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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Anion Binding by Macrocyclic Receptors: Computational Landscape of 1:1 and 2:1 Stoichiometries

Macrocyclic receptors play a crucial role in supramolecular chemistry, enabling the selective binding of guest molecules through non-covalent interactions. This study investigates the anion binding properties of three shape-persistent macrocycles, triazolophane, cyanostar, and tricarb, each featuring preorganized cavities with polarized CH hydrogen bond donors. In the 1:1 binding stoichiometries, the macrocycles preferentially bind anions that fit inside their two-dimensional cavities, with this preference being more pronounced in solution. Specifically, the triazolophane favors smaller anions like chloride and bromide, while the larger cavities offered by cyanostar and tricarb macrocycles preferentially bind the larger iodide. For large, polyatomic anions (SCN − , BF$^{−}_{4}$, ClO$^{−}_{4}$, and PF$^{−}_{6}$), the macrocycles self-assemble to form stable 2:1 sandwich complexes, exhibiting stronger binding. This shift in selectivity highlights the versatility of the macrocycles, making them promising candidates for anion sensing and regulation with various complexation stoichiometries.

Che, Minwei [Indiana University, Bloomington, IN (↗
DOE OSTI2025

Direct deflection of Millicharged radiation

Millicharged particles are generic in theories of dark sectors. A cosmic or local abundance of them may be produced by the early universe, stellar environments, or the decay or annihilation of dark matter/dark energy. Furthermore, if such particles are light, these production channels result in a background of millicharged radiation. We show that light-shining-through-wall experiments employing superconducting RF cavities can also be used as “direct deflection” experiments to search for this relativistic background. The millicharged plasma is first subjected to an oscillating electromagnetic field of a driven cavity, which causes charge separation in the form of charge and current perturbations. In turn, these perturbations can propagate outwards and resonantly excite electromagnetic fields in a well-shielded cavity placed nearby, enabling detection. We estimate that future versions of the existing Dark SRF experiment can probe orders of magnitude of currently unexplored parameter space, including millicharges produced from the Sun, the cosmic neutrino background, or other mechanisms that generate a thermal abundance with energy density as small as ~ 10$^{−4}$ that of the cosmic microwave background.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

First results of the CAST-RADES haloscope search for axions at 34.67 μ eV

We present results of the Relic Axion Dark-Matter Exploratory Setup (RADES), a detector which is part of the CERN Axion Solar Telescope (CAST), searching for axion dark matter in the 34.67 μeV mass range. A radio frequency cavity consisting of 5 sub-cavities coupled by inductive irises took physics data inside the CAST dipole magnet for the first time using this filter-like haloscope geometry. An exclusion limit with a 95% credibility level on the axion-photon coupling constant of g aγ ≳ 4 × 10 -13 GeV -1 over a mass range of 34.6738 μeV < m a < 34.6771 μeV is set. This constitutes a significant improvement over the current strongest limit set by CAST at this mass and is at the same time one of the most sensitive direct searches for an axion dark matter candidate above the mass of 25 μeV. The results also demonstrate the feasibility of exploring a wider mass range around the value probed by CAST-RADES in this work using similar coherent resonant cavities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Creep deformation and cavitation in an additively manufactured Al-8.6Cu-0.4Mn-0.9Zr (wt%) alloy

