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DOE OSTI2026

Near-Real-Time Material Tracking: Combining Vis–NIR Spectroscopy with Flow Sensing for Accurate Nd(III) Quantification

A fiber-optic visible–near-infrared (vis–NIR) absorption spectroscopy and flow sensor system has been developed for near-real-time tracking of Nd mass in the effluent stream from a column in a fume hood. The approach leverages two unique data streams and a partial least-squares regression (PLSR) model trained on vis–NIR absorption spectra of Nd(III) (0–1.5 M) in 1 M HNO 3 . In-line volumetric flow rate and vis–NIR spectra are measured in sequence after a chromatography column. The time stamps from each data stream are then synchronized, which allows integrated volumes to be combined with Nd(III) molarities predicted by a PLSR model to accurately calculate the Nd mass flowing through the column. This integrated measurement provides instantaneous mass flow and accumulates these data over time to obtain the total mass processed. The methodology developed in this study contributes critical technical infrastructure to improve monitoring capabilities to support chemical separations and the production of strategic materials and isotopes.

Irvine, Sawyer B. [Oak Ridge National Laboratory (↗

DOE OSTI2022

Isotopic Signatures of Lithium Carbonate and Lithium Hydroxide Monohydrate Measured Using Raman Spectroscopy

Lithium isotopic ratios have wide ranging applications as chemical signatures, including improved understanding of geochemical processes and battery development. Measurement of isotope ratios using optical spectroscopies would provide an alternative to traditional mass spectrometric methods, which are expensive and often limited to a chemical laboratory. In this work, Raman spectra of 7 Li 2 CO 3 , 6 Li 2 CO 3 , 7 LiOH*H 2 O and 6 LiOH*H 2 O have been measured to determine the effect of lithium isotope substitution on the Raman molecular vibrations. Thirteen peaks were observed in the spectrum of lithium carbonate, with discernable isotopic shifts occurring in eleven of the thirteen vibrations, two of which have not been previously reported in the literature. The spectrum of lithium hydroxide monohydrate contained nine peaks, with discernable isotopic shifts occurring in eight of the nine vibrations, four of which have not been previously reported in the literature. The Raman spectral data reported here for lithium carbonate and lithium hydroxide monohydrate are in agreement with the previously reported works in the literature, in which the Raman active modes of these molecules were first identified and assigned. However, due to the stability and resolution of the detection system used in this work, isotopic shifts with a magnitude less than one wavenumber have been identified. Principal Component Regression was used to evaluate the sensitivity to isotopic content of small Raman peak shifts in Li 2 CO 3 and indicates differences greater than 2 atom-% could be reliably determined. These measurements add to the body of work on lithium isotope Raman spectroscopy for these two compounds and increases the number of Raman bands which could be used for lithium isotope content analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Effects of surface treatments on ABS mechanical properties from fused filament fabrication

This paper examines the influence of surface treatments on the mechanical properties of acrylonitrile butadiene styrene (ABS) samples printed by fused filament fabrication (FFF). Prior efforts have applied brushing, painting, solvent dipping, infiltration, and vapor smoothing as post-processing surface treatments to improve the mechanical properties of FFF components. Additionally, because FFF can produce components with undesirable surface roughness, mechanical abrasion, epoxy coating, and acetone treatment may increase tensile strength by decreasing stress concentrations. Ridged surface texture may provide desirable tribological or handling properties. Based on these opportunities, this paper investigates abrasive media blasting, epoxy coating, acetone immersion, and ridged texturing surface treatments on the tensile strength and other mechanical properties of FFF ABS samples. ASTM D638-14 Type-I samples were printed, treated on all sample sides, and tested. From tensile tests, the elastic modulus, tensile strength, and fracture strain for both the untreated and treated ABS samples were calculated. For each sample, the surface finish and fracture macromorphology were observed with optical microscopy and the roughness values for the surface finish were calculated from profilometer data. Furthermore, samples were submerged in water and weighed periodically to measure mass changes due to water absorption. From surface profilometry and optical miscopy data, mechanical media blasting, epoxy coating, and immersion in all concentrations of acetone decreased surface roughness. Overall, on average, grit blasting with large beads and epoxy coating led to 2.6% and 1.2% increases in tensile strength, respectively; immersion in 40% acetone led to a 1.9% increase in tensile strength while treatment in 60% and 80% acetone decreased tensile strength by 4.9% and 1.9%, respectively. The study concludes that only grit blasting with large beads, immersion in 60% acetone, and the ridged texture significantly affected the tensile strength.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump–probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump–probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Development of High-Temperature Bonding Techniques to Enable High-Temperature Static or Dynamic Strain Measurements

