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DOE OSTI2023

Octahedral Distortion and Excitonic Behavior of Cs 3 Bi 2 Br 9 Halide Perovskite at Low Temperature

The metal halide ionic octahedron, represented as [MX 6 ] $n$- (M = metal cation, X = halide anion), serves as the basic structural unit in halide perovskites and plays a crucial role in determining their optoelectronic and chemical properties. Thus, it is possible to correlate the responses of metal halide perovskites to various environmental stimuli with the dynamic behaviors of the [MX 6 ] $n$- octahedra. In this study, with the temperature-dependent single-crystal X ray diffraction (SCXRD) measurements on Cs 3 Bi 2 Br 9 2D halide perovskites, we can identify two classes of distortions through the lowering of temperature: intraoctahedral distortion, which is the off-centering of Bi 3+ cation within a [BiBr 6 ] 3– octahedron due to the Bi 3+ 6s 2 lone pair electrons, and interoctahedral distortion, which is the collective misalignments among the [BiBr 6 ] 3– building blocks. Free exciton (FE) and self-trapped exciton (STE) models are used to study the relationship between the distortion of octahedra in Cs 3 Bi 2 Br 9 and the corresponding changes in its optoelectronic properties, which transform from dominating blue emission above 100 K to red emission at 4 K. In conclusion, this work provides new insights into the excitonic behaviors of perovskites and suggests a possibility that we can design and rationalize the optical properties of halide perovskites by regulating the environmental stimuli based on the knowledge of behaviors of the individual [MX 6 ] $n$- building blocks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Hierarchically Porous Carbons with Highly Curved Surfaces for Hosting Single Metal FeN 4 Sites as Outstanding Oxygen Reduction Catalysts

Iron–nitrogen–carbon (Fe₋N₋C) materials have emerged as a promising alternative to platinum-group metals for catalyzing the oxygen reduction reaction (ORR) in proton-exchange-membrane fuel cells. However, their low intrinsic activity and stability are major impediments. Herein, an Fe₋N–C electrocatalyst with dense FeN 4 sites on hierarchically porous carbons with highly curved surfaces (denoted as FeN 4 - hc C) is reported. The FeN 4 - hc C catalyst displays exceptional ORR activity in acidic media, with a high half-wave potential of 0.85 V (versus reversible hydrogen electrode) in 0.5 m H 2 SO 4 . When integrated into a membrane electrode assembly, the corresponding cathode displays a high maximum peak power density of 0.592 W cm -2 and demonstrates operating durability over 30 000 cycles under harsh H 2 /air conditions, outperforming previously reported Fe–N₋C electrocatalysts. These experimental and theoretical studies suggest that the curved carbon support fine-tunes the local coordination environment, lowers the energies of the Fe d-band centers, and inhibits the adsorption of oxygenated species, which can enhance the ORR activity and stability. This work provides new insight into the carbon nanostructure–activity correlation for ORR catalysis. It also offers a new approach to designing advanced single-metal-site catalysts for energy-conversion applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Mechanical, corrosion, and wear properties of biomedical Ti–Zr–Nb–Ta–Mo high entropy alloys

The microstructures, mechanical, corrosion, and wear behaviors of the Ti x ZrNbTaMo (x = 0.5, 1, 1.5, and 2, molar ratio) high entropy alloys (HEAs) were studied in this work. It was found that the Ti–Zr–Nb–Ta–Mo HEAs showed a dendrite structure with two body-centered-cubic (BCC) solid solution phases. The Ti 0.5 ZrNbTaMo HEA exhibited a high hardness of about 500 HV, high compressive strength approaching 2,600 MPa, and large plastic strain of over 30%. Furthermore, the highly-protective oxide films formed on the surface of Ti–Zr–Nb–Ta–Mo HEAs in the phosphate buffer saline (PBS) solution, which resulted in the high corrosion resistance of the HEAs. The Ti–Zr–Nb–Ta–Mo HEAs exhibited the greater dry- and wet-wear resistance than that of the traditional biomedical Ti6Al4V alloy. The results also indicated that with the decrease in the Ti content, the wear resistance of the Ti–Zr–Nb–Ta–Mo HEAs in the PBS solution improved. Finally, the Ti 0.5 ZrNbTaMo alloy presented the highest corrosive wear resistance among the four HEAs owing to its combination of good mechanical properties and high chemical stability.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Measurement of f1(1285) production in pp collisions at $\sqrt{s}$ = 13 TeV

