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At least 739 records · Page 41

Radiolytic Gas Production from Aluminum Coupons (Alloy 1100 and 6061) in Helium Environments—Assessing the Extended Storage of Aluminum Clad Spent Nuclear Fuel

Corrosion of aluminium alloy clad nuclear fuel, during reactor operation and under subsequent wet storage conditions, promotes the formation of aluminium hydroxide and oxyhydroxide layers. These hydrated mineral phases and the chemisorbed and physisorbed waters on their surfaces are susceptible to radiation-induced processes that yield molecular hydrogen gas (H 2 ), which has the potential to complicate the long-term storage and disposal of aluminium clad nuclear fuel through flammable and explosive gas mixture formation, alloy embrittlement, and pressurization. Here, we present a systematic study of the radiolytic formation of H 2 from aluminium alloy 1100 (AA1100) and 6061 (AA6061) coupons in “dry” (~0% relative humidity) and “wet” (50% relative humidity) helium environments. Cobalt-60 gamma irradiation of both aluminium alloy types promoted the formation of H 2 , which increased linearly up to ~2 MGy, and afforded G-values of 1.1 ± 0.1 and 2.9 ± 0.1 for “dry” and “wet” AA1100, and 2.7 ± 0.1 and 1.7 ± 0.1 for “dry” and “wet” AA6061. The negative correlation of H 2 production with relative humidity for AA6061 is in stark contrast to AA1100 and is attributed to differences in the extent of corrosion and varying amounts of adsorbed water in the two alloys, as characterized using optical profilometry, scanning electron microscopy, Raman spectroscopy, and X-ray diffraction techniques.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Infrared Optical Constants from Pressed Pellets of Powders: I. Improved n and k Values of (NH4)(2)SO(4)from Single-Angle Reflectance

In combination with other parameters, the real, n(?), and imaginary, k(?), components of the complex refractive index, = n + ik, can be used to simulate the optical properties of a material in different forms, e.g. its infrared spectra. But obtaining reliable values of the optical constants n/k for solid materials is challenging due to the lack of optical quality specimens, usually crystals, large enough to measure. An alternative to crystals is to press the powder into a uniform disk. We have produced pellets from ammonium sulfate, (NH4)2SO4, powder and derived the pellets’ n and k values via single-angle reflectance using a specular reflectance device in combination with a Fourier transform infrared spectrometer. The single-angle technique measures amplitude of light reflected from the material as a function of wavelength over a wide spectral domain; the optical constants are determined from the reflectance data using the Kramers-Kronig relationship. We investigate several parameters associated with the pellets and pellet formation and their effects upon delivering the most reliable n/k values. Parameters studied include pellet diameter, mass and density (void space), drying, grinding, sieving and particle size in the pellet formation, as well as pressing pressure and duration. Of these parameters, using size-selected mixtures of dried, small (< 100 µm) particles and pressing at = 10 tons for at least 30 minutes were found key to forming highly reflective samples. Comparison to two sets of previous literature n(?) and k(?) values obtained from crystalline (NH4)2SO4 both as crystal reflectance as well as extinction spectra of aerosols measured in a flow tube show reasonable agreement, but suggests the present values, as confirmed from two independent techniques, represent a substantial improvement for n/k values for (NH4)2SO4, also demonstrating promise to measure the optical constants of other materials.

Optical constants, index of refraction, single-ang↗

Tomographic optical emission spectroscopy of atmospheric pressure plasma interacting with complex surfaces

Plasma distribution in 3D space is heavily influenced by complex surfaces and the coupling interactions between plasma properties and interfacing material properties. For example, guided streamers that transition to surface ionization waves (SIWs) and propagate over structured dielectrics experience field enhancements that can lead to localized increases in ionization rates and complex 3D configurations that are difficult to analyze. Investigating these configurations requires techniques than can provide a more complete 3D picture. To help address this capability gap, a tomographic optical emission spectroscopy (tomo-OES) diagnostic system has been developed at Sandia National Laboratories that can resolve SIWs. The system includes four intensified cameras that measure the angular projections of the plasma light emission through bandpass filters. A dot calibration target co-registers each angular projection to the same voxel grid and an algebraic reconstruction technique (ART) recovers the light intensity at each voxel. An atmospheric pressure plasma jet (APPJ), provided by Peter Bruggeman, has been investigated and representative results are shown in Figure 1. Here, a bandpass filter was used to isolate emission from the N 2 second positive system (SPS) at 337.1 nm to capture the transition of the streamer to SIW on a planar dielectric surface (relative permittivity 3.3) located 3 mm below the APPJ [3]. The surface wave velocity was 3.5x10 4 (m/s), consistent with measurements made by Steven Shannon. Characterization of this APPJ will support the group effort of standing up a reproducible APPJ across institutions for applications such as liquid treatment, catalysis, and plasma aided combustion. Future work will investigate non-planar surfaces and eventually develop tomographic laser-induced fluorescence (tomo-LIF) approaches.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

