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At least 91 records · Page 5

Noncoplanar ferrimagnetism and local crystalline-electric-field anisotropy in the quasicrystal approximant Au 70 Si 17 Tb 13

Neutron scattering experiments have been performed to elucidate magnetic properties of the quasicrystal approximant Au 70 Si 17 Tb 13 , consisting of icosahedral spin clusters in a body-centered-cubic lattice. Bulk magnetic measurements performed on the single crystalline sample unambiguously confirm long-range ordering at T C = 11.6 ± 1 K. In contrast to the simple ferromagnetic response in the bulk measurements, single crystal neutron diffraction confirms a formation of intriguing non-collinear and non-coplanar magnetic order. The magnetic moment direction was found to be nearly tangential to the icosahedral cluster surface in the local mirror plane, which is quite similar to that recently found in the antiferromagnetic quasicrystal approximant Au 72 Al 14 Tb 14 . Inelastic neutron scattering on the powdered sample exhibits a very broad peak centered at hω ≃ 4 meV. The observed inelastic spectrum was explained by the crystalline-electric-field model taking account of the chemical disorder at the fractional Au/Si sites. The resulting averaged anisotropy axis for the crystalline-electric-field ground state is consistent with the ordered moment direction determined in the magnetic structure analysis, confirming that the non-coplanar magnetic order is stabilized by the local uniaxial anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Preliminary Design of a New Pulsed-Neutron Die--Away Experiments with Absorbers (IER-552 CED-1)

This report presents the preliminary design (CED-1) of IER-552, pulsed-neutron die-away (PNDA) experiments with absorbers, to be conducted by Lawrence Livermore National Laboratory (LLNL). The goal of the PNDA experiments with absorbing materials is to produce high-quality, low-cost integral benchmarks that can be used to validate cross sections that are high priority nuclear data for the Department of Energy’s Nuclear Criticality Safety Program (NCSP). PNDA experiments can be used to generate nuclear data validation benchmarks quickly and cheaply, as they do not require fissile material or a nuclear facility to conduct them. The original PNDA experiments were set up at LLNL under IER-501. Extending the PNDA experiments to include absorbing materials leverages existing facilities and resources at LLNL to validate cross sections, with a basic experiment design that uses a neutron generator to impinge a short, mono-energetic neutron pulse on a poisoned, moderating target sample. The neutron pulse lasts 100 µs, after which the neutron population in the sample reaches thermal equilibrium and later spatial equilibrium. In this fully equilibrized state, the neutron population has a characteristic decay-time eigenvalue. The eigenvalue can be used as an integral parameter to validate nuclear data involved with neutron scattering and absorption. Two observables can be measured: the neutron population and the population of secondary γ-rays produced by inelastic and capture reactions. This report explores the feasibility of both approaches. For γ-ray measurements, this allows for direct measurement of reactions of interest for validation. During the neutron burst time, inelastic (prompt) γ-rays dominate, and these data can be isolated for validation of neutron inelastic scattering data. After the pulse ends, neutron capture (delayed) γ-rays dominate and are produced by many reaction channels as neutrons slow down to thermal energies. Two sets of γ-ray spectra (inelastic, capture) can be produced for validation. Additionally, the time-dependent decay of the capture γ-ray population when the neutron population is thermalized and in its fundamental mode can be used for validation. Two experiments can be imagined where pulsed neutrons are used to validate the nuclear data of absorbing materials. The first integrates well into the existing PNDA testbed at LLNL. The absorber material would be introduced into a moderating target and the same neutron generator, neutron detectors, electronics, and shielding box used for IER-501 would be employed. From the same experimental setup, many absorbing materials can be validated by simply changing the neutron poison in the moderator. The only significant modification would be the introduction of a γ-ray detector. Such an experiment would primarily serve to validate nuclear data in the thermal energy range. The second kind of experiment would validate the fast and epithermal energy range. It would involve pulsing neutron into a bare assembly of the absorber material and measuring the die-away of neutrons. The fast leakage of such an assembly requires nanosecond neutron-generator pulse widths and fast detectors/electronics that could measure ~200 ns die-away curves. This kind of experiment would ideally be performed at a cyclotron, like that available at Lawrence Berkeley National Laboratory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Accessing metal-specific orbital interactions in C–H activation with resonant inelastic X-ray scattering