This study presents the first measurement of the f 1 (1285) resonance using the ALICE detector in inelastic proton–proton collisions at a center-of-mass energy of 13 TeV. The resonance is reconstructed at midrapidity (|y| < 0.5) through the hadronic decay channel f 1 (1285)→ K$^0_S$K ± π ± . Key measurements include the determination of its mass, transverse-momentum integrated yield, and average transverse momentum. Additionally, the ratio of the transverse-momentum integrated yield of f 1 (1285) to pion is compared with calculations from the canonical statistical hadronization model. The model calculation, assuming a zero total strangeness content for f 1 (1285), reproduces the data within 1σ deviation, shedding light on the quark composition of f 1 (1285).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order

Layered metal–organic frameworks are promising candidates for new two-dimensional magnets, as their synthetic programmability of these materials can provide a route to diverse structural and electronic properties. However, such framework materials typically lack the heavy elements that engender magnetocrystalline anisotropy in the monolayer ferromagnets reported to date. Alternative sources of magnetic anisotropy are therefore needed in these materials. Here, we report the synthesis of single crystals of the framework material (NMe 4 ) 2 [Fe 2 L 3 ] (H 2 L = 3,6-dichloro-2,5-dihydroxybenzoquinone) and evaluate the angular dependence of its magnetic properties. Oriented-crystal magnetization measurements reveal strong uniaxial anisotropy, where the easy axis is aligned with the crystallographic c axis. While the spin carriers of this structure are isotropic $S = ^5/_2$ Fe III metal centers and $S = ^1/_2$ organic linkers, the anisotropy energy of the framework material is comparable to that of reported 2D ferromagnets. Density functional theory calculations indicate that the observed magnetocrystalline anisotropy arises from ligand-to-metal charge transfer that enhances the magnetic anisotropy of the otherwise isotropic Fe centers, suggesting that metal–ligand covalency can be utilized as a general additive for the development of 2D magnets. These results in this study show the possibility for (NMe 4 ) 2 [Fe 2 L 3 ] to retain magnetic order down to the 2D monolayer limit. In addition, the combination of large magnetic anisotropy and semiconducting character in (NMe 4 ) 2 [Fe 2 L 3 ] highlights its potential as a new 2D magnetic semiconductor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Photochemical CO 2 Reduction by a Postsynthetically Modified Zr-MOF

Metal–organic frameworks are an excellent platform for photochemical CO 2 reduction into valuable chemicals. Herein, we report the synthesis and photocatalytic behavior of Ru@MOF-808, a Zr-based MOF, modified with a Ru-polypyridyl complex. The postsynthetic modification was achieved using solvent-assisted incorporation of bipyridine–carboxylate ligands onto the nodes of the MOF-808, followed by the coordination of Ru(II)-terpyridine moiety. A thorough characterization including 1 H NMR, diffuse reflectance UV/vis, X-ray absorption spectroscopy and gas adsorption studies, combined with DFT calculations, provides strong support for efficient incorporation of the molecular Ru-complex at the loading of one Ru center per node. In the presence of a strong sacrificial reductant BIH, Ru@MOF-808 was found to catalyze the photochemical reduction of CO 2 into a mixture of CO and formate ion. When compared to the homogeneous model catalyst Ru(tpy)(bpy) 2+ , Ru@MOF-808 was found to exhibit higher formate yields. Additionally, to explain these formate enhancements, we propose a mechanism that involves CO 2 capture at the MOF nodes to form Zr-bicarbonate species, which further react in a hydride transfer reaction with photogenerated Ru–H donor, thereby outperforming molecular catalysts in HCOO – production. Overall, the results presented in this work indicate the potential of Zr-based MOFs in integrating CO 2 capture with its photochemical conversion to desired products.

