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At least 829 records · Page 46

Ultrashort XUV pulse absorption spectroscopy of partially oxidized cobalt nanoparticles

High-order harmonic generation (HHG) based transient extreme ultraviolet (XUV) absorption spectroscopy is an emerging technique to trace photoinduced charge carrier dynamics in condensed phase materials with femtosecond and even attosecond temporal resolution and elemental specificity. However, its application to nanoparticulate samples that are relevant, for example, for novel photocatalytic light harvesting concepts, has been limited. This is in part due to the challenge to produce residual-free samples on ultrathin, XUV-transparent substrates as well as a widespread understanding that sparsely distributed nanoparticles do not provide sufficient contrast for XUV absorption measurements. Here, we present static XUV absorption spectra of partially oxidized Co nanowire-structures with diameters of approximately 4.5 nm and lengths between 10 and 40 nm, recorded with an ultrashort pulse HHG light source. Nanoparticles are synthesized by the agglomeration of Co atoms inside superfluid helium droplets, followed by surface deposition and oxidation in ambient air. The method is uniquely suited for residual-free synthesis of transition metal nanowires and their deposition on ultrathin substrates. Analysis by high-resolution transmission electron microscopy reveals the formation of CoO nanowires with regions of unoxidized Co in their interior. The nanoparticle samples are investigated in an HHG-driven ultrafast XUV absorption setup. Despite the low surface coverage of only 23%, the recorded spectrum exhibits a distinct absorption feature at the Co M 2,3 (2p) edge near 60 eV with a peak height of about 40 mOD. Finally, the results support the feasibility of table-top ultrafast transient XUV absorption studies of photoinduced dynamics in transition metal oxide nanoparticles with sub-monolayer surface coverage.

74 ATOMIC AND MOLECULAR PHYSICS↗

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

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

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Cosmological implications of the full shape of anisotropic clustering measurements in BOSS and eBOSS

We present the analysis of the full shape of anisotropic clustering measurement from the extended Baryon Oscillation Spectroscopic Survey (eBOSS) quasar sample together with the combined galaxy sample from the Baryon Oscillation Spectroscopic Survey (BOSS), re-analysed using an updated recipe for the non-linear matter power spectrum and the non-local bias parameters. We obtain constraints for flat Lambda cold dark matter cosmologies, focusing on the cosmological parameters that are independent of the Hubble parameter h. Our recovered value for the Root Mean Square (RMS) linear perturbation theory variance as measured on the scale of 12 Mpc is σ 12 = 0.805 ± 0.049, while using the traditional reference scale of 8 h –1 Mpc gives σ 8 = 0.815 ± 0.044. We quantify the agreement between our measurements and the latest cosmic microwave background data from Planck using the suspiciousness metric, and find them to be consistent within 0.64 ± 0.03σ. Combining our clustering constraints with the 3 × 2pt data sample from the Dark Energy Survey Year 1 release slightly degrades this agreement to the level of 1.54 ± 0.08σ, while still showing an overall consistency with Planck. We furthermore study the effect of imposing a Planck – like prior on the parameters that define the shape of the linear matter power spectrum, and find significantly tighter constraints on the parameters that control the evolution of density fluctuations. In particular, the combination of low-redshift data sets prefers a value of the physical dark energy density ω DE = 0.335 ± 0.011, which is 1.7σ higher than the one preferred by Planck.

79 ASTRONOMY AND ASTROPHYSICS↗

Intrinsic spatial chirp of subcycle terahertz pulsed beams

Here, we present an analysis of spatial chirp in subcycle pulsed beams corroborated by spatiotemporal electro-optic sampling measurements of terahertz radiation. Modeling the subcycle pulsed beam as a superposition of monochromatic Gaussian beams, free-space propagation is shown to directly lead to lateral spatial chirp with the spectrum on-axis substantially bluer than the overall energy spectrum. The two-transverse + one-temporal dimensional profile of terahertz subcycle pulsed beams from organic crystals DSTMS and OH1 are measured and compared with observed spatiospectral correlations consistent with the model.