Photochemically prepared transition-metal complexes are known to be effective at cleaving the strong C–H bonds of organic molecules in room temperature solutions. There is also ample theoretical evidence that the two-way, metal to ligand (MLCT) and ligand to metal (LMCT), charge-transfer between an incoming alkane C–H group and the transition metal is the decisive interaction in the C–H activation reaction. What is missing, however, are experimental methods to directly probe these interactions in order to reveal what determines reactivity of intermediates and the rate of the reaction. Here, using quantum chemical simulations we predict and propose future time-resolved valence-to-core resonant inelastic X-ray scattering (VtC-RIXS) experiments at the transition metal L-edge as a method to provide a full account of the evolution of metal–alkane interactions during transition-metal mediated C–H activation reactions. For the model system cyclopentadienyl rhodium dicarbonyl (CpRh(CO) 2 ), we demonstrate, by simulating the VtC-RIXS signatures of key intermediates in the C–H activation pathway, how the Rh-centered valence-excited states accessible through VtC-RIXS directly reflect changes in donation and back-donation between the alkane C–H group and the transition metal as the reaction proceeds via those intermediates. We benchmark and validate our quantum chemical simulations against experimental steady-state measurements of CpRh(CO) 2 and Rh(acac)(CO)2 (where acac is acetylacetonate). Our study constitutes the first step towards establishing VtC-RIXS as a new experimental observable for probing reactivity of C–H activation reactions. More generally, the study further motivates the use of time-resolved VtC-RIXS to follow the valence electronic structure evolution along photochemical, photoinitiated and photocatalytic reactions with transition metal complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermal Neutron Scattering Improvements and Fixes for MCNP6.3 [Slides]

Major error (10,000+ pcm) discovered when using uranium-dioxide or uranium-nitride included in ENDF80SaB2 release. Improvements are being made towards preparing the code for ENDF/B-VIII.1 (ACE) format updates. A minor error (0-10’s pcm) was discovered while working on new capability development for Lab Directed Research & Development (LDRD) project. Previously, only a single coherent or incoherent elastic channel (along with an inelastic channel) was allowed in a thermal neutron scattering evaluation and subsequent processed ACE file. Based on what is planned in ENDF/B-VIII.1 release, there will be (a) new thermal scattering evaluation(s) which uses this mixed-mode coherent and incoherent elastic scattering blocks. MCNP6.3 has been modified to be able to handle such data in the future. Some reorganization has been made in the cross section calculation (acetot, sabcol, colidn) in the presence of TSL data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Gamma-ray imaging of inertial confinement fusion implosions reveals remaining ablator carbon distribution

The joint LANL/LLNL nuclear imaging team has acquired the first gamma-ray images of inertial confinement fusion implosions at the National Ignition Facility. The gamma-ray image provides crucial information to help characterize the inertially confined fuel and ablator assembly at stagnation, information that would be difficult to acquire from neutron or x-ray observations. Gamma imaging visualizes both gamma radiation emitted directly in deuterium–tritium (DT) fusion reactions as well as gamma rays produced when DT fusion neutrons scatter inelastically on carbon nuclei in the remaining ablator of the fuel capsule. The resulting image provides valuable information on the position and density of the remaining ablator and potential contamination of the hot spot—a powerful diagnostic window into the capsule assembly during burn.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-fidelity dimer excitations using quantum hardware

The quantum simulation of entangled spin systems can play a central role in quantum magnetic materials discovery. Additionally, the simulation of spectroscopic signatures, such as the dynamical structure factor accessed in inelastic neutron scattering (INS), necessitates a long timescale for circuit evolution. This is because the energy resolution is directly related to the time over which the circuit could be meaningfully evolved. However, canonical Trotterization requires deep circuits precluding such long-time evolution—even for a small number of qubits. Here, in this study, we demonstrate “direct” resource efficient fast-forwarding (REFF) measurements with short-depth circuits that can be used to capture longer time dynamics of spin Hamiltonians. We showcase the results of the dynamics of a quantum spin dimer, the basic quantum unit of emergent many-body spin systems, whose density of states we simulate accurately. The long temporal evolution and measurement of the two-spin correlation functions enable the calculation of the dynamical structure factor S⁡(Q = 0, ω) measured in the neutron scattering cross-section. We exhibit the clarity of the triplet gap and the triplet splitting of the quantum dimer with class-leading fidelity that enables comparison to experimental neutron data. Our results on current circuit hardware outline an important workflow to predict and benchmark against the outputs of INS experiments of quantum magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spectroscopic Evidence of Kondo-Induced Quasiquartet in CeRh 2 As 2

