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At least 217 records · Page 12

Spatiotemporal mapping of mesoscopic liquid dynamics

The study of liquid dynamics at mesoscopic scales is still strewn with difficulty due to limitations in theory and experiment. Historically, significant attention has been given to the analysis of space-time correlation functions and their frequency-Fourier transforms at a few discrete wave numbers. The massive computing power afforded by modern high performance computing clusters and the advent of a wide-angle neutron spin-echo spectrometer, however, have unlocked a more intuitive and fruitful approach to this problem. Using molecular dynamics simulations, here we demonstrate the benefits of spatiotemporally mapping intermediate scattering functions on a dense grid of correlation times and wave numbers. Four model systems are investigated: a Lennard-Jones liquid, a coarse-grained bead-spring polymer, a molten sodium chloride, and a poly(ethylene oxide) melt. We show that the spatiotemporal mapping approach is particularly useful for elucidating the mesoscopic dynamics in these liquids, where several underlying mechanisms, such as molecular relaxations, hydrodynamic modes, and nonhydrodynamic excitations, are potentially at play. Therefore, compared to the traditional method, direct visualization of density space-time correlation functions on two-dimensional color maps permits appraisals of complicated dynamical behavior at mesoscales in a global manner. For example, the scaling relations between space and time for different types of molecular motions can be straightforwardly identified on these plots, without any model-dependent analysis. Additionally, we show how theoretical ideas regarding collective mesoscopic dynamics, such as the classical hydrodynamic theory, the convolution approximation, and a recently proposed phenomenological model, can be discussed in terms of the global features of spatiotemporal maps of intermediate scattering functions. The new perspective offered by the spatiotemporal mapping method should prove useful for the study of liquid dynamics in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tracking seasonal variability in plant traits from spaceborne PRISMA and NEON AOP across forest types and ecoregions

Plant traits serve as critical indicators of how plants adapt to environmental changes and influence ecosystem functions. While airborne hyperspectral remote sensing effectively maps plant traits through detailed reflectance properties, it is limited by cost and scale, making large-scale and temporal studies challenging. The recently launched spaceborne hyperspectral imager, PRecursore IperSpettrale della Missione Applicativa (PRISMA), offers frequent, large scale and high-fidelity observations on a spatial resolution of 30 m and a revisit time of around 29 days, making it suitable for large-scale seasonal trait mapping. However, their potential remains largely unexplored. This study developed a multi-stage framework by leveraging the PRISMA spaceborne hyperspectral data and National Ecological Observatory Network (NEON) Airborne Observation Platform (AOP) hyperspectral data to investigate the seasonal dynamics of four key plant traits — chlorophyll content, carotenoid content, equivalent water thickness, and nitrogen content — across eleven NEON sites representing diverse forest types and ecoregions in the contiguous U.S. Our results demonstrated that PRISMA hyperspectral data can reliably track seasonal variability in plant traits, achieving overall R 2 values ranging from 0.78 to 0.88 and normalized root mean square error (NRMSE) values ranging from 5.4% to 8.4% for the four traits. Seasonal patterns revealed bell-shaped trajectories for chlorophyll and carotenoids, while equivalent water thickness decreased steadily across most sites, driven by structural changes during leaf maturation and senescence. Nitrogen content exhibited less pronounced seasonal variation but followed expected nutrient resorption patterns. Analysis of environmental drivers showed that seasonal variability is primarily controlled by solar radiation and day length in northern sites, vapor pressure in semi-arid regions, and temperature in mid-southeastern sites. Spatial variability, meanwhile, was primarily driven by soil properties, particularly during the peak growing season. However, the influence of soil variables slightly declines toward the end of the season at several sites, as climatic factors become more prominent. This study highlights the capability of PRISMA, and potentially other similar spaceborne hyperspectral data for large-scale, time-series plant trait mapping and provides valuable insights into the interactions between plant traits and environmental factors. In conclusion, these findings contribute to advancing our understanding of plant functional ecology and improving predictions of ecosystem responses to environmental changes.