43 PARTICLE ACCELERATORS↗

Atacama Cosmology Telescope: Multiprobe cosmology with unWISE galaxies and ACT DR6 CMB lensing

We present a joint analysis of the cosmic microwave background (CMB) lensing power spectra measured from the Data Release 6 of the Atacama Cosmology Telescope (ACT) and Planck PR4, cross-correlations between the ACT and Planck lensing reconstruction and galaxy clustering from unWISE, and the unWISE clustering auto-spectrum. We obtain 1.5% constraints on the matter density fluctuations at late times parametrized by the best constrained parameter combination 𝑆$^{3⁢x⁢2⁢pt}_{8}$ ≡ 𝜎 8 ⁢(Ω 𝑚 /0.3) 0.4 = 0.815 ± 0.012. The commonly used 𝑆 8 ≡ 𝜎 8⁢ (Ω 𝑚 /0.3) 0.5 parameter is constrained to 𝑆 8 = 0.816 ± 0.015. In combination with baryon acoustic oscillation (BAO) measurements we find 𝜎 8 = 0.815 ± 0.012. We also present sound-horizon-independent estimates of the present day Hubble rate of 𝐻 0 = 66.4$^{+3.2}_{−3.7}$ km s −1 Mpc −1 from our large scale structure data alone and 𝐻 0 = 64.3$^{+2.1}_{−2.4}$ km s −1 Mpc −1 in combination with uncalibrated supernovae from Pantheon+. Using parametric estimates of the evolution of matter density fluctuations, we place constraints on cosmic structure in a range of high redshifts typically inaccessible with cross-correlation analyses. Combining lensing cross- and autocorrelations, we derive a 3.3% constraint on the integrated matter density fluctuations above 𝑧 = 2.4, one of the tightest constraints in this redshift range and fully consistent with a Λ cold dark matter (Λ⁢CDM) model fit to the primary CMB from Planck. Finally, combining with primary CMB observations and using the extended low redshift coverage of these combined datasets we derive constraints on a variety of extensions to the Λ⁢CDM model including massive neutrinos, spatial curvature, and dark energy. We find in flat Λ⁢CDM⁢ ∑𝑚 𝜈 < 0.12 eV at 95% confidence using the large scale structure data, BAO measurements from Sloan Digital Sky Survey, and primary CMB observations.

79 ASTRONOMY AND ASTROPHYSICS↗

Sandia Electromagnetic Environment Simulator Facilities

Sandia National Laboratories’ (Sandia’s) Electrical Sciences Group (1350) provides a spectrum of solutions for electromagnetic (EM) environment effects on electrical systems to advance physical understanding including experiments, analytical and numerical model development leveraging first-principles physics, and high-performance computational modeling and simulation (M&S). The six departments in the Electrical Sciences Group provide analysis, design guidance, and experiments in support of nuclear weapons qualification in normal, abnormal, and hostile environments, as well as research and development for advanced electrical systems that can operate through these environments. This document is intended to provide a quick summary of Sandia’s EM experimental facilities, most of which provide unique national capabilities.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamic infrared gas analysis from longleaf pine fuel beds burned in a wind tunnel: observation of phenol in pyrolysis and combustion phases

Pyrolysis is the first step in a series of chemical and physical processes that produce flammable organic gases from wildland fuels that can result in a wildland fire. We report results using a new time-resolved Fourier transform infrared (FTIR) method that correlates the measured FTIR spectrum with an infrared thermal image sequence, enabling the identification and quantification of gases within different phases of the fire process. The flame from burning fuel beds composed of pine needles (Pinus palustris) and mixtures of sparkleberry, fetterbush, and inkberry plants was the natural heat source for pyrolysis. Extractive gas samples were analyzed and identified in both static and dynamic modes synchronized to thermal infrared imaging: a total of 29 gases were identified including small alkanes, alkenes, aldehydes, nitrogen compounds, and aromatics, most previously measured by FTIR in wildland fires. This study presents one of the first identifications of phenol associated with both pre-combustion and combustion phases using ca. 1 Hz temporal resolution. Preliminary results indicate ~2.5× greater phenol emissions from sparkleberry and inkberry compared to fetterbush, with differing temporal profiles.