CO2 reduction↗

DOE OSTI2020

Metal–Organic Framework-Based Microfluidic Impedance Sensor Platform for Ultrasensitive Detection of Perfluorooctanesulfonate

The growing global concerns to public health from human exposure to perfluorooctanesulfonate (PFOS) requires rapid, sensitive, in-situ detection where current, state-of-the-art techniques are yet to adequately meet sensitivity and selectivity standards of the real-world. This work presents, for the first time, a synergistic approach for the targeted affinity-based capture of PFOS using a porous sorbent probe that enhances detection sensitivity by embedding it on a microfluidic conductive platform. This novel sorbent-containing platform functions as an electrochemical sensor to directly measure PFOS concentration through a proportional change in electrical response (increase in impedance). The extremely high surface area and pore volume of mesoporous metal-organic framework (MOF) Cr-MIL-101 is used as the probe for targeted PFOS capture based on the affinity of the chromium center towards both the fluorine tail groups as well as the sulfonate functionalities as demonstrated by spectroscopic (NMR and XPS) and microscopic (TEM) studies. Answering the need for an ultrasensitive PFOS detection technique, we are embedding these MOF capture probes inside a microfluidic channel, sandwiched between interdigitated microelectrodes (IDµE). The nanoporous geometry increases the signal to noise ratio of interdigitated microelectrodes tremendously increasing sensitivity; this in combination with the ability of the capture probes to interact with the PFOS at the molecular level and effectively transduce that response electrochemically has allowed us achieve a PFOS detection limit of 0.5 ng/L, which is unprecedented for in-situ analytical PFOS sensors and even comparable to quantification limits achieved using state-of-the-art ex situ techniques.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Actinide Elemental Ratios of Spent Nuclear Fuel Samples by Resonance Ionization Mass Spectrometry

While resonance ionization mass spectrometry (RIMS) has demonstrated utility in measuring isotopic compositions of elements in complex matrices without the need for chemical separation to remove isobaric interferences, it has had limited application in measuring elemental compositions. The ability to determine elemental compositions via an in situ method like RIMS would be an exceptional asset in spent nuclear fuel analysis, where they are important in assessing reactor histories and whose chemical separation presents a radiological hazard. However, quantitative elemental analysis by RIMS requires special considerations because each element is ionized by its own set of lasers tuned to element specific resonant ionization wavelengths. We present the first comprehensive study of measuring elemental ratios by RIMS in spent nuclear fuel. All actinides produced by neutron capture are enhanced significantly radially from the center to the edge of a fuel pellet. This edge effect is not readily accessible by conventional bulk measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Cubic double perovskites host noncoplanar spin textures

Magnetic materials with noncoplanar magnetic structures can show unusual physical properties driven by nontrivial topology. Topologically-active states are often multi-q structures, which are challenging to stabilize in models and to identify in materials. Here, we use inelastic neutron-scattering experiments to show that the insulating double perovskites Ba 2 YRuO 6 and Ba 2 LuRuO 6 host a noncoplanar 3-q structure on the face-centered cubic lattice. Quantitative analysis of our neutron-scattering data reveals that these 3-q states are stabilized by biquadratic interactions. Our study identifies double perovskites as a highly promising class of materials to realize topological magnetism, elucidates the stabilization mechanism of the 3-q state in these materials, and establishes neutron spectroscopy on powder samples as a valuable technique to distinguish multi-q from single-q states, facilitating the discovery of topologically-nontrivial magnetic materials.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Model-independent determination of the strong-phase difference between D 0 and D ¯ 0 → π + π − π + π − decays