Environmental drivers↗

Multi-dimensional incoherent Thomson scattering system in PHAse Space MApping (PHASMA) facility

A multi-dimensional incoherent Thomson scattering diagnostic system capable of measuring electron temperature anisotropies at the level of the electron velocity distribution function (EVDF) is implemented on the PHAse Space MApping facility to investigate electron energization mechanisms during magnetic reconnection. This system incorporates two injection paths (perpendicular and parallel to the axial magnetic field) and two collection paths, providing four independent EVDF measurements along four velocity space directions. For strongly magnetized electrons, a 3D EVDF comprised of two characteristic electron temperatures perpendicular and parallel to the local magnetic field line is reconstructed from the four measured EVDFs. As a result, validation of isotropic electrons in a single magnetic flux rope and a steady-state helicon plasma is presented.

47 OTHER INSTRUMENTATION↗

Quantum magic and multipartite entanglement in the structure of nuclei

Motivated by the Gottesman-Knill theorem, we present a detailed study of the quantum complexity of p -shell and s d -shell nuclei. Valence-space nuclear shell-model wave functions generated by the code are mapped to qubit registers using the Jordan-Wigner mapping (12 qubits for the p shell and 24 qubits for the s d shell), from which measures of the many-body entanglement ( n -tangles) and magic (nonstabilizerness) are determined. While exact evaluations of these measures are possible for nuclei with a modest number of active nucleons, Monte Carlo simulations are required for the more complex nuclei. The broadly applicable Pauli-string I ̂ Z ̂ exact (PSIZe) Markov chain Monte Carlo (MCMC) technique is introduced to accelerate the evaluation of measures of magic in deformed nuclei (with hierarchical wave functions), by factors of ≈ 8 for some nuclei. Significant multinucleon entanglement is found in the s d shell, dominated by proton-neutron configurations, along with significant measures of magic. This is evident not only for the deformed states, but also for nuclei on the path to instability via regions of shape coexistence and level inversion. These results indicate that quantum-computing resources will accelerate precision simulations of such nuclei and beyond. Published by the American Physical Society 2025

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Liquid Sorption-Enhanced Haber–Bosch Process

The use of a liquid sorbent in a traditional Haber-Bosch process enables significant improvements in energy efficiency and potential cost savings for arguably the most important chemical process on the planet. The approach presented in this report employs an incompressible liquid sorbent that absorbs and releases ammonia (NH 3 ) under specific conditions. To achieve this, we investigate reactions of ammonia and pure phosphoric acid (H 3 PO 4 , PA), which rapidly neutralize to form an equilibrated solution of monoammonium phosphate (MAP) and diammonium phosphate (DAP) that functions as a reversible and regenerable sorbent. Through intimate contact of the gas-phase Haber-Bosch reaction mixture with this liquid absorbent, complete equilibrium uptake may be achieved in an appropriately sized separator, and facile separation occurs through the use of independent liquid and gas phases. Following depressurization and release of the ammonia product, only the incompressible fluid needs to be repressurized and returned to the reactor. This study documents proof-of-concept absorption and desorption experiments carried out in 75 mL batch reactors, predominantly charged with precise MAP and DAP mixtures that equilibrate at process-relevant temperatures and pressures. We then assemble the first thermodynamic relationships that underlie this advantaged separation strategy, validated by reactive force field (ReaxFF) interatomic potential simulations, and benchmarked with traditional separation routes via process modeling and technoeconomic analysis. The scale of energy consumption in the century-old Haber-Bosch process is massive, and the elegant liquid sorption approach reported here offers opportunities to enhance its energy efficiency for the next frontier of ammonia synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Liquid Fuel Qualification for Molten Salt Reactors: Identification of Gaps and Challenges