Current light-water nuclear reactors rely on a variety of different sensors and sensor applications to meet their structural health monitoring needs throughout the entirety of the reactor primary, secondary, and containment systems. Optical fiber–based sensor technologies could provide solutions to reduce the sensor system footprint while enhancing the measurement fidelity and spatial resolution by leveraging distributed monitoring techniques. Moreover, advanced reactors may require optical fiber–based sensors for structural health monitoring because their operating temperatures will exceed the limits of conventional transducers used to acquire dynamic strain or acoustic data in nuclear power plants. Therefore, this report describes experiments targeting the development of high-temperature bonding techniques that would allow for potentially long lengths of fibers to be bonded to metallic reactor components in advanced reactor systems. The high temperatures experienced within target application, next-generation nuclear reactors, necessitate a high-temperature resistant bond to limit the amount of tension on the fiber at the target application temperature. The primary bonding method investigated in this work is brazing; hot-rolling has also been investigated to a lesser extent. Both techniques are well-suited to bonding optical fibers to large reactor components such as primary coolant piping, pressure vessels, or heat exchangers. Optical frequency domain reflectometry was used to monitor the strain in metal-coated optical fibers before, during, and after the high-temperature bonding process. On select optical fibers that were successfully bonded, additional thermal cycling was performed to assess the extent to which the fiber remained bonded based on the expected thermal expansion of the test specimen material. The results of the various experiments yielded the following general conclusions: (1) brazing is a viable technique for bonding and allows significant compressive strain to be applied to the fiber at room temperature; (2) hot-rolling is a viable technique as well, which has been more optimized than the brazing technique for bonding, but less residual compressive strain has been observed with this technique; and (3) both techniques will need further development and optimization to demonstrate bonding of a long length of fiber that can provably operate at relevant temperatures for an advanced nuclear reactor application.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Progress toward picosecond on-chip magnetic memory

Here, we offer a perspective on the prospects of ultrafast spintronics and opto-magnetism as a pathway to high-performance, energy-efficient, and non-volatile embedded memory in digital integrated circuit applications. Conventional spintronic devices, such as spin-transfer-torque magnetic-resistive random-access memory (STT-MRAM) and spin–orbit torque MRAM, are promising due to their non-volatility, energy-efficiency, and high endurance. STT-MRAMs are now entering into the commercial market; however, they are limited in write speed to the nanosecond timescale. Improvement in the write speed of spintronic devices can significantly increase their usefulness as viable alternatives to the existing CMOS-based devices. In this article, we discuss recent studies that advance the field of ultrafast spintronics and opto-magnetism. An optimized ferromagnet–ferrimagnet exchange-coupled magnetic stack, which can serve as the free layer of a magnetic tunnel junction (MTJ), can be optically switched in as fast as ~3 ps. Integration of ultrafast magnetic switching of a similar stack into an MTJ device has enabled electrical readout of the switched state using a relatively larger tunneling magnetoresistance ratio. Purely electronic ultrafast spin–orbit torque induced switching of a ferromagnet has been demonstrated using ~6 ps long charge current pulses. We conclude our Perspective by discussing some of the challenges that remain to be addressed to accelerate ultrafast spintronics technologies toward practical implementation in high-performance digital information processing systems.

42 ENGINEERING↗

DOE OSTI2025

Operando XPS in reactive plasmas: The importance of the wall reactions

In this article, advancements in differential pumping and electron optics over the past few decades have enabled x-ray photoelectron spectroscopy (XPS) measurements at (near-)ambient pressures, bridging the pressure gap for characterizing realistic sample chemistries. Recently, we have demonstrated the capabilities of an ambient pressure XPS setup for in situ plasma environment measurements, allowing plasma-surface interactions to be studied in operando rather than using the traditional before-and-after analysis approach. This new “plasma-XPS” technique facilitates the identification of reaction intermediates critical for understanding plasma-assisted surface processes relevant to semiconductor nanomanufacturing, such as physical vapor deposition, etching, atomic layer deposition, and many other plasma applications. In this paper, we apply the plasma-XPS approach to monitor real-time surface chemical changes on a model Ag(111) single crystal exposed to oxidizing and reducing plasmas. We correlate surface-sensitive data with concurrent gas-phase XPS measurements and residual gas mass-spectrum analysis of species generated during plasma exposure, highlighting the significant role of plasma-induced chamber wall reactions. Ultimately, we demonstrate that plasma-XPS provides comprehensive insights into both surface and gas-phase chemistry, establishing it as a versatile and dynamic characterization tool with broad applications in microelectronics research. Finally, we outline potential enhancements and future metrology directions to advance plasma-XPS investigations further.

