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DOE OSTI2025

Characterization of Kariya ( Hildegardia barteri (Mast.) Kosterm) Seed Oil Fatty Acid Methyl Ester Prepared from Basic Catalytic Transesterification

The rising global energy demand, alongside concerns regarding environmental deterioration due to the use of fossil fuels, has spurred extensive investigation into renewable energy alternatives. Biomass-derived biodiesel, especially from lesser-known oil sources, emerges as a promising option. This research focuses on analyzing the fatty acid methyl esters (FAMEs) derived from Kariya (Hildegardia barteri (Mast.) Kosterm) seed oil through basic catalytic transesterification using gas chromatography–flame ionization detector (GC–FID) analysis, assessing its potential as a biodiesel feedstock. Oil extraction from Kariya seeds was carried out using three solvents (n-hexane, ethanol, and a 1:1 blend of hexane and ethanol), followed by transesterification with methanol. Gas chromatography–mass spectrometry (GC–MS) and GC–FID analyses were utilized to identify and quantify FAMEs in the resulting biodiesel. The results revealed various FAMEs, including methyl myristate, methyl palmitate, methyl stearate, methyl oleate, methyl linoleate, and methyl linolenate. Significant differences in FAME composition were observed among the samples, with hexane–ethanol Kariya oil biodiesel (HE-KOB) showing the highest FAME content (76.1%). This combination of solvents exhibited synergistic effects on the composition of HE-KOB, suggesting potential optimization strategies for biodiesel production. Fourier transform infrared spectroscopy (FTIR) provided additional insights into the molecular composition of the biodiesel samples, confirming their biodiesel nature through the identified functional groups such as methyl, methylene, hydrocarbon, ester, aldehyde, and alkene. Thermogravimetric analysis (TGA) for thermal decomposition also gave an insight into FAME composition and its contribution to the degree of conversion of biodiesel to energy. These findings highlight the feasibility of utilizing Kariya seed oil as a biodiesel feedstock, emphasizing the importance of solvent selection and transesterification conditions in optimizing FAME yield and composition. This research contributes to the exploration of underutilized oil sources for sustainable biodiesel production, aligning with the global shift towards cleaner and renewable energy sources.

09 BIOMASS FUELS↗

DOE OSTI2025

Enhancement of Uranium Ionization Efficiencies Using Zn-MOF-74 Derived Nanoporous Ion Emitters for Thermal Ionization Mass Spectrometry

The recent introduction of nano-porous ion emitters (nano-PIEs) formed from metal organic frameworks (MOFs) has demonstrated the potential to enhance sensitivity for thermal ionization mass spectrometry (TIMS). Nano-PIEs take advantage of the parent MOF’s chemical and structural tunability to form scaffolds for ion emitters. A study by Barpaga et al. 2023 on MOF-74 as the parent material found that with high volatility metals in their framework uranium sample utilization efficiency (SUE) increases by up to nine-fold (e.g., Zn-MOF-74) compared to that of the analyte on a bare filament (~0.05%). Here, in this study, we investigate the performance of Zn-MOF-74 to maximize uranium efficiencies at the trace level (= 10 -12 g) by altering the parent MOF morphology and chemistry (i.e., MOF crystal sizes and thermal degradation) and optimizing its integration with TIMS (i.e., MOF mass on a filament and ramp conditions). We observed improvement in SUE up to 20 times (≤1.0%) that of a bare filament load when nano-PIEs derived from nanocrystals of Zn-MOF-74 were heated under a specific current ramp condition. This demonstrates that rates of nano-PIE structural collapse during TIMS analysis and the subsequently formed nanomaterials (and their features) can be tuned to control analyte ionization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

In-situ hydrogen microstructural characterization of Si heterojunction passivation: Addressing V OC degradation and mitigation pathways