CeRh 2 As 2 is a new multiphase superconductor with strong suggestions for an additional itinerant multipolar ordered phase. The modeling of the low-temperature properties of this heavy-fermion compound requires a quartet Ce 3 + crystal-field ground state. Here, we provide the evidence for the formation of such a quartet state using x-ray spectroscopy. Core-level photoelectron and x-ray absorption spectroscopy confirm the presence of Kondo hybridization in CeRh 2 As 2 . The temperature dependence of the linear dichroism unambiguously reveals the impact of Kondo physics for coupling the Kramer’s doublets into an effective quasiquartet. Nonresonant inelastic x-ray scattering data find that the | Γ 7 − ⟩ state with its lobes along the 110 direction of the tetragonal structure ( x y orientation) contributes most to the multiorbital ground state of CeRh 2 As 2 . Published by the American Physical Society 2024

Christovam, Denise S. (ORCID:0000000250698107)↗

Measurements of low-mode asymmetries in the areal density of laser-direct-drive deuterium–tritium cryogenic implosions on OMEGA using neutron spectroscopy

Areal density is one of the key parameters that determines the confinement time in inertial confinement fusion experiments, and low-mode asymmetries in the compressed fuel are detrimental to the implosion performance. The energy spectra from the scattering of the primary deuterium–tritium (DT) neutrons off the compressed cold fuel assembly are used to investigate low-mode nonuniformities in direct-drive cryogenic DT implosions at the Omega Laser Facility. For spherically symmetric implosions, the shape of the energy spectrum is primarily determined by the elastic and inelastic scattering cross sections for both neutron-deuterium and neutron-tritium kinematic interactions. Two highly collimated lines of sight, which are positioned at nearly orthogonal locations around the OMEGA target chamber, record the neutron time-of-flight signal in the current mode. An evolutionary algorithm is being used to extract a model-independent energy spectrum of the scattered neutrons from the experimental neutron time-of-flight data and is used to infer the modal spatial variations (l = 1) in the areal density. Experimental observations of the low-mode variations of the cold-fuel assembly (ρL 0 + ρL 1 ) show good agreement with a recently developed model, indicating a departure from the spherical symmetry of the compressed DT fuel assembly. As a result, another key signature that has been observed in the presence of a low-mode variation is the broadening of the kinematic end-point due to the anisotropy of the dense fuel conditions.

47 OTHER INSTRUMENTATION↗

Observation of van der Waals phonons in the single-layer cuprate ( Bi , Pb ) 2 ( Sr , La ) 2 CuO 6 + δ

Interlayer van der Waals (vdW) coupling is generic in two-dimensional materials such as graphene and transition-metal dichalcogenides, which can induce very low-energy phonon modes. Using high-resolution inelastic hard x-ray scattering, we uncover the ultralow energy phonon mode along the Cu-O bond direction in the high- T c cuprate (Bi,Pb) 2 (Sr,La) 2 ⁢CuO 6+$\delta$ (Bi2201). The energy and full-width half-maximum (FWHM) of these modes are independent of temperature, while their intensity decreases with doping in accordance with an increasing c -axis lattice parameter. Here, we compare the experimental results to first-principles density functional theory simulations and identify the observed mode as a van der Waals phonon, which arises from the shear motion of the adjacent Bi-O layers. This shows that Bi-based cuprate has vibrational properties similar to graphene and transition-metal dichalcogenides, which can be exploited to engineer novel heterostructures.

