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At least 271 records · Page 15

[18F]Tosyl fluoride as a versatile [18F]fluoride source for the preparation of 18F-labeled radiopharmaceuticals

Abstract Positron emission tomography (PET) is an in vivo imaging technology that utilizes positron-emitting radioisotope-labeled compounds as PET radiotracers that are commonly used in clinic and in various research areas, including oncology, cardiology, and neurology. Fluorine-18 is the most widely used PET-radionuclide and commonly produced by proton bombardment of 18 O-enriched water in a cyclotron. The [ 18 F]fluoride thus obtained generally requires processing by azeotropic drying in order to completely remove H 2 O before it can be used for nucleophilic radiofluorination. In general, the drying step is important in facilitating the radiofluorination reactions and the preparation of 18 F-labeled PET radiotracers. In this communication, we have demonstrated the feasibility of using [ 18 F]tosyl fluoride ([ 18 F]TsF) as a versatile [ 18 F]fluoride source for radiofluorination to bypass the azeotropic drying step, and we have developed a continuous flow solid-phase radiosynthesis strategy to generate [ 18 F]TsF in a form that is excellent for radiofluorination. [ 18 F]TsF shows high reactivity in radiofluorination and provides the features suitable for preparing PET radiotracers on a small scale and exploring novel radiolabeling technologies. Thus, using [ 18 F]TsF as a [ 18 F]fluoride source is a promising strategy that facilitates radiofluorination and provides a convenient and efficient solution for the preparation of 18 F-labeled radiopharmaceuticals that is well matched to the emerging trends in PET imaging technologies.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

An intercomparison of wall fluxes in a turbulent thermal convection chamber: Direct numerical simulations and wall-modeled large-eddy simulations enhanced by machine learning

Thermal convection in a closed chamber is driven by a warm bottom, a cold top, and side walls at various temperatures. Although wall fluxes are the source of convection energy, accurately modeling these fluxes (i.e., the wall model) is challenging. In large-eddy simulations (LESs), many wall models are traditionally derived from the canonical boundary layer, which may be unsuitable for thermal convection bounded by both horizontal and vertical walls. This study conducts a model intercomparison of dry convection in a cubic-meter chamber using three direct numerical simulations (DNSs) and four LESs with different wall models. The LESs employ traditional wall models, a new wall model employing physics-aware neural networks, and a refined grid near the walls. The experiment involves four cases with varying sidewall temperatures. Our results show that LESs capture the main flow features and the trends of mean fluxes. The physics-aware neural networks and refined wall grids can improve the temporally averaged local fluxes when the large-scale circulation has a preferred direction. Even without the local improvement of wall fluxes, the LES flow quantities (temperature and velocities) can still largely match those in DNSs, provided the mean flux largely matches the DNSs. Additionally, DNSs reveal that a variation in corner treatments has minimal impacts on the flow quantities away from corners. Finally, LESs underestimate the mean fluxes of the entire wall due to their inability to resolve corner regions, but their mean flux away from the corner can better match DNS.

54 ENVIRONMENTAL SCIENCES↗

Optical conductivity of layered topological semimetal TaNiTe 5

Here, we present an infrared spectroscopy study of the layered topological semimetal TaNiTe 5 , a material with a quasi-one-dimensional structure and strong in-plane anisotropy. Despite its structural features, infrared reflectivity and electronic transport measurements along the 𝑎 and 𝑐 crystallographic axes show metallic behavior without evidence of reduced dimensionality. Optical conductivity reveals an anisotropic but conventional metallic response with low scattering rates and a single sharp infrared-active phonon mode at 396cm −1 ⁢(49meV). Ab initio calculations closely match the experimental optical data and confirm a three-dimensional electronic structure. Our results demonstrate that TaNiTe 5 behaves as a three-dimensional anisotropic semimetal in its electronic and optical properties.