Si heterojunction (SHJ) solar cells have demonstrated record efficiency >27%, approaching the theoretical limit of ≈ 29%, primarily due to best surface/interface defect passivation provided by deposited thin layers of hydrogenated amorphous silicon (a-Si:H). Such excellent surface/interface passivation reduces recombination loss and result in >100 mV improvement of cell open circuit voltage (V OC ) to ≈ 750 mV, thus the cell efficiency. However, fielded SHJ modules exhibit loss of V OC and hence efficiency over time in years, presumably due to degradation related to a-Si:H layers. This adversely affects the technology’s market acceptance, and levelized cost of energy (LCOE). It is hypothesized that the origin of a-Si:H degradation is somehow related to the presence of weak Si–Si bonds and hydrogen in a-Si:H films. The objective of this project is to test this hypothesis by directly measuring chemical and structural changes occurring within SHJ component layers and solar cells. This is achieved by developing an innovative in-situ Fourier transform infrared (FTIR) spectrometry apparatus to monitor hydrogen microstructural changes occurring within amorphous silicon and decipher hydrogen evolution kinetics over time when samples are exposed to heat and/or light stress. These in-situ measured hydrogen microstructural changes are correlated to the changes in effective minority carrier lifetime (τ eff ), implied V OC (iV OC ), surface recombination velocity (S), and cell V OC . These mechanistic understandings will provide critical guidance to mitigate the V OC -driven degradation of SHJ solar cell performance. Passivation optimization and degradation analysis of individual SHJ component structures were achieved through systematic deposition of three symmetric structures and the completed SHJ solar cell structure. The three symmetric structures used were intrinsic a-Si:H [(i)a-Si:H] layers in a bilayer structure, intrinsic and p-type doped stacked layers [(i-p)a-Si:H] representing the front heterojunction in the SHJ cell, and intrinsic and n-typed doped stacked layers [(i-n)a-Si:H] representing the back-side back surface field (BSF) in the SHJ cell. State-of-the-art passivation qualities are demonstrated by a champion iV OC of 740 mV for the (i)a-Si:H layers, and the (i-n)a-Si:H symmetric structure. A 725 mV iV OC is observed for the (i-p)a-Si:H symmetric structure. These symmetric passivated SHJ component structures were subsequently subjected to different accelerated lifetime (ALT) stressors to identify which conditions contribute the most to iV OC degradation. Degradation of the thin (10 nm) (i)a-Si:H passivation layers without any additional overlying layers is minimal; complexity of this study arises due to unavoidable surface oxidation of (i)a-Si:H layer during most of the stress application, which is likely irrelevant for a full SHJ cell configuration with overlying protective layers. The iV OC degradation of symmetric structures is found to occur primarily at the (i-p)a-Si:H passivation stack under dark heat stress with associated hydrogen loss from the (p)a-Si:H layer. An activation energy for increase in S (defect creation) of 0.65 eV can be correlated to the activation energy of ≈ 0.4 eV for hydrogen loss from the (i-p)a-Si:H stack. This also suggests the presence of weakly bonded hydrogen in the (p)a-Si:H films, which effuses out of the film stack at such low activation energy. When light and heat stress are applied together, similar hydrogen loss from (i-p)a-Si:H stack is observed, however, does not appreciably degrade iV OC or increase S. This is an important result and departure from direct correlation between hydrogen loss and defect creation. This perhaps indicates additional defect chemistries or annealing that might be occurring in the presence of light requiring further detailed defect measurements. The full SHJ cell structure used for this project is depicted in Fig.1(d). SHJ cells with an initial V OC ≈ 700 mV were fabricated and subjected to similar ALT stress conditions. Cell V OC is found to degrade the most under dark heat stress and is confirmed by observed hydrogen migration out of the (i-p)a-Si:H stack. However, hydrogen cannot escape from the cell stack, it accumulates near the (p)a-Si:H/ITO contact interface, where ITO acts as a barrier preventing hydrogen loss. Furthermore, light-heat combined stress does not degrade V OC appreciably, confirming the occurrence of a defect annealing process.

14 SOLAR ENERGY↗

DOE OSTI2025

A variant of the MenB strain of Synechocystis sp. PCC 6803 disrupts a stress response pathway allowing DMPBQ to occupy the A 1 sites of photosystem I