This report identifies and describes challenges in implementing the MSR fuel qualification process described in NUREG/CR-7299 Fuel Qualification for Molten Salt Reactors. This report provides additional information including examples and additional use case descriptions to assist applicants in understanding the content and structure of the information necessary to develop a fuel qualification report. In particular, the current report emphasizes the relationship of fuel salt qualification to the contents of the plant safety analysis report. This report is limited to the safety functions relevant to the reactor aspects of the nuclear power plant. MSRs that include significant fuel salt processing would also need to address the safety aspects of the processing facility. No significant gaps were found in NUREG/CR-7299. However, NUREG/CR-7299 focuses on generic descriptions of how the fuel salt supports achievement of plant fundamental safety functions. A fuel salt qualification report will need explicitly address the role of the fuel salt in meeting regulatory requirements for a particular plant. NUREG/CR-7299 also provides a regulatory mapping between NRC rules and the safety functions. However, by remaining at a fundamental level, NUREG/CR-7299 does not address plant specific safety analysis. Some aspects of the safety analysis may require additional emphasis for designs that incorporate particular features (such as additional confirmation of decay heat rejection performance for higher power reactors). This report provides additional structure to enable an applicant to develop their plant-specific safety analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Growth of Nanometer-Thick γ-InSe on Si(111) 7 × 7 by Molecular Beam Epitaxy for Field-Effect Transistors and Optoelectronic Devices

γ-InSe is a semiconductor that holds promising potential in high-performance field-effect transistors and optoelectronic devices. Large-scale, single-phase γ-InSe deposition has proven challenging because of the difficulty in precise control of stoichiometry and the coexistence of different indium selenide phases. In this study, we demonstrate the wafer-scale combinatorial approach to map out the growth window as functions of the Se/In ratio and growth temperature for γ-InSe on the Si(111) 7 × 7 substrate in molecular beam epitaxy. X-ray diffraction (XRD) was used to identify the indium selenide phases, while atomic force microscopy revealed four distinct surface morphologies of γ-InSe, enabling a discussion of the growth mechanisms associated with each morphology. Cross-sectional atomic resolution scanning transmission electron microscopy confirmed that the film was of high crystalline quality and had nearly single-phase γ-InSe. In conclusion, our comprehensive study elucidates the In–Se phase map for thin film growth parameters, providing invaluable landmarks for the reproducible synthesis of high-quality γ-InSe layers.

36 MATERIALS SCIENCE↗

Wave-packet manipulation of He Rydberg states by a seeded free-electron laser

We report a two-dimensional pump-control-probe spectroscopic study of the dynamics of singly excited He Rydberg-state wave packets with a seeded extreme ultraviolet (XUV) free-electron laser (FEL) source. A pair of coherent XUV pulses, defined by their coarse time separation and relative phase, created and manipulated the wave packets. The He atoms were postionized by infrared (IR) pulses, and the ion yield was measured as a function of XUV phase and IR arrival time. We tagged and sorted the relative phase of the XUV pulse pair on a single-shot basis by fitting each FEL spectrum with a suitable function that accounts for nonidealities of the XUV pulse pairs, associated with the seeding process; more generally, the fit returns the time-dependent electric field of the FEL spectra. The experimental two-dimensional maps of ion yields, measured as a function of IR (probe) delay and of XUV (pump-control) phase, were compared with the solution of the first-order time-dependent Schrödinger equation for this field. Despite the fact that the experimental conditions imply strong excitation, beyond the approximations of first-order perturbation theory, the simulated map satisfactorily reproduces the experimental one for temporally well-separated pulses. We show that by selecting data at appropriate values of pump-control phase, we enhance or suppress the amplitude of chosen wave-packet components consisting of two or more Rydberg states. When the temporal overlap of the pulse pair cannot be neglected, the phase reconstruction is underdetermined, and we provide a simplified comparison between data and simulations. Published by the American Physical Society 2024

Dumergue, Mathieu (ORCID:0000000236984406)↗

Thermochemical Data Fusion Using Graph Representation Learning

Large databases are required for “Big Data” applications in catalysis and materials science. Thermochemical databases can be created by combining data from various sources and by correcting low-fidelity datasets to higher accuracy with minimal computation. To achieve this “data fusion”, thermochemical quantities of interest, calculated at various levels of density functional theory (DFT), need to be mapped to the same, high levels of theory. In this work, a graph theoretical, statistical framework is proposed for such tasks. Subgraph frequencies are shown to provide a natural representation for learning these fusion maps. The maps are linear and are learnt with automated descriptor selection. Using a dataset of as few as ~1% from the QM9 database of 133,885 molecules, these models can predict multiple thermochemical quantities at a higher level of theory with an accuracy of 1 kcal/mol. Here, the method is explainable, generalizable, and provides a diagnostic tool for outlier identification

