T c superconducting YBCO films, PHiTPAD, at the High Flux Isotope Reactor at Oak Ridge National Laboratory. Furthermore, we introduce a conceptual design that utilizes wavelength-independent adiabatic transitions to adapt spherical neutron polarimetry for use with pulsed neutron sources, thereby expanding its potential applications in neutron scattering research.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Anomalies in the electromagnetic response and peculiarities of the domain structure in the magnetic Weyl semimetal Co 3⁢ Sn 2 ⁢S 2

In this paper, we present a comprehensive study of magnetic properties of Co 3 ⁢Sn 2 ⁢S 2 (CoSnS) crystals using macroscopic characterization and observations of the domain structure (DS) in a wide range of easy- and hard-axis fields (𝐻) and temperatures (𝑇). From macroscopic measurements, we derive temperature dependences of the basic magnetic parameters of the material [saturation magnetization 𝑀 𝑠 ⁡(𝑇), uniaxial anisotropy constant 𝐾⁡(𝑇), and exchange stiffness 𝐴⁡(𝑇)] and, based on them, calculate the thermodynamic magnetization 𝑀⁡(𝐻,𝑇) curves and DS parameters for pinning-free samples. We find important qualitative and quantitative differences between the theory and experiment defined by the efficient pinning of domain walls (DWs) in our samples. It turns out that, already at temperatures close to the ferromagnetic transition 𝑇 𝑐 , the DW dynamics falls into the heavy creep regime, resulting in a strong deferral of the DS adjustment into the equilibrium state. Here, we suggest that specific magnetic defects, responsible for pinning and causing field-tuned reproducible domain nucleation patterns observed in our high-quality samples, are pointlike. Recently found magnetic polarons formed around vacancies and impurities, which carry strong diamagnetic moments of spin-orbit nature and are intrinsic for CoSnS and expected in other Weyl semimetals, are a possible source of pinning yielding peculiar 𝑀⁡(𝐻,𝑇) response of CoSnS.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Solid-State Nuclear Magnetic Resonance as a Tool to Probe the Impact of Mechanical Preprocessing on the Structure and Arrangement of Plant Cell Wall Polymers

Efficient separation of the plant cell wall polymers during lignocellulose processing has been historically challenging due to insolubility of the polymers and their propensity for recalcitrant reassembly. Methods, such as “lignin first” extraction techniques, have advanced efficient biomass use, but the molecular mechanisms for recalcitrance remain enigmatic. Here, we discuss how solid-state Nuclear Magnetic Resonance (NMR) approaches report on the 3D organization of cellulose, xylan, and lignin in the plant cell wall. Recent results illustrate that the organization of these polymers varies across biomass sources and sample preparation methods, with even minimal physical processing causing significant effects. These structural differences contribute to variable extraction efficiencies for bioproducts after downstream processing. We propose that solid-state NMR methods can be applied to follow biomass processing, providing an understanding of the polymer rearrangements that can lead to poor yields for the desired bioproducts. The utility of the technique is illustrated for mechanical processing using lab-scale vibratory ball milling of Sorghum bicolor .

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Quantum Accurate Prediction of Plutonium–Plutonium Dihydride Phase Equilibrium Using a Lattice Gas Model

Plutonium-based materials are vital for use as nuclear fuels and as portable power sources for space vehicles. However, elucidating their sensitivity to hydriding corrosion represents an extreme challenge because of the toxicity of Pu as well as their anomalous magnetic properties. In this work, we develop a lattice gas model of plutonium–plutonium dihydride (Pu–PuH 2 ) phase equilibrium that retains the accuracy of density functional theory, while yielding many orders of magnitude improvement in computational efficiency. Using Monte Carlo and free-energy sampling algorithms, we compute a number of Pu–PuH 2 equilibrium properties that are difficult to probe experimentally, including equilibrium pressures and phase compositions and the PuH 2 heat of formation. In conclusion, our method will have particular impact on these types of materials studies, where there is a strong need for computationally efficient approaches to bridge time and length scale gaps between quantum calculations and experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Optical activation and detection of charge transport between individual colour centres in diamond