Phylloquinone (PhQ) plays a unique role in photosynthesis as the A1A and A1B intermediates in light-driven electron transfer in Photosystem I (PSI). When PhQ biosynthesis is inhibited by deletion of the menB gene in the cyanobacterium Synechocystis sp. PCC 6803, previous studies have shown that plastoquinone-9 (PQ-9) occupies the A 1 sites. However, a recent cryo-electron microscopy structure of a strain of ΔmenB from the year 2023 revealed an unusual quinone in the A 1 sites with a benzoquinone headgroup similar to PQ-9 and a phytyl tail similar to PhQ. Here, we investigate its biosynthesis and binding properties. Mass spectrometry confirms that PSI from the 2023 ΔmenB strain contains 2,3-dimethyl-5-phytyl-1,4-benzoquinone (DMPBQ), while PSI from the original strain contains PQ-9. Whole genome sequencing reveals that a mutation in slr1737 (tocopherol cyclase) leads to the accumulation of DMPBQ, an intermediate in the tocopherol biosynthetic pathway. Transient optical and electron paramagnetic resonance spectroscopy studies show that when DMPBQ occupies the A 1 sites, it does not exchange with exogenously supplied PhQ in contrast to PQ-9, which exchanges readily. We propose that the slr1737 mutation in the 2023 ΔmenB strain is a likely candidate for the source of the phenotype. This new strain has sacrificed tocopherol synthesis, the absence of which is known to have no effect on growth under low stress conditions, resulting in incorporation of DMPBQ in the A 1 sites. The tighter binding and function of DMPBQ likely allow this ΔmenB strain to outcompete its peers under optimal growth conditions and thus dominate the population.

2,3-dimethyl-5-phytyl-1,4-benzoquinone↗

DOE OSTI2024

Untargeted Spatial Metabolomics and Spatial Proteomics on the Same Tissue Section

An increasing number of spatial multiomic workflows have been recently developed. Some of these approaches have leveraged initial mass spectrometry imaging (MSI)-based spatial metabolomics to inform region of interest (ROI) selection for downstream spatial proteomics. However, these workflows have been limited by varied substrate requirements between modalities or have required analyzing serial sections (i.e., one section per modality). To mitigate these issues, we present a novel multiomic workflow that uses desorption electrospray ionization (DESI)-MSI to identify representative spatial metabolite patterns on-tissue prior to spatial proteomic analyses on the same tissue section. Further, this workflow is demonstrated here with a model mammalian tissue (coronal rat brain section) mounted on a polyethylene naphthalate-membrane slide. Initial DESI-MSI resulted in 160 annotations (SwissLipids) within to the METASPACE platform (≤20% false discovery rate). A segmentation map from the annotated ion images informed downstream ROI selection for spatial proteomics characterization from the same sample. The unspecific substrate requirements and minimal sample disruption inherent to DESI-MSI allowed for an optimized, downstream spatial proteomics assay, resulting in 3888 ± 240 to 4717 ± 48 proteins being confidently directed per ROI (200 µm x 200 µm). Finally, we demonstrate the integration of multiomic information, where we found ceramide localization to be correlated with SMPD3 abundance (ceramide synthesis protein), and we also utilized protein abundance to resolve metabolite isomeric ambiguity. Overall, the integration of DESI-MSI into the multiomic workflow allows for complementary spatial and molecular-level information to be achieved from optimized implementations of each MS assay inherent to the workflow itself.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

mzPeak: Designing a Scalable, Interoperable, and Future-Ready Mass Spectrometry Data Format

Advances in mass spectrometry (MS) instrumentation, such as higher resolution, faster scan speeds, and improved sensitivity, have significantly increased the volume and complexity of data. The growing adoption of imaging and ion mobility further amplifies these challenges across MS-based omics fields, including proteomics, metabolomics, and lipidomics. While these technologies unlock new possibilities, they also present significant challenges in data management, storage, and accessibility. Existing open formats, such as the XML-based community standards mzML and imzML, struggle to meet the demands of modern MS workflows due to their large file sizes, slow data access, and limited metadata support. Vendor-specific formats, while optimized for proprietary instruments, lack interoperability, comprehensive metadata support and long-term archival reliability. This white paper lays the groundwork for mzPeak, a next-generation community data format designed to address these challenges and support high-throughput, multi-dimensional MS workflows. By adopting a hybrid model that combines efficient binary storage for numerical data and both human and machine-readable metadata storage, mzPeak will reduce file sizes, accelerate data access, and offer a scalable, adaptable solution for evolving MS technologies. For researchers, mzPeak will enable enhanced interoperability across platforms, seamless support for complex workflows including ion mobility and MS imaging, and faster data access compared to existing community formats such as mzML. Its design will ensure data is managed in compliance with regulatory standards, essential for applications such as precision medicine and chemical safety, where long-term data integrity and accessibility are critical. For vendors, mzPeak provides a streamlined, open alternative to proprietary formats, reducing the burden of regulatory compliance while aligning with the industry's push for transparency and standardization. By offering a high-performance, interoperable solution, mzPeak positions vendors to meet customer demands for sustainable data management tools which will be able to handle emerging and future data types and workflows. mzPeak aspires to become the cornerstone of MS data management, empowering researchers, vendors, and developers to innovate and collaborate more effectively.