An electro-optical Mott neuron based on niobium dioxide

Various applications—including brain-like computing and on-chip artificial vision—increasingly demand a combination of electronic and photonic techniques. However, integrating both approaches on a single chip is challenging, and solutions typically rely on disparate components with power-hungry signal conversions. Here, in this paper, we report electro-optical Mott neurons that combine visible light emission with electrical threshold switching, as well as neuron-like oscillations. The devices are based on thin films of sputtered niobium dioxide (NbO 2 ), a Mott insulator–metal transition material, operating at room temperature and emitting light that peaks around 810 nm. Operando measurements reveal an electronic origin to the light emission: charge carrier relaxation initiated by high-field transport in the NbO 2 . Our devices combine electrical and optical functions within a single material, thereby expanding the options available for future artificial intelligence hardware.

electrical engineering↗

Evaluation of Stripping Resistance of Organoclay-Modified Asphalt Binder and Aggregate Systems Using an Optical Contact Angle Analyzer

Organoclays, often referred to as nanoclays (NCs), are organically modified phyllosilicates. They are derived from naturally occurring clay minerals and possess unique characteristics in improving the physical and mechanical properties of polymers and rubbers. Recently, NCs have drawn interest in the modification of asphalt binders as micro-scale fillers. A few recent studies have revealed that the addition of NCs in asphalt binders improved binders’ stiffness, aging characteristics, and fatigue resistance. This study aims to evaluate the changes in moisture resistance of different NC-modified asphalt binders through the surface free energy (SFE) technique. This technique estimates SFE properties of binders and aggregates from static contact angle (SCA) data measured from an optical contact angle analyzer (OCA). Further, this study examines the changes in chemical compositions (functional groups) of binders due to the addition of selected NCs by using the Fourier Transformation Infrared (FTIR) technique. To this end, a commonly used performance grade (PG) binder (PG 64-22) modified with four different types (shape and size) of NCs, namely, Cloisite® 15 (C-15), Cloisite® 20 (C-20), Cloisite® Na+ (C-Na), and Cloisite® Ca++ (C-Ca) were evaluated in this study. The SFE data of five different types of aggregates from Oklahoma, namely, Davis Limestone (DL), Snyder Granite (SG), Dolese-Cooperton Limestone (DCL), Hanson-Davis Rhyolite (HDR), and Martin-Marietta-Mill-Creek Granite (MMMG), were used to perform their compatibility with the aforementioned NC-modified binders. The FTIR spectra revealed the presence of various alcohols, ethers, and esters in NC-modified asphalt binders. The moisture susceptibility analysis shows that the addition of NC results in an increase of SFE and cohesive energy of an asphalt binder, which are desired for improved moisture resistance. The addition of NC also shows improved compatibility in cases of all aggregates. Among the five aggregates, MMMCG showed the highest compatibility with all binders, followed by DCL, HDR, DL, and SG. In regard to NCs, the C-15 sample showed the highest compatibility followed by C-20, C-Na, and C-Ca.

Hossain, Zahid↗

Non-destructive identification of absorptive damage sites by photoluminescence brightening

We present a non-destructive photoluminescence (PL) imaging strategy for probing damage growth behavior in fused silica under laser irradiation. Transient wide-field PL image measurements were conducted at varying excitation intensities to investigate the dynamics of radiative defect generation and annihilation in laser-induced damage sites. Our results reveal that, while low excitation intensities predominantly induce PL quenching due to defect annihilation, high-intensity excitation (>0.3 GW/cm 2 at 532 nm) triggers pronounced PL brightening (PLB), indicative of radiative defect generation. Image analysis demonstrates that PLB events are strongly correlated with subsequent damage growth (10 J/cm 2 at 351 nm), whereas overall PL intensity is not. No optically detectable morphological changes were observed during PLB, confirming the non-destructive nature of the technique. We propose that PLB arises from defect-assisted absorption of multiple photons at pre-existing absorptive centers, which enhances local absorptivity and initiates further defect formation. These findings establish PLB monitoring as a sensitive diagnostic tool for identifying damage sites with elevated absorptivity, enabling targeted maintenance and improved laser damage management in optical materials.