Understanding the capture of charge carriers by colour centres in semiconductors is important for the development of novel forms of sensing and quantum information processing, but experiments typically involve ensemble measurements, often impacted by defect proximity. In this study, we show that confocal fluorescence microscopy and magnetic resonance can be used to induce and probe charge transport between individual nitrogen-vacancy centres in diamond at room temperature. In our experiments, a ‘source’ nitrogen vacancy undergoes optically driven cycles of ionization and recombination to produce a stream of photogenerated carriers, one of which is subsequently captured by a ‘target’ nitrogen vacancy several micrometres away. We use a spin-to-charge conversion scheme to encode the spin state of the source colour centre into the charge state of the target, which allows us to set an upper bound to carrier injection from other background defects. We attribute our observations to the action of unscreened Coulomb potentials producing giant carrier capture cross-sections, orders of magnitude greater than those measured in ensembles.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Optimizing detachment control using the magnetic configuration of divertors

Abstract As tokamak research moves to reactor conditions, the control of a stable, optimally-detached divertor plasma has become increasingly relevant. Simple predictions of such detachment control have been performed previously using the detachment location sensitivity (DLS) model (Lipschultz et al 2016 Nucl. Fusion 56 056007). In this study the DLS model is extended and combined with SOLPS-ITER simulations of isolated divertor grids to study the effects of alternate divertor magnetic field properties on detachment control. The DLS model predicts that divertors can achieve easier access to detachment through a long connection length, a high total flux expansion, and a high average magnetic field in the divertor compared with that at the x -point. SOLPS-ITER simulations suggest an even stronger impact of total flux expansion and connection length on detachment access than the DLS model predicts. In terms of detachment evolution, both simulation and modelling show a high gradient in the total magnetic field and low B p o l B are able to more easily keep a detachment front at a desired poloidal location. Regions with no stable detachment front locations can arise for high magnetic field gradients directed towards the target. Significant differences have been found between impurity scan simulations and the DLS model. These differences may be attributed to sources and sinks of power and electron pressure, and should be explored further in future work.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Beam loss mechanisms in the PIP-II linac and beam transfer line at Fermilab

Beam loss in high-intensity H- linacs, such as the PIP-II linac at Fermilab, is a critical challenge that requires comprehensive study and understanding to ensure efficient and safe operation. This study explores the various beam loss mechanisms encountered in the PIP-II linac and its beam transfer line, drawing parallels from other high-intensity H- linacs. Key loss mechanisms include residual gas stripping, where H- ions interact with residual gas molecules leading to electron detachment; field stripping, caused by the interaction of H- ions with magnetic fields; and intra-beam stripping, resulting from interactions within the beam itself. Beam halo formation, particularly due to Twiss function mismatch, is another significant source of beam loss, which can be exacerbated by Landau damping mechanisms. Adhering to the 1 W/m loss criterion is essential to maintain hands-on maintenance capability and ensure the longevity of the accelerator components. By understanding these mechanisms and implementing targeted mitigation strategies, the PIP-II linac can achieve its design goals while maintaining safe and efficient operations.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Transfer Line at Fermilab

Pathak, Abhishek↗

DOE OSTI2025

Constraints on light QCD and CP-violating axions from the death line of rotation-powered pulsars

For axions that couple to nucleons, the presence of dense nuclear matter can displace the axion from its vacuum minimum, sourcing large field gradients around neutron stars (and, more generally, compact objects). These gradients, which we refer to as axion hair, couple to the local background magnetic field, inducing a large voltage drop near the surface of the star; here, we demonstrate that the presence of axion hair decouples local near-field particle acceleration in the open magnetic field line bundle from the rotational frequency of the pulsar itself. This is significant as the non-observation of old slowly-rotating pulsars is attributed to the fact the rotationally-induced electric fields are not strong enough to sustain $e^\pm$ pair production. In this work, we review the evidence for the existence for `pulsar death', i.e. the threshold at which $e^\pm$ pair production (and thus, by association, coherent radio emission) ceases, and demonstrate using both semi-analytics and particle-in-cell simulations that the existence of axion hair can dramatically extend pulsar lifetimes. We show that the non-observation of extremely old, slowly rotating, pulsars allows for a new probe of light QCD and CP-violating axions. We also demonstrate how the observation of emission from both poles of pulsars with nearly orthogonal rotational and magnetic axes, as seen e.g. in PSR J1906+0746, can be used to set competitive limits on CP-violating axion-nucleon interactions.