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pattern formation and flocking for particles near the jamming transition on resource gradient substrates

Here, we numerically examine a bidisperse system of active and passive particles coupled to a resource substrate. The active particles deplete the resource at a fixed rate and move toward regions with higher resources, while all of the particles interact sterically with each other. We show that at high densities, this system exhibits a rich variety of pattern-forming phases along with directed motion or flocking as a function of the relative rates of resource absorption and consumption as well as the active to passive particle ratio. These include partial phase separation into rivers of active particles flowing through passive clusters, strongly phase separated states where the active particles induce crystallization of the passive particles, mixed jammed states, and fluctuating mixed fluid phases. For higher resource recovery rates, we demonstrate that the active particles can undergo motility-induced phase separation, while at high densities, there can be a coherent flock containing only active particles or a solid mixture of active and passive particles. The directed flocking motion typically shows a transient in which the flow switches among different directions before settling into one direction, and there is a critical density below which flocking does not occur. We map out the different phases as function of system density, resource absorption and recovery rates, and the ratio of active to passive particles.

97 MATHEMATICS AND COMPUTING↗

A Principled Framework to Assess the Information-Theoretic Fitness of Brain Functional Sub-Circuits

In systems and network neuroscience, many common practices in brain connectomic analysis are often not properly scrutinized. One such practice is mapping a predetermined set of sub-circuits, like functional networks (FNs), onto subjects’ functional connectomes (FCs) without adequately assessing the information-theoretic appropriateness of the partition. Another practice that goes unchallenged is thresholding weighted FCs to remove spurious connections without justifying the chosen threshold. This paper leverages recent theoretical advances in Stochastic Block Models (SBMs) to formally define and quantify the information-theoretic fitness (e.g., prominence) of a predetermined set of FNs when mapped to individual FCs under different fMRI task conditions. Our framework allows for evaluating any combination of FC granularity, FN partition, and thresholding strategy, thereby optimizing these choices to preserve the important topological features of the human brain connectomes. By applying to the Human Connectome Project with Schaefer parcellations at multiple levels of granularity, the framework showed that the common thresholding value of 0.25 was indeed information-theoretically valid for group-average FCs, despite its previous lack of justification. Our results pave the way for the proper use of FNs and thresholding methods, and provide insights for future research in individualized parcellations.

Duong-Tran, Duy (ORCID:0009000944967575)↗

Presentation of gas-phase-reactant-accessible single-rhodium-atom catalysts for CO oxidation, via MOF confinement of an Anderson polyoxometalate

Geometric or electronic confinement of guests within nanoporous hosts holds promise for imparting catalytic functionality, including single-metal-atom catalytic functionality, to existing materials. When the nanoporous host is a metal–organic framework (MOF), single-metal-ion catalysts have typically been installed by grafting to an open site on an inorganic node, with the node effectively becoming the support for the catalyst. This approach, however, imposes compositional constraints, as the node not only needs to be receptive to grafting, but also must be capable of stabilizing the framework against solvent evacuation, chemical exposure, and heating. Here, we show that disk-like, Anderson polyoxometalate clusters (RhMo 6 O 24 n- and Mo 7 O 24 m- ; POMs) can be confined in pore-specific and orientation-specific fashion within the hierarchically porous, Zr(IV)-based MOF, NU1K. Self-limiting loading of one cluster per pore, and associated nano-confinement, serve to isolate each POM and prevent consolidation caused by sintering. Additionally, the oriented confinement serves to expose individual rhodium atoms to candidate gas-phase reactants, while enabling the rhodium atom to employ a well-defined oxy-molybdenum cluster, rather than a MOF node, as a support. Synchrotron-based difference-electron-density maps and differential pair-distribution-function analyses of scattered X-rays establish cluster siting and orientation and confirm isolation. Nanoconfined (i.e., MOF- and POM-confined) single-rhodium(III)-atoms are catalytically competent for an illustrative gas-phase reaction, CO oxidation by O 2 , with the MOF-isolated POM enormously outperforming nonporous, MOF-free, solid (NH 4 ) 3 [H 6 RhMo 6 O 24 ]·6H 2 O. This paper highlights the value of MOF-based nano-confinement and oriented isolation of planar POMs as a means of uniformly presenting and stabilizing potent single-metal-atom catalysts, in reactant-accessible form, on well-defined supports.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale Phase Identification Using Two-Dimensional Pair Correlation Functions: A Case Study on Hafnium Oxide