09 BIOMASS FUELS↗

Reactions of U(DMSO) 8 (ClO 4 ) 4 with Terpyridine Yield Dimeric Hydrolysis Products and Induce C–C Coupling

Reactions have been carried out using UIV(DMSO) 8 (ClO 4 ) 4 with 2,2′:6′,2″-terpyridine (terpy) under nonaqueous conditions. At room temperature in acetonitrile, the combination of the U(IV) starting material with terpy resulted in a mixture containing [UO 2 (DMSO) 2 terpy][ClO 4 ] 2 ·MeCN, while increasing the water content led to the hydrolysis products [(UO 2 (DMSO)terpy) 2 (μ 2 –O)][ClO 4 ] 2 and [(UO 2 terpy) 2 (μ 2 –OH) 2 ][ClO 4 ] 2 ·MeCN·H 2 O. Performing the reaction at slightly elevated temperature with no added water led to the formation of [UO 2 sexipyridine][ClO 4 ] 2 ·MeCN. This new uranyl complex contains the hexadentate ligand 2,2′:6′,2″:6″,2″:6‴,2⁗:6⁗,2⁗′-sexipyridine, which formed in situ from the tetravalent uranium starting material, where photoexcited uranyl or in situ generated peroxide could have induced C–C coupling. Analysis of bonding in the dimeric uranyl species via quantum chemical methods revealed a small increase in covalency of the bridging oxo unit and a slightly greater stability compared to the bridging hydroxo compound, which causes a significant shift in the uranyl symmetric stretch in the Raman spectrum. Structural, spectroscopic, and computational comparisons are made across the series of compounds, providing insight into the bonding and reactivity of uranium in nonaqueous media.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Normal modes, rotational inertia, and thermal fluctuations of trapped ion crystals

The normal modes of a trapped ion crystal are derived using an approach based on the Hermitian properties of the system’s dynamical matrix. This method is equivalent to the standard Bogoliubov method, but for classical systems it is arguably simpler and more general in that canonical coordinates are not necessary. The theory is developed for stable, unstable, and neutrally-stable systems. The method is then applied to ion crystals in a Penning trap. Reduced eigenvalue problems for the case of large applied magnetic field are developed, for which the spectrum breaks into E x B drift modes, axial modes, and cyclotron modes. Thermal fluctuation levels in these modes are analyzed and shown to be consistent with the Bohr-van-Leeuwen theorem, provided that neutrally-stable modes associated with crystal rotations are included in the analysis. An expression for the rotational inertia of the crystal is derived, and a magnetic contribution to this inertia, which dominates in large magnetic fields, is described. An unusual limit is discovered for the special case of spherically-symmetric confinement, in which the rotational inertia does not exist and changes in angular momentum leave the rotation frequency unaffected.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Design of an epithermal neutron velocity selection system for the Penn State Breazeale Reactor