36 MATERIALS SCIENCE↗

Shutdown dose rate analysis with the Shift Monte Carlo radiation transport code and modular verification workflow

Calculation of the shutdown dose rate is crucial for safe fusion reactor operations. The Rigorous-two-step (R2S) method is a method that requires connected neutron transport, activation, and gamma transport. Shift has integrated variance reduction with a deterministic solver Denovo, supports multiple geometry formats, and is scalable. These features make it an attractive transport solver choice for an R2S workflow. An R2S workflow for the Shift Monte Carlo code is developed and compared to the existing Oak Ridge National Laboratory Shutdown Dose Rate Code Suite (ORCS) workflow. Also, a Python framework for integrating two R2S workflows is developed to mix and match each step in the R2S workflow for improved collaboration and verification experience. In this study, results show that the Shift-Denovo R2S workflow and the ORCS workflow calculate the shutdown dose rate of the ITER Shutdown Dose Rate benchmark problem with an average relative error of 2.285%.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Clusters have edges: the projected phase-space structure of SDSS redMaPPer clusters

ABSTRACT We study the distribution of line-of-sight velocities of galaxies in the vicinity of Sloan Digital Sky Survey (SDSS) red-sequence Matched-filter Probabilistic Percolation (redMaPPer) galaxy clusters. Based on their velocities, galaxies can be split into two categories: galaxies that are dynamically associated with the cluster, and random line-of-sight projections. Both the fraction of galaxies associated with the galaxy clusters, and the velocity dispersion of the same, exhibit a sharp feature as a function of radius. The feature occurs at a radial scale Redge ≈ 2.2Rλ, where Rλ is the cluster radius assigned by redMaPPer. We refer to Redge as the ‘edge radius’. These results are naturally explained by a model that further splits the galaxies dynamically associated with a galaxy cluster into a component of galaxies orbiting the halo and an infalling galaxy component. The edge radius Redge constitutes a true ‘cluster edge’, in the sense that no orbiting structures exist past this radius. A companion paper tests whether the ‘halo edge’ hypothesis holds when investigating the full three-dimensional phase-space distribution of dark matter substructures in numerical simulations, and demonstrates that this radius coincides with a suitably defined splashback radius.

79 ASTRONOMY AND ASTROPHYSICS↗

Bioengineered algal lipids enriched in structured medium- and long-chain triacylglycerols, linoleate, and sn -2 palmitate for human milk fat substitutes

Human milk fat (HMF) contains triacylglycerol (TAG) as its primary component, providing over 50% of the calories for infant nutrition, along with structural and bioactive lipids that are important for immune and nervous system development. Palmitic acid, comprising 20-25% of the fatty acid complement of HMF, is predominantly esterified to the sn -2 position on the glycerol backbone. This regiospecific positioning facilitates absorption as 2-palmitoyl-monoacylglycerol after hydrolysis of the fatty acids at sn -1 and sn -2 by gut lipases. Other features of HMF include enrichment in structured medium- and long-chain triglycerides (MLCTs), and variation in the ratio of oleic acid to linoleic acid with maternal diet and geography. We have engineered Auxenochlorella, an oleaginous green alga, for biosynthesis of an MLCT- and sn -2 palmitate-enriched HMF substitute for infant formula, matching the regioisomeric composition and proportions of the most abundant fatty acids in HMF.

Lin, Jon Y-T [University of California, Berkeley;]↗

Redox‐Mediated Electrochemical Regeneration of Spent LiFePO 4 Battery Cathodes

Direct recycling of lithium-ion battery cathodes offers considerable appeal over metallurgical approaches. Here, we demonstrate a mediated electrochemical method for direct regeneration of degraded LiFePO 4 (LFP). The approach uses a redox mediator, iron propylenediamine tetraacetate, that undergoes electrochemical reduction and is circulated through an external reservoir, where it supplies the electrons needed to regenerate LFP in the presence of Li + ions derived from LiOH oxidation. Rapid outer-sphere electron transfer is observed from the mediator to the degraded LFP material. This feature, together with good aqueous solubility of the mediator (0.3 M), supports current densities up to 100 mA/cm 2 , and this electrochemical recycling process is demonstrated on 100 g scale. 57 Fe Mössbauer spectroscopy is used to monitor the correction of structural defects in the degraded LFP, providing the basis for regeneration of LFP that matches the electrochemical performance of pristine LFP.