36 MATERIALS SCIENCE↗

DOE OSTI2025

The Atacama Cosmology Telescope: DR6 power spectrum foreground model and validation

We discuss the model of astrophysical emission at millimeter wavelengths used to characterize foregrounds in the multi-frequency power spectra of the Atacama Cosmology Telescope (ACT) Data Release 6 (DR6), expanding on Louis et al. (2025) (2503.14452). We detail several tests to validate the capability of the DR6 parametric foreground model to describe current observations and complex simulations, and show that cosmological parameter constraints are robust against model extensions and variations. We demonstrate consistency of the model with pre-DR6 ACT data and observations from Planck and the South Pole Telescope. We evaluate the implications of using different foreground templates and extending the model with new components and/or free parameters. In all scenarios, the DR6 ΛCDM and ΛCDM+N eff cosmological parameters shift by less than 0.5σ relative to the baseline constraints. Some foreground parameters shift more; we estimate their systematic uncertainties associated with modeling choices. From our constraint on the kinematic Sunyaev-Zel'dovich power, we obtain a conservative limit on the duration of reionization of Δz rei < 4.4, assuming a reionization midpoint consistent with optical depth measurements and a minimal low-redshift contribution, with varying assumptions for this component leading to tighter limits. Finally, we analyze realistic non-Gaussian, correlated microwave sky simulations containing Galactic and extragalactic foreground fields, built independently of the DR6 parametric foreground model. Processing these simulations through the DR6 power spectrum and likelihood pipeline, we recover the input cosmological parameters of the underlying cosmic microwave background field, a new demonstration for small-scale CMB analysis. These tests validate the robustness of the ACT DR6 foreground model and cosmological parameter constraints.

CMBR experiments↗

DOE OSTI2023

Student Travel Support for the Inaugural Gordon Research Seminar on Multiphoton Processes (Final Technical Report)

This project provided financial support for early-career participants of the 2022 Gordon Research Seminar (GRS) on Multiphoton Processes, which was held on June 11 & 12, 2022 in Smithfield, Rhode Island, in conjunction with the Gordon Research Conference (GRC) on the same topic, held on June 12-17, 2022 in the same location. The GRC on Multiphoton Processes is an established conference series in the field of Atomic, Molecular and Optical (AMO) Physics with intense lasers. It regularly attracts around one hundred fifty researchers from around the world to present and discuss their forefront research featuring light-matter interaction in a variety of systems, ranging from atoms and molecules to nanosystems. In order to increase the attendance of early-career researchers at the GRC, in particular graduate students, post-docs, and other scientists with comparable levels of experience and education, the general assembly of the GRC on Multiphoton Processes decided during their last session in 2018 to organize a Gordon Research Seminar in conjunction with the next conference and organized and attended by early-career researchers. The GRS's primary intent is to provide a forum to graduate students and post-docs working in the field of intense and ultrafast AMO physics to present and exchange new data and cutting-edge ideas and to network with their peers at other research institutions around the U.S. and the world.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2024

Statistical Complexity of Quantum Learning

Abstract Learning problems involve settings in which an algorithm has to make decisions based on data, and possibly side information such as expert knowledge. This study has two main goals. First, it reviews and generalizes different results on the data and model complexity of quantum learning, where the data and/or the algorithm can be quantum, focusing on information‐theoretic techniques. Second, it introduces the notion of copy complexity, which quantifies the number of copies of a quantum state required to achieve a target accuracy level. Copy complexity arises from the destructive nature of quantum measurements, which irreversibly alter the state to be processed, limiting the information that can be extracted about quantum data. As a result, empirical risk minimization is generally inapplicable. The paper presents novel results on the copy complexity for both training and testing. To make the paper self‐contained and approachable by different research communities, an extensive background material is provided on classical results from statistical learning theory, as well as on the distinguishability of quantum states. Throughout, the differences between quantum and classical learning are highlighted by addressing both supervised and unsupervised learning, and extensive pointers are provided to the literature.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2025

Tree-level carbon stock estimations across diverse species using multi-source remote sensing integration