Witte, Samuel J. [Oxford U., Theor. Phys.; DESY; H↗

DOE OSTI2023

From ash to oxides: Recovery of rare-earth elements as a step towards valorization of coal fly ash waste

Coal fly ash (CFA) is both a valuable waste material and a potential source of environmental contamination. The inclusion of metals such as rare-earth elements offer a possible incentive towards waste valorization if the metals can be extracted and recovered in an economical manner. Rare-earth elements (REEs) have many technological applications and are critically important in the manufacture of electric vehicles, communication devices, and industrial magnets. However, the global supply of rare-earth elements has faced shortages and price shocks. Current methods for separating and isolating individual rare-earth elements use large amounts of energy and organic solvents, raising concerns over environmental impacts. These factors have led to the investigation of nontraditional sources and separation techniques for these elements. Here, we describe a column-based system that uses a newly developed ligand-associated organosilica sorbent to concentrate and separate rare-earth elements from fly ash leachate. The fly ash used in this study originally contained 0.024 wt% rare-earth elements and the final oxide powder after enrichment contained > 10 wt% rare-earth elements, which is a enrichment of > 400 times. This process requires no additional organic solvents after the sorbent media has been synthesized, offering an alternative to the current standard using solvent extraction for rare-earth element recovery.

42 ENGINEERING↗

DOE OSTI2025

Electromagnetic moments of 215,217 Bi: Probing shell evolution beyond N = 126

The nuclear properties of bismuth isotopes (Z = 83) , with just one valence proton above the closed spherical shell at (Z = 82) , are expected to be governed by a single unpaired proton. However, already in semimagic 209 Bi (Z = 83, N = 126) , , the magnetic moment (μ) strongly deviates from the single-particle Schmidt value. A near linear decrease in μ with the increase of N after the N = 126 magic number was observed up to N = 130 . In order to test whether this trend is kept at N > 130 and to reveal the underlying mechanisms, an investigation of 215,217 Bi (N = 132, 134) has been undertaken. The magnetic dipole and electric quadrupole moments of the I π = 9/2 - nuclear ground states in these isotopes have been measured for the first time using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). It has been shown that the linearly decreasing trend of μ( 209,211,213 Bi g ) is broken in 215,217 Bi with a nearly constant value of μ observed. Experimental data have been compared to calculations in the framework of the configuration-interaction shell model with the monopole-based universal V MU +LS interaction. The peculiarities in the behavior of μ(Bi, 9/2 - ) with increasing neutron number are explained as being due to the shell evolution, change of the neutron orbitals occupancies and strong configuration mixing beyond N = 130 . Also, the difference in the μ trends for bismuth (Z = 83) and astatine (Z = 85) isotopes with N > 126 are reproduced by the shell-model calculations. It is shown that monopole interaction plays noticeable role in the description of the peculiarities of the μ behaviour. Additionally, the extension of the application of the V MU interaction to the μ isotopic trends for heavy nuclei is important for further study of the capabilities of this promising version of the shell-model calculations.

Dipole magnetic moments↗

DOE OSTI2022

A sustained high-temperature fusion plasma regime facilitated by fast ions

Nuclear fusion is one of the most attractive alternatives to carbon-dependent energy sources. Harnessing energy from nuclear fusion in a large reactor scale, however, still presents many scientific challenges despite the many years of research and steady advances in magnetic confinement approaches. State-of-the-art magnetic fusion devices cannot yet achieve a sustainable fusion performance, which requires a high temperature above 100 million kelvin and sufficient control of instabilities to ensure steady-state operation on the order of tens of seconds. Here, in this study, we report experiments at the Korea Superconducting Tokamak Advanced Research device producing a plasma fusion regime that satisfies most of the above requirements: thanks to abundant fast ions stabilizing the core plasma turbulence, we generate plasmas at a temperature of 100 million kelvin lasting up to 20 seconds without plasma edge instabilities or impurity accumulation. A low plasma density combined with a moderate input power for operation is key to establishing this regime by preserving a high fraction of fast ions. This regime is rarely subject to disruption and can be sustained reliably even without a sophisticated control, and thus represents a promising path towards commercial fusion reactors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Effect of magnetic field inclination on black hole jet power and particle acceleration

Rotating black holes are known to launch relativistic jets and accelerate particles if they accrete a magnetized plasma. It remains unclear, however, how the global magnetic field orientation affects the jet powering efficiency. We propose the first kinetic study of a collisionless plasma around a Kerr black hole embedded in a magnetic field that is inclined with respect to the black hole spin axis. Using three-dimensional general relativistic particle-in-cell simulations, we show that while oblique magnetic field configurations significantly reduce the jet power, particle acceleration still remains highly efficient. This suggests that black holes producing a weak jet might still be bright sources of nonthermal radiation and cosmic rays.

acceleration of particles↗