Electrochemical Relithiation↗

Direct Observation of the ππ* to nπ* Transition in 2-Thiouracil via Time-Resolved NEXAFS Spectroscopy

The photophysics of nucleobases has been the subject of both theoretical and experimental studies over the past decades due to the challenges posed by resolving the steps of their radiationless relaxation dynamics, which cannot be described in the framework of the Born–Oppenheimer approximation (BOA). In this context, the ultrafast dynamics of 2-thiouracil has been investigated with a time-resolved NEXAFS study at the Free Electron Laser FLASH. Near Edge X-ray Absorption Fine Structure spectroscopy (NEXAFS) can be used to observe electronic transitions in ultrafast molecular relaxation. We performed time-resolved UV-pump/X-ray probe absorption measurements at the sulfur 2s (L1) and 2p (L2/3) edges. We are able to identify absorption features corresponding to the S2 (ππ*) and S1 (nπ*) electronic states. We observe a delay of 102 ± 11 fs in the population of the nπ* state with respect to the initial optical excitation and interpret the delay as the time scale for the S2 → S1 internal conversion. We furthermore identify oscillations in the absorption signal that match a similar observation in our previous X-ray photoelectron spectroscopy study on the same molecule.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A high fidelity and user-friendly equation-oriented optimization model for carbon capture using a novel water-lean solvent

Research Triangle Institute (RTI) International and SLB have developed a novel water-lean solvent technology for carbon capture, demonstrating low specific reboiler duty (SRD) values at capture rates exceeding 90%. At the Technology Centre Mongstad (TCM) pilot plant, the technology achieved an SRD of 2.55 GJ/t-CO2 at 95% capture, utilizing an intercooler and a 5°C temperature approach in the lean/rich solvent cross exchanger. To meet varying carbon capture targets for Front End Engineering and Design (FEED) studies and to enable real-time optimization and advanced process control, an efficient optimization model is required. This model needs to minimize energy demand for a given capture rate and determine optimal operating parameters in response to fluctuating flue gas conditions. While an existing Aspen Plus simulation model, developed by RTI and SLB, accurately matches TCM plant data, its sequential modular (SM) strategy is too slow for real-time applications due to recycle streams and tight heat integration inherent in solvent-based carbon capture processes. Although an equation-oriented (EO) modeling strategy is more suitable for optimizing these processes, its adoption has been limited by several factors: feature limitations in Aspen Plus EO mode (e.g., lack of balance block support), a less user-friendly interface for variable identification and loop solving, complex troubleshooting of convergence issues, and the necessity for accurate initial values.

carbon capture↗

Analysis of the 2021 Milford, Utah earthquake swarm: Enhanced earthquake catalog and migration patterns

An earthquake swarm occurred in Spring 2021 in south-central Utah near the town of Milford. The University of Utah Seismograph Stations located 125 earthquakes between March 19 and May 10 with magnitudes ranging from 0.5 to 3.2. We implement a matched-filter technique in order to identify additional earthquakes that went undetected during the routine network location. The 125 network-located earthquakes are used as templates and are cross-correlated with continuous data for the dates Feb 17—June 10. This time period corresponds to approximately 1 month before the earthquake swarm began through 1 month after it ended. For the matched-filter analysis, we rely heavily on station FOR1, which is located within 5 km of most template events. Four other stations within 20–30 km of most template events provide a supplement to the closest station. The matched-filter implementation results in the detection of over 600 earthquakes in addition to the original 125 catalog events. This is one of the largest swarms ever recorded in Utah, and no previous large swarms have been recorded in this location. We use HypoDD to obtain relative double-difference locations of the catalog events. Both routine locations and HypoDD relocations of the catalog events suggest a fault dipping west beneath the mountain range, opposite of typical Basin and Range normal faults that dip beneath alluvial valleys. Moment tensors for the largest five events show normal faulting consistent with the west-dipping fault seen in the seismicity. Hydrothermal features in the area, including a geothermal power plant, suggest that fluids may be a contributing factor to the earthquake swarm triggering. We examine the role of fluids by exploring bounds on diffusion parameters and investigating spatial migration characteristics of the swarm seismicity. We conclude that this swarm is the result of heterogenous stress conditions in a prefractured region.