Forests are critical carbon sinks, and remote sensing has been increasingly widely used for forest monitoring and biomass estimations. However, species-specific tree-level studies remain limited. In this study, we demonstrated the feasibility of integrating UAV-based LiDAR with high-resolution optical satellite imagery (0.5 m) to estimate biomass for individual trees across different species. The proposed method accurately estimated biomass for 53 trees (R² = 0.82, rRMSE = 0.44), with species-specific datasets, showing an average 25.2% increase in R² and a 14.8% reduction in rRMSE. A novel vegetation index combining forest structure parameters with vegetation indices (VIs) was developed using high-resolution multispectral satellite data (3 m) to explore its relationship with individual tree biomass. Combining forest structural parameters with VIs further improved estimation accuracy, achieving an R²of 0.89 and an rRMSE of 0.34. Species-specific datasets show an 11.6% increase in R²compared to methods without VIs, and a 22.2% improvement over methods using only VIs. SHapley Additive exPlanations (SHAP) analysis shows that the volume feature played a key role in model performance and remained stable throughout the training process. Altogether, the proposed approach enhances individual tree biomass and carbon sink estimations, showing great potential for large-scale precise forest carbon monitoring using multi-source remote sensing data.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

NanoPSD: A software for automatic detection of Nano-Particle Shape Distribution in electron microscopy images

Accurate quantification of the size and morphology of nanoparticles from electron microscopy (EM) images is essential to understand growth mechanisms, surface reactivity, and functional behavior in nanoscale materials. Manual analysis remains slow, subjective, and difficult to reproduce in large datasets. We introduce NanoPSD (Nano-Particle Shape Distribution), an open-source and fully automated framework for quantitative particle detection and morphology analysis from EM images. NanoPSD integrates adaptive contrast enhancement, polarity-agnostic scale-bar detection, Optical Character Recognition (OCR)-based calibration, and classical segmentation via Otsu thresholding with morphological refinement. Particle contours are used to extract geometric descriptors, including equivalent circular diameter, aspect ratio, circularity, and solidity, enabling automated classification into spherical, rod-like, and aggregate morphologies. The framework supports both single-image and batch processing, generating publication-quality visualizations, LaTeX-ready tables, and structured comma-separated values (CSV) datasets. As a demonstration, we applied NanoPSD to plasma-synthesized nanoparticle samples diagnosed via transmission electron microscopy (TEM). The code produced statistically robust size and morphology distributions spanning a few to tens of nanometers with minimal user supervision. The pipeline demonstrates high reproducibility and scalability, processing large image collections with consistent calibration and output formatting. Its modular design enables seamless integration of future deep-learning-based segmentation models, providing a pathway toward intelligent, data-driven electron microscopy analysis.

36 MATERIALS SCIENCE↗

DOE OSTI2022

High temporal resolution estimates of Arctic snowfall rates emphasizing gauge and radar-based retrievals from the MOSAiC expedition

This article presents the results of snowfall rate and accumulation estimates from a vertically pointing 35-GHz radar and other sensors deployed during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. The radar-based retrievals are the most consistent in terms of data availability and are largely immune to blowing snow. The total liquid-equivalent accumulation during the snow accumulation season is around 110 mm, with more abundant precipitation during spring months. About half of the total accumulation came from weak snowfall with rates less than approximately 0.2 mmh–1. The total snowfall estimates from a Vaisala optical sensor aboard the icebreaker are similar to those from radar retrievals, though their daily and monthly accumulations and instantaneous rates varied significantly. Compared to radar retrievals and the icebreaker optical sensor data, measurements from an identical optical sensor at an ice camp are biased high. Blowing snow effects, in part, explain differences. Weighing gauge measurements significantly overestimate snowfall during February–April 2020 as compared to other sensors and are not well suited for estimating instantaneous snowfall rates. The icebreaker optical disdrometer estimates of snowfall rates are, on average, relatively little biased compared to radar retrievals when raw particle counts are available and appropriate snowflake mass-size relations are used. These counts, however, are not available during periods that produced more than a third of the total snowfall. While there are uncertainties in the radar-based retrievals due to the choice of reflectivity-snowfall rate relations, the major error contributor is the uncertainty in the radar absolute calibration. The MOSAiC radar calibration is evaluated using comparisons with other radars and liquid water cloud–drizzle processes observed during summer. Overall, this study describes a consistent, radar-based snowfall rate product for MOSAiC that provides significant insight into Central Arctic snowfall and can be used for many other purposes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Dry in-pile fracture test (DRIFT) for separate-effects validation of ceramic fuel fracture models