Measurements of the strong-phase difference between D 0 and D ¯ 0 → π + π − π + π − are performed in bins of phase space. The study exploits a sample of quantum-correlated D D ¯ mesons collected by the BESIII experiment in e + e − collisions at a center-of-mass energy of 3.773 GeV, corresponding to an integrated luminosity of 2.93 fb − 1 . Here, D denotes a neutral charm meson in a superposition of flavor eigenstates. The reported results are valuable for measurements of the C P -violating phase γ (also denoted ϕ 3 ) in B ± → D K ± , D → π + π − π + π − decays, and the binning schemes are designed to provide good statistical sensitivity to this parameter. The expected uncertainty on γ arising from the precision of the strong-phase measurements, when applied to very large samples of B -meson decays, is around 1.5° or 2°, depending on the binning scheme. The binned strong-phase parameters are combined to give a value of F + 4 π = 0.746 ± 0.010 ± 0.004 for the C P -even fraction of D 0 → π + π − π + π − decays, which is around 30% more precise than the previous best measurement of this quantity. Published by the American Physical Society 2024

Ablikim, M.↗

DOE OSTI2026

What Shapes Transportation Charging Infrastructure Availability? Evidence from Tennessee

This study examines how community, travel, and freight characteristics relate to public charging infrastructure availability across Tennessee ZIP codes. We link Alternative Fuels Data Center station locations with traffic, socioeconomic, demographic, commuting, and freight employment data to build a ZIP code-level dataset. Ordinary least squares regression captures variation in chargers per 10,000 residents (R2=0.311). Quantile regressions at the 25th, 50th, and 75th percentiles, with pseudo R2 values up to 0.099, show that the determinants of infrastructure availability differ across low-, medium-, and high-availability areas. Percent female, percent car commuters, average household size, and median age are negatively associated with charging availability across much of the distribution. Truck traffic is positively associated only in lower-availability ZIP codes, while vehicle miles traveled shifts from a negative association at the lower end of the distribution to a positive association at the upper end. The results provide insight into how public charging deployment aligns with community characteristics, mobility demand, and freight activity across Tennessee. Future work can distinguish charger types and power levels, incorporate land-use and temporal rollout patterns, and examine how charging infrastructure needs differ across urban and rural contexts.

Calderón, Oriana [University of Tennessee, Knoxvil↗

DOE OSTI2022

COVID-19 Exposure Assessment Tool (CEAT): Exposure quantification based on ventilation, infection prevalence, group characteristics, and behavior

The coronavirus disease 2019 (COVID-19) Exposure Assessment Tool (CEAT) allows users to compare respiratory relative risk to severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) for various scenarios, providing understanding of how combinations of protective measures affect risk. CEAT incorporates mechanistic, stochastic, and epidemiological factors including the (i) emission rate of virus, (ii) viral aerosol degradation and removal, (iii) duration of activity/exposure, (iv) inhalation rates, (v) ventilation rates (indoors/outdoors), (vi) volume of indoor space, (vii) filtration, (viii) mask use and effectiveness, (ix) distance between people (taking into account both near-field and far-field effects of proximity), (x) group size, (xi) current infection rates by variant, (xii) prevalence of infection and immunity in the community, (xiii) vaccination rates, and (xiv) implementation of COVID-19 testing procedures. CEAT applied to published studies of COVID-19 transmission events demonstrates the model’s accuracy. We also show how health and safety professionals at NASA Ames Research Center used CEAT to manage potential risks posed by SARS-CoV-2 exposures.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Performance trade-offs in reconfigurable networks for HPC

Designing efficient interconnects to support high-bandwidth and low-latency communication is critical toward realizing high performance computing (HPC) and data center (DC) systems in the exascale era. At extreme computing scales, providing the requisite bandwidth through overprovisioning becomes impractical. These challenges have motivated studies exploring reconfigurable network architectures that can adapt to traffic patterns at runtime using optical circuit switching. Despite the plethora of proposed architectures, surprisingly little is known about the relative performances and trade-offs among different reconfigurable network designs. We aim to bridge this gap by tackling two key issues in reconfigurable network design. First, we study how cost, power consumption, network performance, and scalability vary based on optical circuit switch (OCS) placement in the physical topology. Specifically, we consider two classes of reconfigurable architectures: one that places OCSs between top-of-rack (ToR) switches—ToR-reconfigurable networks (TRNs)—and one that places OCSs between pods of racks—pod-reconfigurable networks (PRNs). Second, we tackle the effects of reconfiguration frequency on network performance. Our results, based on network simulations driven by real HPC and DC workloads, show that while TRNs are optimized for low fan-out communication patterns, they are less suited for carrying high fan-out workloads. PRNs exhibit better overall trade-off, capable of performing comparably to a fully non-blocking fat tree for low fan-out workloads, and significantly outperform TRNs for high fan-out communication patterns.