58 GEOSCIENCES↗

Methods to Evaluate Subcolumn Profiles Based on Two-Point Diagnostics

In atmospheric models, stochastic generation of subgrid-scale profiles or “subcolumns” has been used for a variety of purposes. Such subcolumns can be generated from subgrid probability density functions (PDFs) at different vertical levels, when such PDFs are available. To do so, the generator needs to decide how strongly points should be correlated in the vertical, that is, how much the values should be overlapped. This is sometimes called “PDF overlap.” To assess vertical correlation in a simplified, observable setting, here the vertical correlation of vertical velocity in subcloud layers is examined. Doppler lidar is used to evaluate the vertical profiles of vertical velocity produced by a large-eddy simulation (LES) model and the Subgrid Importance Latin Hypercube Sampler (SILHS) subcolumn generator. In order to diagnose unrealistic features in subcolumn profiles, various statistical diagnostics are examined here, including the bivariate PDF of vertical velocity at two separated points (i.e., altitudes), the two-point velocity correlation, the integral correlation length, the PDF of two-point velocity differences, and the skewness and kurtosis of two-point velocity differences. The profiles produced by LES match lidar well, except that they are too smooth at small scales. The profiles produced by SILHS exhibit sharp jumps from updraft to downdraft that are not observed in the lidar data. To reduce the generation of these unrealistically sharp jumps, the SILHS sampling method is revised. The diagnostics confirm that the revised sampling method reduces the overprediction of sharp jumps.

54 ENVIRONMENTAL SCIENCES↗

Signatures of fractional charges via anyon–trions in twisted MoTe 2

Fractionalization of the electron charge e is one of the most striking phenomena arising from strong electron–electron interactions. A celebrated example is the emergence of anyons with fractional charges in fractional quantum Hall effect (FQHE) states. Recently, zero-field fractional Chern insulators (FCIs), lattice analogues of the FQHE states that form without Landau levels, have been realized. FCIs provide a unique platform to investigate anyons, yet their detection remains a challenge. Here we report the observation of anyon–trions, a new type of excitonic complex formed by binding a trion with a fractional charge in twisted MoTe 2 bilayers. Photoluminescence spectroscopy of quantum-confined excitons reveals emergent peaks that appear only within slightly doped FCI states. The new spectral features are red-shifted relative to the trions in undoped FCIs, but share the same electric field, temperature and magnetic field dependence. These observations suggest their origin as trions binding with elementary quasi-particles, that is, anyon–trions. Crucially, the ratio of binding energies between the anyon–trions in the −2/3 and −3/5 FCI states matches the expected fractional charge ratio of e/3 to e/5. This provides strong evidence for fractional charges in FCI—an essential property of anyons. Our results address a fundamental question in FCI physics and establish trion spectroscopy as a powerful probe of fractionally charged excitations, complementary to transport- and tunnelling-based approaches.

Quantum Hall↗

Ecophysiological and genomic analyses of a representative isolate of highly abundant Bacillus cereus strains in contaminated subsurface sediments

Abstract Bacillus cereus strain CPT56D‐587‐MTF (CPTF) was isolated from the highly contaminated Oak Ridge Reservation (ORR) subsurface. This site is contaminated with high levels of nitric acid and multiple heavy metals. Amplicon sequencing of the 16S rRNA genes (V4 region) in sediment from this area revealed an amplicon sequence variant (ASV) with 100% identity to the CPTF 16S rRNA sequence. Notably, this CPTF‐matching ASV had the highest relative abundance in this community survey, with a median relative abundance of 3.77% and comprised 20%–40% of reads in some samples. Pangenomic analysis revealed that strain CPTF has expanded genomic content compared to other B. cereus species—largely due to plasmid acquisition and expansion of transposable elements. This suggests that these features are important for rapid adaptation to native environmental stressors. We connected genotype to phenotype in the context of the unique geochemistry of the site. These analyses revealed that certain genes (e.g. nitrate reductase, heavy metal efflux pumps) that allow this strain to successfully occupy the geochemically heterogenous microniches of its native site are characteristic of the B. cereus species while others such as acid tolerance are mobile genetic element associated and are generally unique to strain CPTF.