Fracture is an important component of nuclear fuel behavior, and significant efforts have been invested into developing fuel performance models that are capable of accurately representing fracture. Usable data on the process of fracture propagation in nuclear fuel under realistic service conditions are very limited. To address this need, a series of separate-effects experiments were developed and performed at Idaho National Laboratory's Transient Reactor Test (TREAT) facility. These experiments employ a heat sink to radially remove heat from the fuel in a manner that approximates the effect of coolant in an operating light-water reactor (LWR). The test holder for these experiments is known as the Dry In-pile Fracture Test (DRIFT). A series of experiments employing DRIFT and TREAT were performed to provide data on the extent and nature of fracture in fresh fuel at various points during a ramp to full power. Novel aspects of these experiments include the way they employ a heat sink to replicate steady-state LWR conditions, as well as the use of fiber optic sensors for in-reactor thermal instrumentation. Details on the development of this experiment, experimental conditions, and resulting data (including in situ thermal measurements and post-irradiation imaging of fracture) are provided in this work. LWR-equivalent powers ranging from 10 to 25 kW/m were tested using this apparatus. Cracking was visible at all power levels, with increasing cracking extent as the power level increased, although there was little difference in the cracking between the two highest-power tests, which had LWR-equivalent powers of 20 and 25 kW/m.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Bayesian Optimization of a Free-Electron Laser

The Linac Coherent Light Source X-ray free-electron laser is a complex scienti c apparatus which changes con gurations multiple times per day, necessitating fast tuning strategies to reduce setup time for successive experiments. To this end, we employ a Bayesian approach to maximizing X- ray laser pulse energy by controlling groups of quadrupole magnets. A Gaussian process model provides probabilistic predictions for the machine response with respect to control parameters, enabling a balance of exploration and exploitation in the search for the global optimum. We show that the model parameters can be learned from archived scans, and correlations between devices can be extracted from the beam transport. Furthermore, the result is a sample-e cient optimization routine, combining both historical data and knowledge of accelerator physics to signi cantly outperform existing optimizers.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Bayesian tomography of high-dimensional on-chip biphoton frequency combs with randomized measurements

Abstract Owing in large part to the advent of integrated biphoton frequency combs, recent years have witnessed increased attention to quantum information processing in the frequency domain for its inherent high dimensionality and entanglement compatible with fiber-optic networks. Quantum state tomography of such states, however, has required complex and precise engineering of active frequency mixing operations, which are difficult to scale. To address these limitations, we propose a solution that employs a pulse shaper and electro-optic phase modulator to perform random operations instead of mixing in a prescribed manner. We successfully verify the entanglement and reconstruct the full density matrix of biphoton frequency combs generated from an on-chip Si 3 N 4 microring resonator in up to an 8 × 8-dimensional two-qudit Hilbert space, the highest dimension to date for frequency bins. More generally, our employed Bayesian statistical model can be tailored to a variety of quantum systems with restricted measurement capabilities, forming an opportunistic tomographic framework that utilizes all available data in an optimal way.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Hyperspectral Light Sheet Raman Imaging of Leaf Metabolism (Final Report)

This final technical report details the accomplishment and findings of a project that developed technology related to imaging metabolic processes in plants. The report gives technical details of the design, construction and characterization of a Raman microscope system capable of identifying chemical species using the wavelength shifts of scattered excitation light. Some of the unique aspects of the design include: use of a Bessel beam excitation source, which allow long excitation lines that are resistant to scattering in complex media such as plants; excitation at 785 nm to avoid fluorescence emission that can occur in photosynthetic organisms; and a flat optical design that makes construction and alignment significantly simpler. This project also used stable isotope labeling to look at photorespiratory flux in the leaves of three different types of plants that have different photosynthesis pathways. Gas chromatography–mass spectrometry was used to look at which metabolites and amino acids had altered oxygen, carbon and hydrogen uptake under various conditions of environmental oxygen. This generated a rich data set that is being further analyzed to understand metabolic pathways in plants. This project also used the natural fluorescence in sorghum and rice to conduct an extensive experiment across different developmental stages. Spectral differences were identified at most of the developmental stages and these can be attributed to differential pigment and pigment-protein complexes present in different relative abundances as the plant develops.

09 BIOMASS FUELS↗

DOE OSTI2022

A super-resolution technique to analyze single-crystal inelastic neutron scattering measurements using direct-geometry chopper spectrometers

Direct-geometry time-of-flight chopper neutron spectroscopy is instrumental in studying dynamics in liquid, powder, and single crystal systems. We report here that real-space techniques in optical imagery can be adapted to obtain reciprocal-space super resolution dispersion for phonon or magnetic excitations from single-crystal neutron spectroscopy measurements. The procedure to reconstruct super-resolution energy dispersion of excitations relies on an accurate determination of the momentum and energy-dependent point spread function and a dispersion correction technique inspired by an image disparity calculation technique commonly used in stereo imaging. Here by, applying these methods to spinwave dispersion data from a virtual neutron experiment demonstrates ~5-fold improvement over nominal energy resolution.

47 OTHER INSTRUMENTATION↗