36 MATERIALS SCIENCE↗

Benchmarking universal machine learning interatomic potentials for rapid analysis of inelastic neutron scattering data

The accurate calculation of phonons and vibrational spectra remains a significant challenge, requiring highly precise evaluations of interatomic forces. Traditional methods based on the quantum description of the electronic structure, while widely used, are computationally expensive and demand substantial expertise. Emerging universal machine learning interatomic potentials (uMLIPs) offer a transformative alternative by employing pre-trained neural network surrogates to predict interatomic forces directly from atomic coordinates. This approach dramatically reduces computation time and minimizes the need for technical knowledge. In this paper, we produce a phonon database comprising nearly 5000 inorganic crystals to benchmark the performance of several leading uMLIPs. We further assess these models in real-world applications by using them to analyze experimental inelastic neutron scattering data collected on a variety of materials. Through detailed comparisons, we identify the strengths and limitations of these uMLIPs, providing insights into their accuracy and suitability for fast calculations of phonons and related properties, as well as the potential for real-time interpretation of neutron scattering spectra. Our findings highlight how the rapid advancement of AI in science is revolutionizing experimental research and data analysis.

inelastic neutron scattering↗

Metastable nuclear isomers as dark matter accelerators

Inelastic dark matter and strongly interacting dark matter are poorly constrained by direct detection experiments since they both require the scattering event to deliver energy from the nucleus into the dark matter in order to have observable effects. We propose to test these scenarios by searching for the collisional deexcitation of metastable nuclear isomers by the dark matter particles. The longevity of these isomers is related to a strong suppression of γ- and β-transitions, typically inhibited by a large difference in the angular momentum for the nuclear transition. The collisional deexcitation by dark matter is possible since heavy dark matter particles can have a momentum exchange with the nucleus comparable to the inverse nuclear size, hence lifting tremendous angular momentum suppression of the nuclear transition. This deexcitation can be observed either by searching for the direct effects of the decaying isomer, or through the rescattering or decay of excited dark matter states in a nearby conventional dark matter detector setup. Existing nuclear isomer sources such as naturally occurring 180m Ta, 137m Ba produced in decaying Cesium in nuclear waste, 177m Lu from medical waste, and 178m Hf from the Department of Energy storage can be combined with current dark matter detector technology to search for this class of dark matter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Phase and Morphology of Water-ice Grains Formed in a Cryogenic Laboratory Plasma

Abstract Grains of ice are formed spontaneously when water vapor is injected into a weakly ionized laboratory plasma in which the background gas has been cooled to cryogenic temperatures comparable to those of deep space. These ice grains are levitated indefinitely within the plasma so that their time evolution can be observed under free-floating conditions. Using microscope imaging, ice grains are shown to have a spindle-like fractal structure and grow over time. Both crystalline and amorphous phases of ice are observed using Fourier transform infrared spectroscopy. A mix of crystalline and amorphous grains coexists under certain thermal conditions, and a linear mixing model is used on the ice absorption band surrounding 3.2 μ m to examine the ice phase composition and its temporal stability. The extinction spectrum is also affected by inelastic scattering as grains grow, and characteristic grain radii are obtained from Mie scattering theory and compared to size measurements from direct imaging. Observations are used to compare possible ice nucleation mechanisms, and it is concluded that nucleation is likely catalyzed by ions, as ice does not nucleate in the absence of plasma and impurities are not detected. Ice grain properties and infrared extinction spectra show similarity to observations of some astrophysical ices observed in protoplanetary disks, implying that the fractal morphology of the ice and observed processes of homogeneous ice nucleation could occur as well in such astrophysical environments with weakly ionized conditions.

Astronomy & Astrophysics↗

Resonant inelastic X-ray scattering tools to count 5 $f$ electrons of actinides and probe bond covalency

The actinides possess a complex electronic structure, making their chemical and physical properties among the least understood in the periodic table. Advanced spectroscopic tools, able to obtain deep insights into the electronic structure and binding properties of the actinides, are highly desirable. Here, we introduce two sensitive spectroscopic tools: one determines the number of localized 5f electrons on an actinide atom, and another assesses the covalent character of actinide-ligand bonding. Both tools are based on the multiplet structure present in actinide M 4 edge core-to-core resonant inelastic X-ray scattering (CC-RIXS) maps. The spectral intensity of different many-body final-state multiplets directly depends on the local many-electron ground-state symmetry including the local 5 f spin configuration. By comparing U M 4 edge CC-RIXS data for 21 U, Np, Pu and Am compounds, we demonstrate the ability to compare the number of localized 5 f electrons and bond covalency across the actinide series.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Neutron Next-Event Estimators Kinematics (Rev.2)