59 BASIC BIOLOGICAL SCIENCES↗

Viral but not bacterial community successional patterns reflect extreme turnover shortly after rewetting dry soils

As central members of soil trophic networks, viruses have the potential to drive substantial microbial mortality and nutrient turnover. Pinpointing viral contributions to terrestrial ecosystem processes remains a challenge, as temporal dynamics are difficult to unravel in the spatially and physicochemically heterogeneous soil environment. In Mediterranean grasslands, the first rainfall after seasonal drought provides an ecosystem reset, triggering microbial activity during a tractable window for capturing short-term dynamics. In this report we simulated precipitation in microcosms from four distinct dry grassland soils and generated 144 viromes, 84 metagenomes and 84 16S ribosomal RNA gene amplicon datasets to characterize viral, prokaryotic and relic DNA dynamics over 10 days. Vastly different viral communities in each soil followed remarkably similar successional trajectories. Wet-up triggered a significant increase in viral richness, followed by extensive compositional turnover. Temporal succession in prokaryotic communities was much less pronounced, perhaps suggesting differences in the scales of activity captured by viromes (representing recently produced, ephemeral viral particles) and total DNA. Still, differences in the relative abundances of Actinobacteria (enriched in dry soils) and Proteobacteria (enriched in wetted soils) matched those of their predicted phages, indicating viral predation of dominant bacterial taxa. Rewetting also rapidly depleted relic DNA, which subsequently reaccumulated, indicating substantial new microbial mortality in the days after wet-up, particularly of the taxa putatively under phage predation. Production of abundant, diverse viral particles via microbial host cell lysis appears to be a conserved feature of the early response to soil rewetting, and results suggest the potential for ‘Cull-the-Winner’ dynamics, whereby viruses infect and cull but do not decimate dominant host populations.

54 ENVIRONMENTAL SCIENCES↗

PAC in DESI. II. Galaxy-halo connection into the $10^{6}{\rm M}_{\odot}$ frontier

Understanding dwarf galaxy formation is crucial for testing dark matter models and reionization physics. However, constructing stellar-mass complete spectroscopic samples at low masses is increasingly difficult, and the potential existence of a local void complicates studies in an average environment. The Photometric object Around Cosmic webs (PAC) method, which combines deep photometric and spectroscopic data to measure the excess surface density $\bar{n}_2w_{\rm{p}}(r_{\rm{p}})$ of photometric objects around spectroscopic tracers, offers a promising path forward. We model 349 $\bar{n}_2w_{\rm{p}}(r_{\rm{p}})$ measurements from DESI Y1 BGS and DECaLS, reaching $M_*=10^{6.4}\,{\rm M}_{\odot}$, using a stellar mass-halo mass relation (SHMR)-based subhalo abundance matching framework applied to two high-resolution $N$-body simulations from the Jiutian suite. The resulting SHMR is constrained down to $M_{\rm h}\simeq10^{8.0}\,h^{-1}{\rm M}_{\odot}$, revealing a clear upturn at $\sim10^{10.0}\,h^{-1}{\rm M}_{\odot}$ toward lower masses, indicating rising star-formation efficiency (SFE) in small haloes. This feature persists under extensions of the model that allow mass-dependent scatter, reionization-induced suppression of the halo occupation fraction, galaxy assembly bias, and alternative cosmologies. Combining with the results from Paper I, we find that central red galaxies dominate the low-mass regime. Our results motivate a hypothesis in which SFE is significantly higher than previously thought prior to reionization, enabling relatively massive galaxies to form in small haloes. These systems are subsequently quenched by the UV background, producing the central red dwarf galaxies observed. Finally, we obtain $3σ$ and $5σ$ upper mass bounds of $10^{8.80}\,h^{-1}{\rm M}_{\odot}$ and $10^{10.24}\,h^{-1}{\rm M}_{\odot}$ on the smallest haloes required to exist.