Accurate identification of local phases in nanocrystalline materials is essential for understanding their functional properties, but it remains a significant challenge for polymorphic materials to locally differentiate them at nanoscale. This challenge is further compounded in polycrystalline materials with randomly oriented grains and the coexistence of multiple phases. In this report, we present a methodology for phase and orientation identification at the nanoscale by leveraging vector pair correlation functions extracted from atomically resolved scanning transmission electron microscopy (STEM) images. We demonstrate the accuracy of the methodology on both simulated and experimental data from HfO 2 -based films, a material that exhibits multiple coexisting phases in films with thicknesses ranging from 5 to 20 nm. While demonstrated on HfO 2 films, the methodology can be extended to other polymorphic nanocrystalline systems with complex phase coexistence.

36 MATERIALS SCIENCE↗

Evolution of magnetic field induced ordering in the layered quantum Heisenberg triangular-lattice antiferromagnet Ba 3 CoSb 2 O 9

Quantum fluctuations in the effective spin-12 layered triangular-lattice quantum Heisenberg antiferromagnet Ba 3 CoSb 2 O 9 lift the classical degeneracy of the antiferromagnetic ground state in magnetic field, producing a series of novel spin structures for magnetic fields applied within the crystallographic ab plane, including a celebrated collinear “up-up-down” spin ordering with magnetization equal to 1/3 of the saturation magnetization over an extended field range. Theoretically unresolved, however, are the effects of interlayer antiferromagnetic coupling and transverse magnetic fields on the ground states of this system. Additional magnetic field induced phase transitions are theoretically expected and in some cases have been experimentally observed, but details regarding their number, location, and physical character appear inconsistent with the predictions of existing models. Conversely, an absence of experimental measurements as a function of magnetic-field orientation has left other key predictions of these models untested. To address these issues, in this study we have used specific heat, neutron diffraction, thermal conductivity, and magnetic torque measurements to map out the phase diagram as a function of magnetic field intensity and orientation relative to the crystallographic ab plane. For H||ab, we have discovered an additional magnetic field induced phase transition at low temperature and an unexpected tetracritical point in the high-field phase diagram, which coupled with the apparent second-order nature of the phase transitions eliminates several theoretically proposed spin structures for the high-field phases. Our calorimetric measurements as a function of magnetic field orientation are in general agreement with theory for field-orientation angles close to plane parallel (H||a) but diverge at angles near plane perpendicular; a predicted convergence of two phase boundaries at finite angle and a corresponding change in the order of the field induced phase transition are not observed experimentally. Our results emphasize the role of interlayer coupling in selecting and stabilizing field induced phases, provide guidance on the nature of the magnetic order in each phase, and reveal the need for new physics to account for the nature of magnetic ordering in this archetypal two-dimensional spin-12 triangular-lattice quantum Heisenberg antiferromagnet.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A VR-based volumetric medical image segmentation and visualization system with natural human interaction

Volume rendering produces informative two-dimensional (2D) images from a 3-dimensional (3D) volume. It highlights the region of interest and facilitates a good comprehension of the entire data set. However, volume rendering faces a few challenges. First, a high-dimensional transfer function is usually required to differentiate the target from its neighboring objects with subtle variance. Unfortunately, designing such a transfer function is a strenuously trial-and-error process. Second, manipulating/visualizing a 3D volume with a traditional 2D input/output device suffers dimensional limitations. To address all the challenges, we design NUI-VR 2 , a natural user interface-enabled volume rendering system in the virtual reality space. NUI-VR 2 marries volume rendering and interactive image segmentation. It transforms the original volume into a probability map with image segmentation. A simple linear transfer function will highlight the target well in the probability map. More importantly, we set the entire image segmentation and volume rendering pipeline in an immersive virtual reality environment with a natural user interface. NUI-VR 2 eliminates the dimensional limitations in manipulating and perceiving 3D volumes and dramatically improves the user experience.