Creep deformation and cavitation were investigated at 300 ºC in both tension and compression for an additively manufactured Al-8.6Cu-0.5Mn-0.9Zr (wt%) alloy in the as-fabricated state and after various aging treatments (aging at 300 °C/200 h or 350 °C/24 h and overaging at 400 °C/200 h). Creep mechanisms at 300 °C were determined by relating the measured creep response to corresponding microstructural and X-ray computed tomography observations. In compression, alloys in the as-fabricated and two aging conditions exhibited similarly high creep resistance. Overaging (400 °C/200 h) led to substantial coarsening of intragranular θ-Al2Cu precipitates and an expected drop in their Orowan strengthening contribution. In tension, minimum strain rates comparable to those in compression were obtained at any given stress; however, upon accumulation of some plastic strain in the matrix, creep cavities started to form, leading to accelerated tertiary stage creep deformation and rupture. Cavitation occurred exclusively along melt pool boundaries due to locally enhanced diffusion enabled by (i) large grain-boundary area in adjacent fine-grained zones and (ii) localization of creep strain in nearby heat-affected zones. Although cavity growth was initially diffusion-controlled, its rate was determined by matrix creep rate, consistent with constrained cavity growth mechanisms. This study reveals how microstructural complexities induced by the additive manufacturing process affect the creep and cavitation behavior of Al-Cu-Mn-Zr alloys. The underlying creep and cavitation mechanisms uncovered in this study point to pathways that improve the high-temperature properties of additively manufactured alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Enhanced flow boiling heat transfer on chromium coated zircaloy-4 using cold spray technique for accident tolerant fuel (ATF) materials

Flow boiling heat transfer tests were conducted to evaluate the Critical Heat Flux (CHF) and Heat Transfer Coefficient (HTC) of conventional and accident tolerant fuel (ATF) cladding materials, i.e., bare Zircaloy-4 (Zr4), and Zircaloy-4 coated with Chromium using physical vapor deposition (PVD) (Zr4-Cr-PVD) and cold spray process (Zr4-Cr-CS), respectively. The tests were performed on a single heater rod with a uniform heat flux profile, at the atmospheric pressure, inlet temperature (24 °C) and mass flow rate (750 kg/m 2 s). HTC’s were increased by 5.2% and 3.3% on Zr4-Cr-CS compared to bare Zr4 and Zr4-Cr-PVD. Improved HTCwas attributed to the increased void fraction and high roughness (Ra = 532 nm) of the Zr4-Cr-CS. In detail, the micro-cavities, which act as bubble seeds, were entirely distributed on the Zr4-Cr-CS, and these micro-cavities generated smaller and faster bubbles, thus the void fraction increased by 10.9% compared to bare Zr4. HTC is improved by these smaller and faster bubbles which can remove heat from the heater rod surface more efficiently. To identify the exact location of CHF, the surface temperature profile was measured using advanced fiber-optic sensors which have high temporal/spatial resolution (distance between point to point: ~2.5 mm, frequency ~100 Hz). CHF occurred at 80–95% along the heated length and showed an 11.6% reduction on Zr4-Cr-CS compared to bare Zr4. We hypothesize the CHF reduction was caused by the lower wettability of the Zr4-Cr-CS which reduces the liquid supply to the surface, and vigorous bubble accumulation owing to high void fraction near the outlet, which results in early formation of the vapor film. During the post-CHF quenching phase, the rougher Zr4-Cr-CS showed larger cooling rates compared to the bare Zr4 and Zr4-Cr-PVD, preventing of oxidation by chromium layer. In conclusion, we demonstrate that the high roughness on the Zr4-Cr-CS increased the number of micro-cavities on the surface, resulting in 5.2% increase in HTC and improvement in the quenching heat transfer performance whereas CHF was 11.6% reduced compared to bare Zr4. Overall statistically there is little effect in the coating with regards to CHF and slight improvement in HTC.

42 ENGINEERING↗
DOE OSTI2021

Three influential factors on colloidal nanoparticle deposition for heat conduction enhancement in 3D chip stacks

Thermal management is one of the major challenges facing the development of three-dimensional (3D) chip stacks. Recently, experimental studies have shown that neck-based thermal structure (NTS) between chip layers formed by drying of colloidal suspension in cavity filled with micro-size particles can improve the vertical heat conduction threefold. However, a deep understanding of the mechanisms of neck formation and its influence on heat conduction is still lacking. In this paper, we numerically study the effects of three parameters, i.e., initial nanoparticle concentration, drying temperature and chip surface wettability on neck formation between filler particles and on the resulting heat conduction of the NTS. With increasing nanoparticle concentration, the size and number of necks increase, resulting in an increased effective thermal conductivity (ETC) of NTS. The drying temperature is found to have only little influence on the ETC of resultant NTS, while the neck size and spatial distribution become more uniform at higher drying temperature. When reducing the wettability of the top and bottom surfaces of the cavity, the necks shrink in size until completing evacuating at the top and bottom layers, while the size of the necks between filler particles in the middle height of the cavity expands slowly. In consequence, the ETC of NTS drops at an increasing rate. Being able to reveal the underlying multiple mechanisms of two-phase flow, phase change and heat transport, the current numerical study suggests optimal values for the deposition process, with initial nanoparticle concentration over 0.8%, a drying temperature of 60°C and a uniform contact angle of 30° for practical production of NTS.