Xu, Kun [Pennsylvania U.; Durham U., ICC; Tsung-Da↗

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero‐Bicrystal

Abstract Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO 3 ) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO 3 ‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy. It is experimentally demonstrated that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and these results are quantitatively matched with a simple analytic model. Polaritonic cavity modes and polariton propagation along “forbidden” directions are also investigated in microscale bicrystals, which arise from the finite in‐plane dimension of the synthesized MoO 3 micro‐ribbons. The findings shed light on the unique dispersion properties of polaritons in van der Waals heterostructures and pave the way for applications leveraging deeply sub‐wavelength mid‐infrared light‐matter interactions.

36 MATERIALS SCIENCE↗

NUMERICAL MODELING OF A SOLID OXIDE FUEL CELL FOR USE IN REAL-TIME SIMULATION AND CYBER-PHYSICAL SYSTEMS

Cyber-physical systems provide a mechanism with which to investigate the physical phenomena and behavior of traditionally cost-prohibitive or otherwise fragile equipment. For the National Energy Technology Laboratory (NETL), this approach resulted in the Hybrid Performance (Hyper) facility which features a gas turbine-SOFC hybrid cycle utilizing real turbomachinery and a simulated SOFC stack. This allows for the investigation of combined cycle performance and control strategies, in an exhaustive manner, both without fear of destroying delicate state-of-the-art fuel cells, and with the full accuracy of real-world turbomachinery. Issues arose between the transient response of the SOFC model being limited to a sample time of 80 milliseconds, due to the calculation time of the SOFC model taking on average 40 milliseconds to calculate for a given timestep with spikes in calculation time reaching the 80 millisecond threshold. In order to be able to match the speed of transients from the turbomachinery and likewise better discern transient behavior, it was determined that the SOFC model must be optimized to operate at a sample time of 5 milliseconds. Therefore, it is necessary to optimize the SOFC model in order to decrease the calculation time from around 40 milliseconds, down to at the most 5 milliseconds. To do this, both the electrochemical algorithm and the thermal algorithm used to simulate the physical behavior of the SOFC are investigated to determine where improvements can be made. To this end the rootfinding numerical recipes of the electrochemical algorithm are investigated as the complex electrochemistry requires a highly iterative nested dual convergence loop to resolve the voltage-current relationship, and likewise the temporal discretization of the thermal algorithm is modified for the sake of higher accuracy and stability. Ultimately the new electrochemical algorithm featuring higher order rootfinding schemes proves to be efficient enough to reach the sub 5 millisecond target, signifying an order of magnitude reduction in calculation time, and when coupled with the new temporal discretization similar calculation time characteristics show that a fully implicit, higher order temporal discretization can also successfully be used if desired. Ultimately this result means that the cyber-physical simulation system can operate at higher sample rates, and resolve transient events at significantly higher resolution and fidelity.

Arias, Jesus↗

Phase Segmentation in Atom-Probe Tomography Using Deep Learning-Based Edge Detection

Abstract Atom-probe tomography (APT) facilitates nano- and atomic-scale characterization and analysis of microstructural features. Specifically, APT is well suited to study the interfacial properties of granular or heterophase systems. Traditionally, the identification of the interface between, for precipitate and matrix phases, in APT data has been obtained either by extracting iso-concentration surfaces based on a user-supplied concentration value or by manually perturbing the concentration value until the iso-concentration surface qualitatively matches the interface. These approaches are subjective, not scalable, and may lead to inconsistencies due to local composition inhomogeneities. We introduce a digital image segmentation approach based on deep neural networks that transfer learned knowledge from natural images to automatically segment the data obtained from APT into different phases. This approach not only provides an efficient way to segment the data and extract interfacial properties but does so without the need for expensive interface labeling for training the segmentation model. We consider here a system with a precipitate phase in a matrix and with three different interface modalities—layered, isolated, and interconnected—that are obtained for different relative geometries of the precipitate phase. We demonstrate the accuracy of our segmentation approach through qualitative visualization of the interfaces, as well as through quantitative comparisons with proximity histograms obtained by using more traditional approaches.

47 OTHER INSTRUMENTATION↗