42 ENGINEERING↗

RAD51C-XRCC3 structure and cancer patient mutations define DNA replication roles

$RAD51C$ is an enigmatic predisposition gene for breast, ovarian, and prostate cancer. Currently, missing structural and related functional understanding limits patient mutation interpretation to homology-directed repair (HDR) function analysis. Here we report the RAD51C-XRCC3 (CX3) X-ray co-crystal structure with bound ATP analog and define separable RAD51C replication stability roles informed by its three-dimensional structure, assembly, and unappreciated polymerization motif. Mapping of cancer patient mutations as a functional guide confirms ATP-binding matching RAD51 recombinase yet highlights distinct CX3 interfaces. Analyses of CRISPR/Cas9-edited human cells with $RAD51C$ mutations combined with single-molecule, single-cell and biophysics measurements uncover discrete CX3 regions for DNA replication fork protection, restart and reversal, accomplished by separable functions in DNA binding and implied 5’ RAD51 filament capping. Collective findings establish CX3 as a cancer-relevant replication stress response complex, show how HDR-proficient variants could contribute to tumor development, and identify regions to aid functional testing and classification of cancer mutations.

59 BASIC BIOLOGICAL SCIENCES↗

A method for convex black-box integer global optimization

Here we study the problem of minimizing a convex function on a nonempty, finite subset of the integer lattice when the function cannot be evaluated at noninteger points. We propose a new underestimator that does not require access to (sub)gradients of the objective; such information is unavailable when the objective is a blackbox function. Rather, our underestimator uses secant linear functions that interpolate the objective function at previously evaluated points. These linear mappings are shown to underestimate the objective in disconnected portions of the domain. Therefore, the union of these conditional cuts provides a nonconvex underestimator of the objective. We propose an algorithm that alternates between updating the underestimator and evaluating the objective function. We prove that the algorithm converges to a global minimum of the objective function on the feasible set. We present two approaches for representing the underestimator and compare their computational effectiveness. We also compare implementations of our algorithm with existing methods for minimizing functions on a subset of the integer lattice. We discuss the difficulty of this problem class and provide insights into why a computational proof of optimality is challenging even for moderate problem sizes.

97 MATHEMATICS AND COMPUTING↗

Systematic discovery of new nano-scale metastable intermetallic eutectic phases in laser rapid solidified Aluminum-Germanium alloy

Laser surface remelting of as-cast Al-Ge eutectic alloy is shown to produce ultrafine lamellar eutectic morphology with interlamellar spacing refined up to ∼60 nm and composed of FCC Al solid solution and unusual Al x Ge y intermetallic phases that do not form during near-equilibrium solidification. The microstructures are characterized and analyzed using a combination of selected area electron diffraction, high-resolution scanning transmission electron microscopy, energy dispersive X-ray spectroscopy to obtain high-resolution elemental maps, and atomistic modeling using density functional theory followed by atomic-scale image simulation. Depending on the local solidification conditions, the crystallography of the Al x Ge y intermetallic phases in the eutectic microstructure is either monoclinic (C 2/c) or monoclinic (P 2 1 ), with high densities of defects in both cases. This is in sharp contrast to the as-cast alloys that showed nominally pure Al and Ge phases with significant solute partitioning and equilibrium FCC and diamond cubic crystal structures, respectively. Corresponding kinetic phase diagrams are proposed to interpret the evolution of nano-lamellar eutectic morphologies with equilibrium Al and metastable Al x Ge y phases, and to explain increased solid solubility in the Al phases manifested by precipitation of ultrafine clusters of Ge. Furthermore, the reasons for the formation of these metastable eutectics under laser rapid solidification are discussed from the perspective of the competitive growth criterion.

Al-Ge eutectic↗