Materials science↗

Double-pulse speckle contrast correlations with near Fourier transform limited free-electron laser light using hard X-ray split-and-delay

Abstract The ability to deliver two coherent X-ray pulses with precise time-delays ranging from a few femtoseconds to nanoseconds enables critical capabilities of probing ultra-fast phenomena in condensed matter systems at X-ray free electron laser (FEL) sources. Recent progress made in the hard X-ray split-and-delay optics developments now brings a very promising prospect for resolving atomic-scale motions that were not accessible by previous time-resolved techniques. Here, we report on characterizing the spatial and temporal coherence properties of the hard X-ray FEL beam after propagating through split-and-delay optics. Speckle contrast analysis of small-angle scattering measurements from nanoparticles reveals well-preserved transverse coherence of the beam. Measuring intensity fluctuations from successive X-ray pulses also reveals that only single or double temporal modes remain in the transmitted beam, corresponding to nearly Fourier transform limited pulses.

42 ENGINEERING↗

Improving OFDR Distributed Fiber Sensing by Fibers With Enhanced Rayleigh Backscattering and Image Processing

This article investigates using optical fibers with enhanced backscattering profiles to improve distributed fiber sensor performance and reduce instrumentation costs. Using a femtosecond (fs) laser direct writing technique, the Rayleigh backscattering profile of a standard telecom fiber was enhanced by more than 40 dB to improve the signal-to-noise ratio (SNR) for optical frequency domain reflectometry (OFDR). The enhanced backscattering signals enable effectively distributed strain measurements using a low-cost tunable laser (TL). Median filtering is applied to denoise cross correlation results to further improve measurement outcomes. Results presented in this article show that a TL with a 1-nm tuning range, which is far less than the tuning range used in commercial OFDR interrogators, can perform effectively distributed strain measurements using sensing fibers with enhanced backscattering profiles. The sensing fiber with over 40-dB backscattering enhancement achieved 4.8-cm spatial resolution in strain measurements with a root mean square accuracy of less than 2.70 με when 10–50 με were exerted to the sensing fiber. In conclusion, results presented in this article reveal both the potential and limitations of sensing fibers with enhanced backscattering for OFDR-based distributed fiber sensors.

42 ENGINEERING↗

Spectrally reconfigurable quantum emitters enabled by optimized fast modulation

The ability to shape photon emission facilitates strong photon-mediated interactions between disparate physical systems, thereby enabling applications in quantum information processing, simulation and communication. Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is particularly attractive for realizing such applications on-chip. Here we propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Using a scattering-matrix formalism, we find that a two-level system, when modulated faster than its optical lifetime, can be treated as a single-photon source with a widely reconfigurable photon spectrum that is amenable to standard numerical optimization techniques. To enable the experimental demonstration of this spectral control scheme, we investigate the Stark tuning properties of the silicon vacancy in silicon carbide, a color center with promise for optical quantum information processing technologies. We find that the silicon vacancy possesses excellent spectral stability and tuning characteristics, allowing us to probe its fast modulation regime, observe the theoretically-predicted two-photon correlations, and demonstrate spectral engineering. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Adaptive shape control of wavefront-preserving X-ray mirrors with active cooling and heating

This article describes the development and testing of a novel, water cooled, active optic mirror system (called “REAL: Resistive Element Adjustable Length”) that combines cooling with applied auxiliary heating, tailored to the spatial distribution of the thermal load generated by the incident beam. This technique is theoretically capable of sub-nanometer surface figure error control even at high power density. Tests conducted in an optical metrology laboratory and at synchrotron X-ray beamlines showed the ability to maintain the mirror profile to the level needed for the next generation storage rings and FEL mirrors.

42 ENGINEERING↗

Hybrid Machine Learning for Scanning Near-Field Optical Spectroscopy

The underlying physics behind an experimental observation often lacks a simple analytical description. This is especially the case for scanning probe microscopy techniques, where the interaction between the probe and the sample is nontrivial. Realistic modeling to include the details of the probe is always exponentially more difficult than its "spherical cow" counterparts. On the other hand, a well-trained artificial neural network based on real data can grasp the hidden correlation between the signal and sample properties. In this work, we show that, via a combination of model calculation and experimental data acquisition, a physics-infused hybrid neural network can predict the tip-sample interaction in the widely used scattering-type scanning near-field optical microscope. This hybrid network provides a long-sought solution for accurate extraction of material properties from tip-specific raw data. The methodology can be extended to other scanning probe microscopy techniques as well as other data-oriented physical problems in general.