3D chip stacks↗
DOE OSTI2020

Revealing the synergistic effects of sequential and simultaneous dual beam irradiations in tungsten via in-situ TEM

Elucidating the synergistic effects of different energetic beams on the radiation response of nuclear materials is critical for developing an improved methodology for their evaluation when exposed to extreme environments. This article describes in-situ sequential (He implantation followed by Kr irradiation and vice-versa) and simultaneous (heavy ion Kr irradiation and He implantation) dual beam irradiations performed on tungsten at 1223 K. Dislocation loop density, average area, and total loop damage as a function of irradiation history and dose/fluence are quantified. The loop Burgers vectors and cavity damage (cavity density, size and total change in volume) are also determined at the final maximum dose for each condition. The loop damage evolution was different in all cases, with the smallest loop damage observed in the simultaneous experiment. Annihilation of Kr generated dislocation loops during He implantation in the Kr + He experiment was an unanticipated observation that may be explained by the dynamic evolution of dislocation loop sink strengths and time-dependent defect fluxes. Dislocation loop raft formation, denuded zones near extended defects, and cavity damage are compared across the different conditions. The phenomena observed and discussed in this work will stimulate further experimental and computational modeling activities leading to improved fundamental understanding of the irradiation response of nuclear materials under reactor-similar environments.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Microstructural characterization of cold-worked 316 stainless steel flux thimble tubes irradiated up to 100 dpa in a commercial Pressurized Water Reactor

Two flux thimble tubes (FTT) made of 15% cold-worked 316 stainless steel (SS) were harvested from Ringhals Pressurized Water Reactor (PWR) Unit 2, with peak damages of 76 and 100 displacements per atom (dpa) after 29 and 34 years’ service, respectively. Specimens sectioned from parent tubes were comprehensively characterized with nominal damage levels of ~0, ~41, ~74, 76, and 100 dpa at a nominal temperature range of 285-323 °C. Both FTTs contained helium and hydrogen gases as transmutation products. The helium follows a production rate of ~9.8 appm/dpa, while environmental factors complicate hydrogen production obscuring an exact H/dpa ratio. Irradiation-induced dislocation loops, nano-cavities, solute clusters, and microsegregation were all observed. The dislocation loops and nano-cavities indicated saturation at 41 dpa. The solute clusters continued to evolve with Ni-Si clusters formed at 41 dpa, and Ni-Si-Mn-P clusters formed at 74 and 100 dpa, but neither clusters exhibited distinct diffraction patterns at any damage levels. Solute clusters were observed to frequently be co-located with dislocation loops, but fully decorated loops were rarely detected. Significant radiation-induced segregation (RIS) was observed around grain boundaries at all damage levels. The modified inverse Kirkendall (MIK) model captured the RIS behavior of major elements. Large cavities within or around an Mn-S rich region were observed for the first time. Through all the damage levels, void swelling is always below 0.05%, making significant dimensional change unlikely in core internals when used at similar conditions. Meanwhile, the role of overwhelming nanocavities, presumably helium bubbles, should be considered in other potential degradation mechanisms, including irradiation-assisted stress corrosion cracking, embrittlement, and loss of fracture toughness, which remain the concerns for extended operation of nuclear power plants.