data formats↗

DOE OSTI2025

Hydrogen Production from Polyethylene Pyrolysis

Hydrogen is anticipated to play a pivotal role in the future of clean energy and decarbonization efforts, serving as an energy storage medium, a power generation source, and a clean fuel for transportation. While most hydrogen is produced from carbonaceous fossil feedstocks like natural gas, petroleum, and coal, there is growing interest in using refuse-derived fuels such as waste plastics and municipal solid waste (MSW) as alternative feedstocks. Thermochemical processes such as pyrolysis and catalytic cracking can convert nonrecyclable plastics and organic MSW components to produce hydrogen with lower life cycle greenhouse gas emissions when coupled with CO 2 capture. Such approaches not only address waste-management challenges but also reduce methane emissions from landfills. Furthermore, waste feedstocks are low cost and can support meeting demands for hydrogen across various industries. In this work we examined production of hydrogen from high-density polyethylene (HDPE) as a model polymer using pyrolysis. Analytical studies of pyrolysis utilizing gas chromatography–mass spectrometry (GC/MS) provide insights into conversion pathways for plastic waste, potentially reducing the environmental footprint of traditional hydrogen production methods. This work generates a baseline methodology for hydrogen production from plastic pyrolysis with and without a catalyst and the necessary product distribution baseline from key single plastics. The effect of pyrolysis temperature on the conversion of HDPE was evaluated both with and without a catalyst(s), and the product distributions measured via GC/MS were identified and hydrogen formation was quantified. These results will help guide future research efforts to optimize catalysts and processes for more efficient hydrogen production and mixed plastic waste management.

Catalysts↗

DOE OSTI2024

Oxide dissolution and oxygen diffusion scenarios in niobium and implications on the Bean–Livingston barrier in superconducting cavities

We generalize a native Nb2O5 dissolution model [G. Ciovati, Appl. Phys. Lett. 89, 022507 (2006)] to sequential overlayer dissolutions, multilayer dissolution, and realistic temperature profiles, which may be applicable to other materials. The model is applied to secondary ion mass spectrometry depth profile measurements for varying temperature profiles and two-step oxide dissolution in Nb and found to agree well. In the context of the Meissner screening response due to impurity profiles on the length scale of the London penetration depth, the shallow diffusion of O impurities results in a substantial decrease in the peak supercurrent density near the surface. In this framework, oxide dissolution and oxygen diffusion can account for a rise in peak supportable magnetic field in SRF cavities with baking time and a suppression after the optimal baking time is reached, in good agreement with peak-field baking temperatures and times as well as recent quench field measurements.

Lechner, Eric↗

DOE OSTI2024

Unsupervised Learning for Improved Gamma-Ray Spectrometry in Pixelated Cadmium Zinc Telluride (CZT) Detectors

Machine learning has been found to be ubiquitously useful across many industries, presenting an opportunity to improve radiation detection performance using data-driven algorithms. Improved detector resolution can aid in the detection, identification, and quantification of radionuclides. Here, in this work, a novel, data-driven, unsupervised learning approach is developed to improve detector spectral characteristics by learning, and subsequently rejecting, poorly performing regions of the pixelated detector. Feature engineering is used to fit individual characteristic photo peaks to a Doniach lineshape with a linear background model. Then, principal component analysis is used to learn a lower-dimension latent space representation of each photo peak where the pixels are clustered, and subsequently ranked, based on the cluster mean distance to an optimal point. Pixels within the worst cluster(s) are rejected to improve the full-width at half-maximum (FWHM) by 10% to 15% (relative to the bulk detector) at 50% net efficiency when applied to training data obtained from measurements of a 100 μCi 154 Eu source using a H3D M400i pixelated cadmium zinc telluride detector. These results compare well with, but do not outperform, a greedy algorithm that accumulates pixels in order of FWHM from lowest to highest used as a benchmark. In the future, this approach can be extended to include the detector energy and angular response. Finally, the model is applied to newly seen natural and enriched uranium spectra relevant for nuclear safeguards applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2026