This paper reviews the kinematics of neutron elastic and inelastic scattering with moving and stationary targets for contributions to Neutron Next-Event Estimators (NEEs). NEEs are often used for simulating the response of detectors in locations that have few random walk particles. Contributions to NEEs from collisions differ from sampling the outgoing particle state in standard random walk collisions as the location of the estimator is fixed, thus fixing the scattering angle between the incoming and outgoing directions. To calculate contributions to NEEs, the outgoing energies and probabilities of scatter toward the estimator must be calculated. This paper presents the most general case that encompasses elastic and inelastic scattering with both moving and stationary targets. The moving target case is required for elastic scattering with thermal motion due to the free gas thermal treatment approximation. The stationary target equations are presented for comparison with equations presented in canonical Monte Carlo texts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Coherent detection of hidden spin–lattice coupling in a van der Waals antiferromagnet

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin–lattice coupling in a vdW antiferromagnet FePS 3 that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS 3 selectively couples to the trigonal distortions through partially filled t 2 g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin–lattice coupling in FePS 3 but also establish phase-resolved CPS as a tool to investigate hidden interactions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Neutron scattering and neural-network quantum molecular dynamics investigation of the vibrations of ammonia along the solid-to-liquid transition

Abstract Vibrational spectroscopy allows us to understand complex physical and chemical interactions of molecular crystals and liquids such as ammonia, which has recently emerged as a strong hydrogen fuel candidate to support a sustainable society. We report inelastic neutron scattering measurement of vibrational properties of ammonia along the solid-to-liquid phase transition with high enough resolution for direct comparisons to ab-initio simulations. Theoretical analysis reveals the essential role of nuclear quantum effects (NQEs) for correctly describing the intermolecular spectrum as well as high energy intramolecular N-H stretching modes. This is achieved by training neural network models using ab-initio path-integral molecular dynamics (PIMD) simulations, thereby encompassing large spatiotemporal trajectories required to resolve low energy dynamics while retaining NQEs. Our results not only establish the role of NQEs in ammonia but also provide general computational frameworks to study complex molecular systems with NQEs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Neutron reconstruction via blips in liquid argon time projection chambers

Neutrons are important final-state particles in neutrino interactions, yet they are not considered or reconstructed in most current neutrino liquid argon time projection chamber (LArTPC) physics analyses. In this paper, we present a simulation-based proof-of-concept study of neutron reconstruction in a generic LArTPC detector. Leveraging isolated, MeV-scale energy deposits, or blips, from neutron inelastic scattering, and using realistic blip response from published experimental results, we demonstrate the capability to identify neutrons and to reconstruct the direction and energy of the final-state neutron system in sub-GeV neutrino interactions. We then explore how neutron-related blip attributes can be used to improve physics studies of neutrino interactions, such as enhancing neutrino-antineutrino separation in atmospheric neutrinos and reverse-horn-current beam neutrinos. This study provides an initial quantification of LArTPC neutron reconstruction capabilities, which we expect to improve with future advancements in blip reconstruction, identification, and classification algorithms, as well as the modeling of neutrons.

Morquecho, Miguel Hernandez [Univ. of Minnesota, M↗

Low-energy quasi-circular electron correlations with charge order wavelength in Bi 2 Sr 2 CaCu 2 O 8+δ

Most resonant inelastic x-ray scattering (RIXS) studies of dynamic charge order correlations in the cuprates have focused on the high-symmetry directions of the copper oxide plane. However, scattering along other in-plane directions should not be ignored as it may help understand, for example, the origin of charge order correlations or the isotropic scattering resulting in strange metal behavior. Our RIXS experiments reveal dynamic charge correlations over the qx-qy scattering plane in underdoped Bi 2 Sr 2 CaCu 2 O 8+δ . Tracking the softening of the RIXS-measured bond-stretching phonon, we show that these dynamic correlations exist at energies below approximately 70 meV and are centered around a quasi-circular manifold in the q x -q y scattering plane with radius equal to the magnitude of the charge order wave vector, q CO . This phonon-tracking procedure also allows us to rule out fluctuations of short-range directional charge order (i.e., centered around [q x = ±q CO , q y = 0] and [q x = 0, q y = ±q CO ]) as the origin of the observed correlations.

36 MATERIALS SCIENCE↗