Teh, Min Yee↗

DOE OSTI2020

Characterization Strategy of a Limited Number of Radioactive Waste Effluent Tanks in View of Decommissioning a Large Number of Tanks - 20286

In order to organize the D and D of the former effluent treatment facility at the CEA Cadarache Center (France), the key data to gather through the facility characterization are the following:: volumes and masses, liquid/solid distribution and specific activity. By studying the treatment processes and the history of the facility, families of tanks have been defined and a reference tank chosen for investigation in each family. The intrusive investigations (video, residue thickness, dose rate..), the gamma spectrometry measurements carried out on site on the residue samples and radiochemical results collected in laboratories, led us to conclude that there was a relative radiological homogeneity (for specific activity and Am-241/Cs-137 ratio) within each tank. The next step consisted in extrapolating the specific activity evaluated for the reference tanks, to the other tanks of each family by using data such as geometry, dose rate or the function of the tanks within the process. Thus, a cartography of the 130 tanks of the facility is available. Finally, the conclusions drawn from the radiological homogeneity of the tanks and their affiliation to homogeneous, well-identified tank clusters lead to a simple and efficient operational approach for the D and D of the 130 tanks of the facility. Indeed, because of the residue characteristics (homogeneous activity and strong differentiation of Cs/Am ratio), a sample collected when opening the tank, and measured on site by gamma spectrometry will allow us to validate the operational design and the emptying techniques defined during the D and D study phase thanks to the characterization of a limited number of reference tanks. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Translation of "Contribution a l'etude du diagramme pression-temperature du beryllium pur" (Contribution to the Study of the Pressure-Temperature Diagram of Pure Beryllium)

An unusual feature of beryllium’s phase diagram is the transition from a hexagonal close packed (hcp, or α) to a body-centered cubic (bcc, or β) structure ~20 K below the normal melting temperature of T melt ≈ 1560 K. An early thermal analysis of 99.7% pure Be found two arrests1 : one at 1533-1536 K and another at 1551-1557 K. Without ruling out an allotropic transformation in Be itself, Sloman attributed the first of these to solidification of a Be-BeO eutectic. Losano observed only the higher of the two in 99.962% Be, seeming to confirm the notion that the lower feature was an artifact of impurity. Teitel (99.4%) also measured two arrests and attributed the lower to impurity, but questioned whether oxygen was the culprit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

The S-PLUS Fifth Data Release: Over 4500 Square Degrees of the Southern Sky and a Multicolor View of the Hydra and Antlia Galaxy Clusters

Abstract We present the fifth data release (DR5) of the Southern Photometric Local Universe Survey (S-PLUS), covering 4592 deg 2 across 2491 fields. Observations were conducted with the T80-South, a Brazilian robotic telescope equipped with the Javalambre 12-filter system, containing five broadband and seven narrowband filters. Data products feature FITS images and extensive catalogs containing fluxes, magnitudes, and shape parameters for over 113 million detections. In addition, several value-added catalogs are provided, offering photometric redshifts (photo- zs ), object classifications, masks, and extinction coefficients. For the first time, this release includes coverage of 110 deg 2 along the Galactic disk, facilitating new research into Galactic structure and stellar populations. The release also provides full coverage of the Hydra Supercluster and numerous other nearby clusters with improved data reduction and calibration, enhancing photo- z accuracy, which is vital for large-scale structure studies. A preliminary analysis of the Hydra and Antlia galaxy clusters up to 5 × R 200 yields an updated catalog of 1706 cluster members based on both spectroscopic and high-quality photo- zs . Our photometric data shows that both clusters have a similar proportion of galaxies with an H α excess relative to their clustercentric distance, though Hydra has a higher fraction near its center. Additionally, the spatial distribution of all objects in our sample highlights a bridge connecting both clusters. We verify that S-PLUS DR5 provides a solid foundation for future scientific investigations, ranging from solar system studies to cosmology.