Hydrogen Analysis by Gas Chromatography–Mass Spectrometry

The detection of hydrogen in complex gas mixtures is essential for many applications. Conventional approaches such as gas chromatography (GC) with thermal conductivity detection (TCD) and residual gas analyzers (RGAs) face significant limitations: TCD exhibits poor response when helium is used as a carrier gas, whereas RGAs lack chromatographic separation, preventing reliable quantification of hydrogen because of interference from other species. Traditional GC methods rely on dual-column configurations with packed or molecular-sieve porous layer open tubular (PLOT) columns to separate hydrogen from O2, N2, CO, CO2, CH4, and other hydrocarbons, increasing system complexity and limiting compatibility with mass spectrometry (MS) detection. In this work, we developed and validated a robust GC–MS method capable of directly detecting and quantifying hydrogen using electron ionization (EI) without dopants, reagent gases, or ion–molecule reaction schemes. By integrating a modified EI source and a cryogenically cooled single capillary column configuration, we achieved baseline separation of hydrogen from all major permanent gases and hydrocarbons in a refinery gas mixture using helium as the carrier gas. The method demonstrated excellent linearity, high sensitivity, and exceptional reproducibility. Adjustable sample-loop volumes and split ratios enabled optimization of peak shape and signal-to-noise performance for trace-level and percent-level hydrogen concentrations. Beyond hydrogen quantitation, the method provides simultaneous compositional profiling of other gases in a mixture in a single run, making it valuable for a wide range of tasks.

Lobodin, Vlad [ORNL]↗

DOE OSTI2025

Efficient and Selective Chemical Transformations in Highly Charged and Confined Nanodroplets

The acceleration of chemical reaction rates and the increased product selectivity in microdroplets compared to that in bulk solutions has become a topic of increasing interest that has been extensively characterized by electrospray ionization mass spectrometry (ESI-MS). However, the sources of this acceleration and the detailed relationships between droplet properties and resulting reaction rate acceleration are still under debate. Moreover, droplet properties are governed by multiple interrelated experimental parameters, i.e., electrospray voltage, solution flow rate, etc., which makes it difficult and time-consuming to explore this diverse parameter space using traditional manual experimental or computational approaches. In this work, we developed an automated experimental platform integrating reactions in controlled charged microdroplet environments with ESI-MS characterization and sequential hybrid Bayesian modeling, as well as an optimal experimental design framework, to achieve multidimensional parameter optimization for higher reaction turnover rates, based on a model reaction of tetraethylenepentamine (TEPA) with carbon dioxide. With the current platform, we have achieved automated scans with a range of electrospray voltages and solution flow rates, and determined and optimized parameter settings to achieve increased reaction turnovers. We have also linked this platform to the underlying properties of droplets via a hybrid model incorporating physics, high-level theoretical calculations, and machine learning (ML) approaches. The autonomous platform is broadly applicable to a range of chemical reactions relevant to DOE’s mission in chemical separations, catalysis, and materials synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Defining the Antitumor Mechanism of Action of a Clinical-stage Compound as a Selective Degrader of the Nuclear Pore Complex

Cancer cells are acutely dependent on nuclear transport due to elevated transcriptional activity, suggesting an unrealized opportunity for selective therapeutic inhibition of the nuclear pore complex (NPC). Through large-scale phenotypic profiling of cancer cell lines, genome-scale functional genomic modifier screens, and mass spectrometry–based proteomics, we discovered that the clinical drug PRLX-93936 is a molecular glue that binds and reprograms the TRIM21 ubiquitin ligase to degrade the NPC. Upon compound-induced TRIM21 recruitment, the nuclear pore is ubiquitylated and degraded, resulting in the loss of short-lived cytoplasmic mRNA transcripts and the induction of cancer cell apoptosis. Direct compound binding to TRIM21 was confirmed via surface plasmon resonance and X-ray crystallography, whereas compound-induced TRIM21–nucleoporin complex formation was demonstrated through multiple orthogonal approaches in cells and in vitro. Phenotype-guided optimization yielded compounds with 10-fold greater potency and drug-like properties, along with robust pharmacokinetics and efficacy against pancreatic cancer xenografts and patient-derived organoids.