A series of mechanical neutron choppers to operate as a velocity selection system have been developed for the Pennsylvania State Breazeal Reactor (PSBR). This chopper system will provide pulsed epithermal neutrons in the energy range of 0.5–40 eV with 2% or better energy resolution, and with a transmission of 1E-6 or better. Four different chopper geometries have been evaluated for their utility as mechanical neutron choppers. Specifically, Fermi, ring, piston, and disc choppers have been evaluated to assess their potential neutronics performance and mechanical constructability. A series of high-speed disc choppers were selected for the final design, and optimization work was performed to maximize the neutron pulse intensity. It is estimated that the optimized system will produce an epithermal neutron intensity of approximately 96 n/s. This system can also be operated in a time of flight (TOF) configuration such that the neutrons arriving at the source have a white spectrum. This operation can be accomplished by leaving the second stage of choppers in the open position, or by removing it from the beam completely. Such unique source of epithermal neutrons produced by this chopper system will have applications in both prompt and delayed epithermal neutron activation analysis (ENAA), as well as in neutron resonance transmission analysis (NRTA).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Planck constraints and gravitational wave forecasts for primordial black hole dark matter seeded by multifield inflation

Here, we perform a Markov Chain Monte Carlo analysis of a simple yet generic multifield inflation model characterized by two scalar fields coupled to each other and nonminimally coupled to gravity, fit to Planck 2018 cosmic microwave background (CMB) data. In particular, model parameters are constrained by data on the amplitude of the primordial power spectrum of scalar curvature perturbations on CMB scales A s , the spectral index n s , and the ratio of power in tensor to scalar modes r, with a prior that the primordial power spectrum should also lead to primordial black hole (PBH) production sufficient to account for the observed dark matter abundance. We find that n s in particular controls the constraints on our model. Whereas previous studies of PBH formation from an ultraslow-roll phase of inflation have highlighted the need for at least one model parameter to be highly fine-tuned, we identify a degeneracy direction in parameter space such that shifts by ~10% of one parameter can be compensated by comparable shifts in other parameters while preserving a close fit between model predictions and observations. Furthermore, we find this allowed parameter region produces observable gravitational wave signals in the frequency ranges to which upcoming experiments are projected to be sensitive, including Advanced LIGO and Virgo, the Einstein Telescope, Cosmic Explorer, DECIGO, and LISA.

79 ASTRONOMY AND ASTROPHYSICS↗

Dose Calculations from Source Models and Gamma-Ray Spectra

Gamma-ray dose rates computed by two radiation source model-based methods and five measured spectrum-based methods are compared. With the exception of a Detective DX-100, which reported dose rates that are about 25% less than the mean, dose rates are generally within 10% of mean values. Methods for computation of dose rates employed by the Gamma Detector Response and Analysis Software (GADRAS) are described and critically evaluated. Results are presented for a feasibility evaluation that seeks to use spectra recorded inside vehicles to estimate the minimum dose outside the vehicles.

61 RADIATION PROTECTION AND DOSIMETRY↗

Orbit response measurements with oscillating trajectories

Optical properties of components in a linac can be reconstructed from analysis of the orbit response matrix, composed from responses of BPMs to changes in currents of dipole correctors. An efficient way to record such response, discussed in this note, is to excite the corrector current with a sine wave and record its Fourier component of the BPM spectrum. Because of a narrow band of the excitation signal, response to multiple correctors can be recorded at the same time without significantly affecting the signal-to-noise ratio. For that, the correctors are oscillated at different frequencies, and the corresponding BPM Fourier components are recorded. In an ion (non-relativistic) linac, similar measurements can be performed for the longitudinal plane as well. Examples of measurements at the PIP2IT test linac are shown.

43 PARTICLE ACCELERATORS↗

Improvement and Verification of Online Cross Section Generation Capability of Griffin for TRISO-fueled Reactors