36 MATERIALS SCIENCE↗

Atomic fluctuations in electronic materials revealed by dephasing

The microscopic origin and timescale of the fluctuations of the energies of electronic states has a significant impact on the properties of interest of electronic materials, with implication in fields ranging from photovoltaic devices to quantum information processing. Spectroscopic investigations of coherent dynamics provide a direct measurement of electronic fluctuations. Modern multidimensional spectroscopy techniques allow the mapping of coherent processes along multiple time or frequency axes and thus allow unprecedented discrimination between different sources of electronic dephasing. Exploiting modern abilities in coherence mapping in both amplitude and phase, we unravel dissipative processes of electronic coherences in the model system of CdSe quantum dots (QDs). The method allows the assignment of the nature of the observed coherence as vibrational or electronic. The expected coherence maps are obtained for the coherent longitudinal optical (LO) phonon, which serves as an internal standard and confirms the sensitivity of the technique. Fast dephasing is observed between the first two exciton states, despite their shared electron state and common environment. This result is contrary to predictions of the standard effective mass model for these materials, in which the exciton levels are strongly correlated through a common size dependence. In contrast, the experiment is in agreement with ab initio molecular dynamics of a single QD. Electronic dephasing in these materials is thus dominated by the realistic electronic structure arising from fluctuations at the atomic level rather than static size distribution. The analysis of electronic dephasing thereby uniquely enables the study of electronic fluctuations in complex materials.

36 MATERIALS SCIENCE↗

Optically Enhanced Solid-State 1 H NMR Spectroscopy

Low sensitivity is the primary limitation to extending nuclear magnetic resonance (NMR) techniques to more advanced chemical and structural studies. Photochemically induced dynamic nuclear polarization (photo-CIDNP) is an NMR hyperpolarization technique where light is used to excite a suitable donor–acceptor system, creating a spin-correlated radical pair whose evolution drives nuclear hyperpolarization. Systems that exhibit photo-CIDNP in solids are not common, and this effect has, up to now, only been observed for 13 C and 15 N nuclei. However, the low gyromagnetic ratio and natural abundance of these nuclei trap the local hyperpolarization in the vicinity of the chromophore and limit the utility for bulk hyperpolarization. Here, we report the first example of optically enhanced solid-state 1 H NMR spectroscopy in the high-field regime. This is achieved via photo-CIDNP of a donor–chromophore–acceptor molecule in a frozen solution at 0.3 T and 85 K, where spontaneous spin diffusion among the abundant strongly coupled 1 H nuclei relays polarization through the whole sample, yielding a 16-fold bulk 1 H signal enhancement under continuous laser irradiation at 450 nm. These findings enable a new strategy for hyperpolarized NMR beyond the current limits of conventional microwave-driven DNP.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interference fringe (IF) technique for droplet contact angle and thickness measurements: Ultralow contact angle and nanoscale thickness measurement

Recently, reflection interference fringe (RIF) and transmission fringe (TIF) techniques have been introduced to investigate the origin of far-field interference fringe (IF) formation and to determine a droplet's contact angle and thickness by measuring the fringe radius. In this study, characteristics of the IF technique are analyzed based on the RIF and TIF by varying the schematics, such as configuration (transmission/reflection), the droplet's side (left-hand side/right-hand side), and the substrate types (flat/prism). The analysis also investigates the refraction effect at the droplet edge and the maximum incidence and contact angles. The schematic variation shows that the widest contact angle range can be measured in a transmission configuration with droplet's right-hand side, and that the fringe radius decreases with incidence angles on a prism substrate, consistent with the recent observation. Refraction at the droplet edge causes the fringe radius to increase or decrease depending on the degree of refraction. Based on the characteristics study, it is revealed that the IF technique can determine nanometer-scale thicknesses below 100 nm on droplets, corresponding to ultra-small contact angles of less than 0.01°, with an extended working distance of 3000 mm and an optimized incidence angle, assuming a spherical profile. This finding is significant, as it demonstrates that the nanoscale thickness can be determined in situ under ambient conditions using a simple optical configuration, without requiring a sophisticated setup, such as a microscope. It is anticipated that the IF technique can be combined with other nanoscale thickness measurement techniques to enhance its measurement reliability.