Yuan, Linjie [Stanford School of Medicine, CA (Uni↗

DOE OSTI2024

Oxygen redox activities governing high-voltage charging reversibility of Ni-rich layered cathodes

A schematic illustration indicative of the improved structural reversibility through stabilizing oxidized oxygen by Al doping. The chemical reactions and phase transitions at high voltages are generally considered to determine the electrochemical properties of high-voltage layered cathodes such as Ni-rich rhombohedral oxides. Even if significantly higher SOCs (states-of-charge) are utilized above the capability of transition metal redox (primarily Ni and Co), the effect of oxygen redox on Ni-rich rhombohedral oxides still looks mysterious thereby necessitating research that can clarify the relationship between redox reactions and phase transitions. Here, we performed a comprehensive and comparative study of the cationic and anionic redox reactions, as well as the structural evolution of a series of commercial Ni-rich layered oxides with and without Al doping. We combined the results from X-ray spectroscopy, operando electrochemical mass spectrometry, and neutron diffraction with electrochemical properties and thereby revealed the different oxygen redox activities associated with structural and electrochemical degradations. We reveal that Al doping suppresses the irreversible oxygen release but enhances the lattice oxygen oxidization. With this modulated oxygen redox activity, the Ni-rich layered oxides’ notorious H2–H3 structural phase transition becomes highly reversible. Our findings disentangle the different oxygen redox activities during high-voltage cycling and clarify the role of dopants in the Ni-rich layered oxides in terms of structural and electrochemical stability, shedding light on the future direction of optimizing layered cathode materials for safer high energy-density secondary batteries.

Lee, Gi-Hyeok↗

DOE OSTI2025

Detection of Br and I as atomic anions using liquid sampling – atmospheric pressure glow discharge/Orbitrap mass spectrometry

The quantification and determination of halogen isotope composition is essential in many fields including geochemistry and nuclear forensics. Detection of the halogen elements is commonly attempted with inductively coupled plasma mass spectrometry (ICP-MS) however, there are multiple challenges faced. Most significantly this includes very poor ionization efficiency and the potential for isobaric interferences from either matrix or plasma species. Thus, sensitivity and accuracy are often limiting issues. Here a liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source is coupled with an ultrahigh resolution Orbitrap MS to perform halogen detection of bromine and iodine as initial analytes. This facilitates simple and sensitive detection of these elements as atomic anions from simple aqueous salt solutions. Collision-induced dissociation (CID) and higher-energy collisional dissociation (HCD) energies were optimized to produce the maximum response of Br − and I − . The LS-APGD conditions were optimized using a design of experiments (DOE) approach for Br − and I − concurrently. Response curves for Br − and I − solutions determined limit of detection (LOD) values of 50 pg and 5 pg, respectively, in 20 μL aliquots. The curves indicated response factors of 0.67 for 79 Br − and 0.90 for 127 I − . Br isotope ratios were determined with precision between 0.7 and 7.3% RSD, with the isotope ratios determined with precision 0.8% RSD at concentrations above the limit of quantification. Preliminary tests were conducted to evaluate the effect of different cations (Na + , K + , and Mg 2+ ) on Br − responses, with no discernible impacts observed on the halogen signal responses. This study demonstrates the potential use of the LS-APGD-Orbitrap-MS for the detection of multiple halogens while avoiding interferences, minimizing sample preparation, and overcoming ionization barriers.

Lang, Dehlia A. [Clemson University, SC (United St↗

DOE OSTI2024

Parametric optimization of the liquid sampling-atmospheric pressure glow discharge ionization source coupled to an Orbitrap mass spectrometer for neodymium isotope ratio determinations

Isotope ratio determinations are a valuable tool in several application areas. In nuclear forensics, the isotope ratios of uranium and plutonium are commonly used as a signature for the nuclear material's provenance and processing history. However, signatures from other coexisting elements, such as neodymium and samarium, can offer additional insights. Here, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source coupled to an Orbitrap mass spectrometer (MS) has demonstrated its utility for actinide measurements. This instrumental platform can leverage the high resolution offered by the Orbitrap MS to overcome potential isobaric interferences, such as 144 Nd- 144 Sm, 148 Nd- 148 Sm, and 150 Nd- 150 Sm pairs. The work presented herein demonstrates the rapid, accurate, and precise determination of the isotope ratios for neodymium using the LS-APGD/Orbitrap MS. Both the LS-APGD and Orbitrap MS parameters were optimized systematically, with NdO + found to be the most abundant, most reduced species after applying the optimal collision-induced dissociation modalities. A limit of detection of 3 pg of 142 Nd was achieved when data was acquired and processed using the FTMS Booster, an external data acquisition and processing system offered by Spectroswiss. Excellent accuracy of better than 99 % and precision of <1 % RSD were achieved when a solution of the well-characterized neodymium standard (JNdi-1 standard) was analyzed under the optimized condition, indicating the LS-APGD/Orbitrap's great potential for isotope ratio analysis of Nd and other REEs for diverse applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Imaging and spatially resolved mass spectrometry applications in nephrology