Griffin, a MOOSE-based reactor multiphysics code jointly developed by Idaho National Laboratory and Argonne National Laboratory under the DOE Office of Nuclear Energy’s NEAMS program, has pursued the development of an online multigroup cross section generation capability for a few years to enable high-fidelity, problem-dependent neutronics analyses of advanced thermal reactors. Recent advancements in Griffin’s online multigroup cross section generation capability have significantly improved the accuracy, robustness, and efficiency of self-shielding calculations for both prismatic and pebble-bed TRISO-fueled reactor applications. Key developments include a unified fuel self-shielding method applicable to both TRISO and annular compact/spherical shell fuel zone geometries; an advanced Dancoff Category-based Equivalence Theory using a bell function for non-fuel resonance treatment, achieving more than an order-of-magnitude speedup compared to the Tone method; an on-the-fly multigroup equivalence approach to mitigate group condensation errors; and a streaming correction method for pebble-bed homogenization. A proof-of-concept demonstration of on-the-fly group condensation with consistent P0 transport correction was also achieved. The method reproduced direct fine-group solutions with excellent accuracy (eigenvalue errors within 10 pcm and pin-power differences within 0.5%), but due to performance limitations of the current fixed-source solver, improvements to solver efficiency will be addressed in future work. Verification tests were performed on graphite-moderated TRISO-fueled two-dimensional core benchmark problems representing gas-cooled microreactors, heat pipe-cooled microreactors, gas-cooled pebble-bed reactors, and fluoride salt-cooled high-temperature reactors. Across all cases, Griffin showed excellent agreement with Serpent2 continuous energy Monte Carlo solutions: eigenvalue errors within 200 pcm, pin-power root-mean-square errors within 2%, and control rod and drum worth errors less than 2%. It should be noted that, for the benchmark problem, cross section generation contributed less than 3% of the total simulation times. These results demonstrate that Griffin’s online cross section generation capability delivers accurate and efficient reactor physics solutions across a wide spectrum of TRISO-fueled advanced reactor designs. With further improvements to the fine-group fixed-source solver and planned extensions to depletion, transients, and coupled neutron–gamma transport, Griffin will be well-positioned to become a powerful and comprehensive tool for advanced reactor analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Probabilistic Analysis of Long-Term Degradation of Microwave Cavity Flow Sensor

We are investigating a microwave resonant cavity transducer for flow sensing in the vessel of a high temperature fluid advanced reactor (AR), such as a molten salt cooled reactor (MSCR) or a sodium fast reactor (SFR). This transducer is a hollow metallic cylindrical cavity, with the flat wall of the cylinder flexible enough to undergo microscopic deflection due to dynamic fluid pressure. Membrane deflection leads to a shift in the resonant frequency, which can be detected with a spectrum analyzer. We have performed a proof-of-concept experiment of flow sensing with the transducer in liquid sodium at 340°C in impinging liquid jet geometry. The transducer remained in liquid sodium for 70 days. After removal, no structural damage was observed, and the expected transducer response was verified in a water test. Because long-term (multi-year) experimental tests of transducer resilience to harsh environment are not practical, we have developed a probabilistic model of creep to estimate transducer resilience to the harsh environment. The probabilistic model considers diffusion creep under the condition of high temperature and low stress, where the stress and temperature are allowed to be random variables with Gaussian distributions. Using the probabilistic model, we estimate inelastic membrane deflections due to creep for several temperature ranges. We conclude that for temperatures less than 650°C, creep has negligible long-term effect on the transducer performance. Since a yellowish residue was observed on the transducer surface after 70 days of immersion in liquid sodium, we have investigated possible evidence of corrosion. Chromium depletion is a typical indicator of the corrosion process in stainless steel. Scraping off a residue from the transducer and performing scanning electron microscopy (SEM) with energy dispersive analysis (EDS) did not find any chromium in the residue. Approximately 60% of the residue consisted of copper, which can be attributed to contamination of sodium due to powder residue from machining of copper and brass components of the transducer.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Energetics of oxidation and formation of uranium mononitride