36 MATERIALS SCIENCE↗

Probing single-chain conformation and its impact on the optoelectronic properties of donor–accepter conjugated polymers

The chain conformation of donor–acceptor conjugated polymers (D–A CPs) is critical to their optical and electronic properties. However, probing the conformation of D–A CPs (e.g., persistence length and contour length) at a single-chain level is challenging due to the formation of aggregates in dilute solution, even in a good solvent. In this work, we studied the chain conformation and corresponding optical spectra for high-performance D–A CPs in the single-chain state by multimodal variable-temperature scattering and spectroscopy techniques, as well as by molecular dynamics simulations. Here we found a critical role of the side-chain length and branch point in the persistence length and optical absorption due to steric effects. Hence, it is important to consider both the chain rigidity and coplanarity of the polymer backbone to achieve desirable optoelectronic properties. Our findings bridge the fundamental knowledge gaps to design new CPs with desired optoelectronic properties via molecular engineering for next-generation electronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum control of exciton wave functions in 2D semiconductors

Excitons—bound electron-hole pairs—play a central role in light-matter interaction phenomena and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over excitonic motion. We present a technique using nanostructured gate electrodes to create tailored potential landscapes for excitons in 2D semiconductors, enabling in situ wave function shaping at the nanoscale. Our approach forms electrostatic traps for excitons in various geometries, such as quantum dots, rings, and arrays thereof. We show independent spectral tuning of spatially separated quantum dots, achieving degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wave functions in optical reflection and photoluminescence measurements. This work unlocks possibilities for engineering exciton dynamics and interactions at the nanometer scale, with implications for optoelectronic devices, topological photonics, and quantum nonlinear optics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Engineering the Microstructure and Morphology of Explosive Films via Control of Interfacial Energy

Physical vapor deposition of organic explosives enables growth of polycrystalline films with a unique microstructure and morphology compared to the bulk material. This study demonstrates the ability to control crystal orientation and porosity in pentaerythritol tetranitrate films by varying the interfacial energy between the substrate and the vapor-deposited explosive. Additionally, variation in density, porosity, surface roughness, and optical properties is achieved in the explosive film, with significant implications for initiation sensitivity and detonation performance of the explosive material. Various surface science techniques, including angle-resolved X-ray photoelectron spectroscopy and multiliquid contact angle analysis, are utilized to characterize interfacial characteristics between the substrate and explosive film. Optical microscopy and scanning electron microscopy of pentaerythritol tetranitrate surfaces and fracture cross sections illustrate the difference in morphology evolution and the microstructure achieved through surface energy modification. X-ray diffraction studies with the Tilt-A-Whirl three-dimensional pole figure rendering and texture analysis software suite reveal that high surface energy substrates result in a preferred (110) out-of-plane orientation of pentaerythritol tetranitrate crystallites and denser films. Low surface energy substrates create more randomly textured pentaerythritol tetranitrate and lead to nanoscale porosity and lower density films. This work furthers the scientific basis for interfacial engineering of polycrystalline organic explosive films through control of surface energy, enabling future study of dynamic and reactive detonative phenomena at the microscale. Results of this study also have potential applications to active pharmaceutical ingredients, stimuli-responsive polymer films, organic thin film transistors, and other areas.

36 MATERIALS SCIENCE↗

MUSE adaptive-optics spectroscopy confirms dual active galactic nuclei and strongly lensed systems at sub-arcsec separation

The novel Gaia multi peak (GMP) technique has proven to be able to successfully select dual and lensed active galactic nuclei (AGN) candidates at sub-arcsecond separations. Both populations are important because dual AGN represent one of the central, still largely untested, predictions of ΛCDM cosmology, and compact lensed AGN allow us to probe the central regions of the lensing galaxies. In this work, we present high-spatial-resolution spectroscopy of 12 GMP-selected systems. We used the adaptive-optics assisted integral-field spectrograph MUSE at the VLT to resolve each system and investigate the nature of each component. All targets show the presence of two components confirming the GMP selection. We classify 4 targets as dual AGN, 3 as lensed quasar candidates, and 5 as a chance alignment of a star and an AGN. With separations ranging from 0.30″ to 0.86″, these dual and lensed systems are among the most compact systems discovered to date at z > 0.5. This is the largest sample of distant dual AGN with sub-arcsecond separations ever presented in a single paper.

Scialpi, M. (ORCID:0009000651004986)↗