Vinicius Rodrigues de Lima, Erik [Universidade de ↗

DOE OSTI2025

Isolation of Inner-Sphere Aquo Complexes of Samarium(II)

The cis-anti-cis and cis-syn-cis isomers of [Sm(dicyclohexano-18-crown-6)(H 2 O) 2 ]I 2 exhibiting trans water molecules bound to the Sm 2+ ion have been isolated and characterized. Sm 2+ possesses an electrochemical potential sufficient for water reduction, and thus these complexes add to the recent body of evidence that the oxidation of Sm 2+ by water can operate by a mechanism that is not straightforward. These complexes are obtained by the direct addition of stoichiometric amounts of water to solutions of the respective Sm(dicyclohexano-18-crown-6)I 2 isomers under an inert atmosphere. The parent complex, Sm(dicyclohexano-18-crown-6)I 2 , lacking coordinating water molecules can be obtained through rigorous exclusion of water. It was determined that the bulky cyclohexano-substituents deter intramolecular interactions between [Sm(dicyclohexano-18-crown-6)(H 2 O) 2 ]I 2 complexes and slow the oxidization of the metal centers. The extent of the stability of these complexes to the presence of water has been further probed through cyclic voltammetry, where it was found that the redox potential of both isomers of [Sm(dicyclohexano-18-crown-6)(H 2 O) 2 ]I 2 maintains quasi-reversible behavior with a 50,000-fold excess of water to Sm 2+ in solution with the cis-syn-cis complex being quasi-reversible at even higher concentrations of water. Solution-phase spectroscopy of these complexes in acetonitrile shows a corresponding hypsochromic shift of the Sm 2+ 4f → 5d transition typically observed in the visible region from Sm 2+ complexes. Here, the crystalline compounds obtained in this study support solid-state spectroscopic trends observed from other Sm 2+ crown-ether complexes containing iodide counterions, wherein the proximity of the iodide ions to the metal center determines whether the complex can exhibit 4f → 4f photoluminescence.

Crystals↗

DOE OSTI2023

Structural and Biophysical Properties of a [4Fe-4S] Ferredoxin-Like Protein from Synechocystis sp. PCC 6803 with a Unique Two Domain Structure

Electron carrier proteins (ECPs), binding iron-sulfur clusters, are vital components within the intricate network of metabolic and photosynthetic reactions. They play a crucial role in the distribution of reducing equivalents. In Synechocystis sp. PCC 6803, the ECP network includes at least nine ferredoxins. Previous research, including global expression analyses and protein binding studies, has offered initial insights into the functional roles of individual ferredoxins within this network. This study primarily focuses on Ferredoxin 9 (slr2059). Through sequence analysis and computational modeling, Ferredoxin 9 emerges as a unique ECP with a distinctive two-domain architecture. It consists of a C-terminal iron-sulfur binding domain and an N-terminal domain with homology to Nil-domain proteins, connected by a structurally rigid 4-amino acid linker. Notably, in contrast to canonical [2Fe-2S] ferredoxins exemplified by PetF (ssl0020), which feature highly acidic surfaces facilitating electron transfer with photosystem I reaction centers, models of Ferredoxin 9 reveal a more neutral to basic protein surface. Using a combination of electron paramagnetic resonance spectroscopy and square-wave voltammetry on heterologously produced Ferredoxin 9, this study demonstrates that the protein coordinates 2x[4Fe-4S]2+/1+ redox-active and magnetically interacting clusters, with measured redox potentials of -420 +/- 9 mV and -516 +/- 10 mV vs SHE. A more in-depth analysis of Fdx9's unique structure and protein sequence suggests that this type of Nil-2[4Fe-4S] multi-domain ferredoxin is well conserved in cyanobacteria, bearing structural similarities to proteins involved in homocysteine synthesis in methanogens.

cyanobacteria↗