Post Irradiation Examination, Isotope Dilution Mas↗
DOE OSTI2021

Effects of helium on irradiation response of reduced-activation ferritic-martensitic steels: Using nickel isotopes to simulate fusion neutron response

Understanding the effects of helium on microstructures and mechanical properties of reduced-activation ferritic-martensitic steels is important to use of these steels in fusion reactor structures. The 9Cr-2WVTa steels were doped with 58Ni and 60Ni isotopes at 2 weight percent to control the rate of transmutation helium generation. The samples were irradiated in the High Flux Isotope Reactor to ~24 displacements per atom at nominal temperatures of 300, 400, and 500°C, producing 228 and 7 atomic parts-per-million helium in the 58 Ni- and 60 Ni-doped samples, respectively. Transmission electron microscopy revealed a variety of precipitates and the radiation-induced dislocation loops and cavities (voids or helium bubbles). Tensile tests of the irradiated samples at the irradiation temperatures showed radiation-induced hardening at 300°C and radiation-induced softening at 400°C. Analysis indicates that the hardening primarily originated from the loops and cavities. The 58 Ni-doped samples had greater strengthening contributions from loops and cavities, leading to higher hardening with lower ductility than the 60 Ni-doped samples. The greater helium production of 58 Ni did not show pronounced reductions in ductility of the samples.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Reduced order modeling of a fluidized bed particle receiver for concentrating solar power with thermal energy storage

Oxide particles can serve as both the heat transfer and thermal energy storage (TES) media for next-generation concentrating solar power (CSP) plants where high-temperature TES enables dispatchable electricity from efficient power cycles with firing temperatures above 600 °C. Transferring heat to flowing particles at such high temperatures in a MW-scale central tower receiver remains a challenge for the CSP community. For indirect receivers with external walls to contain the particles, maintaining wall temperatures below the limits of structural metal alloys requires high heat transfer coefficients between the wall and the moving particle stream. Bubbling fluidization of downward-flowing particles can sustain high bed-wall heat transfer coefficients (> 1000 W m -2 K -1 ). Using experimentally calibrated correlations for bed-wall heat transfer and vertical particle dispersion, this study implements an axially discretized zonal model of a counterflow fluidized bed receiver to explore how bubbling fluidization may enable indirect cavity particle receivers. High bed-wall heat transfer coefficients support solar fluxes on angled cavity walls > 200 kW m -2 at peak aperture fluxes of 980 kW m -2 while maintaining external wall temperatures < 950 °C. Lateral particle dispersion enables hotter particles near the receiver leading edge to mix with cooler particles further from the leading edge to lower maximum external wall temperatures. Parametric studies identify how mass fluxes, particle dispersion, and solar concentrations impact indirect receiver thermal efficiency and uniformity for a CSP plant. These studies provide a basis for the design of indirect fluidized-bed cavity receivers that can maintain particle outlet temperatures for TES above 750 °C.

14 SOLAR ENERGY↗
DOE OSTI2024

Kelvin-Helmholtz instability as one of the key features for fast and efficient emulsification by hydrodynamic cavitation

The paper investigates the oil–water emulsification process inside a micro-venturi channel. More specifically, the possible influence of Kelvin-Helmholtz instability on the emulsification process. High-speed visualizations were conducted inside a square venturi constriction with throat dimensions of 450 µm by 450 µm, both under visible light and X-Rays. We show that cavity shedding caused by the instability results in the formation of several cavity vortices. Their rotation causes the deformation of the oil stream into a distinct wave-like shape, combined with fragmentation into larger drops due to cavitation bubble collapse. Later on, the cavity collapse further disperses the larger drops into a finer emulsion. Thus, it turns out that the Kelvin-Helmholtz instability is similarly characteristic for hydrodynamic cavitation emulsification inside a microchannel as is the Rayleigh-Taylor instability for acoustically driven emulsion formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Polariton Formation from Soret Band Excitons in Metal–Organic Frameworks and Plasmonic Lattices