Uranium mononitride (UN) is an advanced nuclear fuel currently being considered for use in several generation IV fast and thermal neutron spectrum core designs, with additional applications to thermal and electric nuclear propulsion reactors. Here, to better understand the thermal behavior and thermodynamic stability of UN, we investigated the bulk thermal oxidation process and thermochemical reactions, including the enthalpy of oxidation and standard enthalpy of formation, by conducting thermalgravimetric analysis – differential scanning calorimetry coupled with mass spectrometry (TGA-DSC-MS), and high temperature transposed temperature drop and oxide melt drop solution calorimetry. The bulk oxidation of UN (containing a small amount of α-UN 1.5+x ) in air was found to follow a step-wise process characterized by consecutive oxidative reactions UN-UN 1.5+x -UO 2 → UO 2 -UO 3 —N k → UO 3 —N k → UO 3 → U 3 O 8 . TGA results support that the UO 2 – U 2 N 3+x passivating layer delays the onset of rapid bulk oxidation of UN in air up to 662 K. Synchrotron X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) analyses were performed to characterize UN and its final oxidized product. The standard enthalpy of formation (ΔH° f ) of UN was determined to be –144.4 ± 5.9 kJ/mol·atom, in good agreement with previously determined values from Pt encapsulation and bomb calorimetric experiments. Lastly, a negative linear correlation between ΔH° f and the N/U molar ratio was established based on the thermochemical data obtained in this work and previously reported enthalpies of formations of β-UN 1.5-x and α-UN 1.5+x .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nonlinear mode coupling and energetics of driven magnetized shear-flow turbulence

To comprehensively understand the saturation of two-dimensional (2D) magnetized Kelvin–Helmholtz-instability-driven turbulence, energy transfer analysis is extended from the traditional interaction between scales to include eigenmode interactions, by using the nonlinear couplings of linear eigenmodes of the ideal instability. While both kinetic and magnetic energies cascade to small scales, a significant fraction of turbulent energy deposited by unstable modes in the fluctuation spectrum is shown to be re-routed to the conjugate-stable modes at the instability scale. They remove energy from the forward cascade at its inception. The remaining cascading energy flux is shown to attenuate exponentially at a small scale, dictated by the large-scale stable modes. Guided by a widely used instability-saturation assumption, a general quasi-linear model of instability is tested by retaining all nonlinear interactions except those that couple to the large-scale stable modes. These complex interactions are analytically removed from the magnetohydrodynamic equations using a novel technique. Observations are an explosive large-scale vortex separation instead of the well-known merger of 2D, a dramatic enhancement in turbulence level and spectral energy fluxes, and a reduced small-scale dissipation length scale. These show the critical role of the stable modes in instability saturation. Possible reduced-order turbulence models are proposed for fusion and astrophysical plasmas, based on eigenmode-expanded energy transfer analyses.

Physics↗

The motional Stark effect diagnostic for ITER

An overview of the plans for the motional Stark effect (MSE) diagnostic installation on the International Thermonuclear Experimental Reactor (ITER) is presented. The MSE diagnostic uniquely provides spatially localized magnetic field measurements inside the plasma. These are used to constrain equilibrium reconstructions to determine q(r), the safety factor as a function of minor radius. Meeting the system requirements to deliver q-profiles and related quantities with the specified radial resolution of 20 points over the minor radius, 10 ms time resolution, and better than 10% accuracy is challenging. MSE systems observe the D/H-α emission near 656.3 nm from neutral beams. As the beam atoms traverse the magnetic field, B⃗, at high velocity, v⃗, they experience a Lorentz electric field, v⃗×B⃗, which causes the spectral emission to be split and polarized due to the Stark effect. Traditional MSE-LP (line polarization) measurements determine the direction of the magnetic field in the observation volume using polarimetric analysis of the detected light. The harsh conditions of ITER are expected to deposit thin films of contaminants on the first mirror, which would alter the polarization state of reflected light significantly. On ITER, the combination of high magnetic field strength and high energy beams makes the Stark spectrum resolution suitable for the determination of the magnetic field magnitude from the line shift, so this approach has been selected. Every aspect of the measurement system must be planned for the burning plasma environment and carefully analyzed ahead of time. Current status and plans for the system are presented.

Instruments & Instrumentation↗