This Letter describes strong coupling between a plasmonic nanoparticle (NP) lattice cavity and Soret excitons in a metal–organic framework (MOF) film. In optical transmission measurements, we observed a lower polariton mode that can be spectrally tuned by infiltrating MOF pores with solvents of different refractive index. Using transient absorption spectroscopy, both the lower and upper polariton modes can be resolved, with an estimated Rabi splitting of ~300 meV, nearly twice that of other plasmonic cavity–organic emitter systems. The polariton modes decay more rapidly than that of the uncoupled exciton. Furthermore, this hybrid system highlights the advantages of open plasmonic cavities for tunable coupling and the use of transient absorption spectroscopy to identify polariton modes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Efficient Intermolecular Charge Transport in π-Stacked Pyridinium Dimers Using Cucurbit[8]uril Supramolecular Complexes

Intermolecular charge transport through π-conjugated molecules plays an essential role in biochemical redox processes and energy storage applications. In this work, we observe highly efficient intermolecular charge transport upon dimerization of pyridinium molecules in the cavity of a synthetic host (cucurbit[8]uril, CB[8]). Stable, homoternary complexes are formed between pyridinium molecules and CB[8] with high binding affinity, resulting in an offset stacked geometry of two pyridiniums inside the host cavity. The charge transport properties of free and dimerized pyridiniums are characterized using a scanning tunneling microscope-break junction (STM-BJ) technique. Our results show that π-stacked pyridinium dimers exhibit comparable molecular conductance to isolated, single pyridinium molecules, despite a longer transport pathway and a switch from intra- to intermolecular charge transport. Control experiments using a CB[8] homologue (cucurbit[7]uril, CB[7]) show that the synthetic host primarily serves to facilitate dimer formation and plays a minimal role on molecular conductance. Molecular modeling using density functional theory (DFT) reveals that pyridinium molecules are planarized upon dimerization inside the host cavity, which facilitates charge transport. In addition, the π-stacked pyridinium dimers possess large intermolecular LUMO–LUMO couplings, leading to enhanced intermolecular charge transport. Altogether, this work demonstrates that supramolecular assembly can be used to control intermolecular charge transport in π-stacked molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Bathymetric Influences on Antarctic Ice-Shelf Melt Rates

Ocean bathymetry exerts a strong control on ice sheet-ocean interactions within Antarctic ice-shelf cavities, where it can limit the access of warm, dense water at depth to the underside of floating ice shelves. However, ocean bathymetry is challenging to measure within or close to ice-shelf cavities. It remains unclear how uncertainty in existing bathymetry datasets affect simulated sub-ice-shelf melt rates. In this work, we infer linear sensitivities of ice-shelf melt rates to bathymetric shape with grid-scale detail by means of the adjoint of an ocean general circulation model. Both idealized and realistic-geometry experiments of sub-ice-shelf cavities in West Antarctica reveal that bathymetry has a strong impact on melt in localized regions such as topographic obstacles to flow. Moreover, response of melt to bathymetric perturbation is found to be non-monotonic, with deepening leading to either increased or decreased melt depending on location. Our computational approach provides a comprehensive way of identifying regions, where refined knowledge of bathymetry is most impactful, and also where bathymetric errors have relatively little effect on modeled ice sheet-ocean interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Ocean Variability Beneath the Filchner-Ronne Ice Shelf Inferred From Basal Melt Rate Time Series

Fourteen phase-sensitive radars (ApRES) were deployed on the Filchner-Ronne Ice Shelf (FRIS) to measure variability in its basal melt rate. Melt rates from sites along the Ronne Depression vary seasonally, consistent with the dynamics of the propagation of seasonal dense water from the western ice front into the cavity. Several sites at the back of the FRIS cavity feature a signal with two seasonal maxima. Sub-ice shelf oceanographic data available from one of the sites indicate that this signal is caused by two different pathways followed by the same source water. Inter-annual variability is strongest along a direct flow pathway between western Ronne Ice Front and western Berkner Island. Highest melting occurred in 1999 and 2018, following anomalously low summer sea-ice concentrations in front of the ice shelf. Inter-annual melt rate variability at the back of the FRIS cavity is limited. If present, it is expressed as a suppression or delay in the arrival of the seasonal melt rate minimum, which can be understood in terms of inter-annual stratification changes and variable inflow pathways toward the sites. Long term mean ApRES melt rates agree with estimates from satellite data over eastern FRIS. However, the satellite estimates overstate the area of active basal freezing in the western part of the ice shelf. Furthermore, the temporal melt rate variability from the satellite estimates exaggerates the range of variability at both seasonal and inter-annual time scales with any correspondence between the in-situ and remotely derived inter-annual variability being limited to a single site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Particle‐In‐Cell Simulations of Starfish Prime

The Starfish Prime high altitude nuclear test created a transient diamagnetic cavity in the Earth's magnetic field above Johnston Island and launched an electromagnetic pulse (EMP) that was detected around the globe. For this work, we use the ion‐kinetic particle‐in‐cell code Topanga to simulate diamagnetic cavity evolution and the E3 EMP signal for Starfish Prime out to over a minute of physical time. The simulation domain has a longitudinal and latitudinal extent of 60° X 60° and a vertical extent of 2,000 km from the surface of the Earth. We compare our simulated results to magnetometer measurements taken in space and on the ground, finding good agreement in both cases. The diamagnetic cavity in the simulation forms in about a second, while the associated debris flux tube takes approximately 30 s to decay. The debris flux tube undergoes significant motion during this timeframe, rising upward. The measured E3 EMP signal on the ground consists of several components, all of which are present in our simulations. We discuss the physical origin of these components in relation to E3a (blast) and E3b (heave).

Belyaev, Mikhail A. [Lawrence Livermore National L↗
DOE OSTI2025

The Nature of Standing Plasma Waves Following Fast Breakdown in Thunderstorms

Narrow bipolar events (NBEs) are produced by large-scale systems of streamer corona discharges that occur inside thunderstorms and radiate intensely at very-high frequencies. Here we examine 14 high-power NBEs recorded in Florida which are followed by a lasting oscillatory signal. We isolate the dominant frequencies of the oscillations using empirical mode decomposition methods, and cross-reference this information with the radiator size inferred from broadband interferometry. We conclude that the oscillations are evidence of a standing electromagnetic wave in the plasma cavity created by the preceding streamer system, that is, the cavity's fundamental mode with wavelength equal to twice the radiator length. Contrasting the dispersive and attenuation properties of these waves across several different events allows us to conclude that the cavity is filled with ions resulting in an average conductivity of 0.01–0.1 mS/m, which are left behind after the streamers decay via electron attachment to oxygen molecules.

58 GEOSCIENCES↗
DOE OSTI2021

Creating heralded hyper-entangled photons using Rydberg atoms

Entangled photon pairs are a fundamental component for testing the foundations of quantum mechanics, and for modern quantum technologies such as teleportation and secured communication. Current state-of-the-art sources are based on nonlinear processes that are limited in their efficiency and wavelength tunability. This motivates the exploration of physical mechanisms for entangled photon generation, with a special interest in mechanisms that can be heralded, preferably at telecommunications wavelengths. Here we present a mechanism for the generation of heralded entangled photons from Rydberg atom cavity quantum electrodynamics (cavity QED). We propose a scheme to demonstrate the mechanism and quantify its expected performance. The heralding of the process enables non-destructive detection of the photon pairs. The entangled photons are produced by exciting a rubidium atom to a Rydberg state, from where the atom decays via two-photon emission (TPE). A Rydberg blockade helps to excite a single Rydberg excitation while the input light field is more efficiently collectively absorbed by all the atoms. The TPE rate is significantly enhanced by a designed photonic cavity, whose many resonances also translate into high-dimensional entanglement. The resulting high-dimensionally entangled photons are entangled in more than one degree of freedom: in all of their spectral components, in addition to the polarization—forming a hyper-entangled state, which is particularly interesting in high information capacity quantum communication. We characterize the photon comb states by analyzing the Hong-Ou-Mandel interference and propose proof-of-concept experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