The application of spatially resolved mass spectrometry (MS) and MS imaging approaches for studying biomolecular processes in the kidney is rapidly growing. These powerful methods, which enable label-free and multiplexed detection of many molecular classes across omics domains (including metabolites, drugs, proteins and protein post-translational modifications), are beginning to reveal new molecular insights related to kidney health and disease. Further, the complexity of the kidney often necessitates multiple scales of analysis for interrogating biofluids, whole organs, functional tissue units, single cells and subcellular compartments. Various MS methods can generate omics data across these spatial domains and facilitate both basic science and pathological assessment of the kidney. Optimal processes related to sample preparation and handling for different MS applications are rapidly evolving. Emerging technology and methods, improvement of spatial resolution, broader molecular characterization, multimodal and multiomics approaches and the use of machine learning and artificial intelligence approaches promise to make these applications even more valuable in the field of nephology. Overall, spatially resolved MS and MS imaging methods have the potential to fill much of the omics gap in systems biology analysis of the kidney and provide functional outputs that cannot be obtained using genomics and transcriptomic methods.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2026

How exudates production along a phosphorus gradient influences mineral dissolution across contrasting soil development stages

Harnessing rhizosphere processes offers a valuable opportunity to optimize nutrient use efficiency in agroecosystems. In nutrient-limited soils, plants discharge part of photosynthate surplus via root exudation, including carboxylates, which may enhance mineral dissolution and nutrient mobilization. We aimed to assess how plant responses to nutrient limitation translated into changes in exudate profiles, and how these exudates, in turn, drive bioweathering processes across soils of contrasting mineralogy and weathering degree. We conducted a hydroponic experiment with Lupinus albus grown under five phosphorus (P) concentrations (5, 10, 20, 30, and 50 µM) over seven weeks. We measured plant biomass and root traits, performed a metabolomics analysis and quantified seven carboxylates in root exudates using gas chromatography-mass spectrometry. To assess bioweathering processes across contrasted soil domains, we conducted batch dissolution tests with exudates using three soil horizons—35 each with distinct physicochemical properties: enriched in organic matter, iron oxides, or primary silicates. At the intermediate level of P supply, shoot biomass was comparable to that under high P, but plants produced more root biomass and a higher total carboxylate exudation rate. Despite low carboxylate concentrations (<100 ppb), exudates promoted the dissolution of Ca, Mg, Si, Fe, P and K in all horizons. Yet, the degree of element released varied among horizons. These findings highlight the importance of root exudates in enhancing mineral dissolution, with effects dependent on soil physicochemical properties. The results suggest that managing agroecosystems under moderate nutrient limitation could be a sustainable strategy to increase root-to-shoot ratios, enhance bioweathering processes and nutrient release in soil solution.

Pollet, Sasha L.↗

DOE OSTI2025

Chemical Analysis of Tantalum Thin Films compared to Niobium Thin Films using SIMS and XPS

Superconducting qubits are a leading platform for quantum computation. These circuits are typically made from superconducting materials like aluminum or niobium. However, the amorphous niobium oxide and aluminum oxide on the surface of these circuits introduce considerable RF loss due to the presence of two-level systems (TLS), which limits the maximum coherence times T1 to ~100 μs. Capping the niobium qubits with a tantalum layer leads to a 3- 5x improvement [Bal et al., 2024]. But even in this case, tantalum forms an amorphous surface oxide that introduces loss. In an effort to devise strategies to eliminate the presence of this oxide, we present a comprehensive study on the nature of Ta oxide using x-ray photoemission spectroscopy (XPS) and secondary ion mass spectrometry (ToF-SIMS) as a function of heat treatment. The thin films were annealed in ultra-high vacuum conditions and analyzed in situ to characterize the composition and evolution of the native tantalum oxide layer and oxide-metal interface. Our analysis reveals two critical differences between tantalum and niobium oxides: Nb2O5 completely dissolves at 400°C, while Ta2O5 persists even at 800°C. Additionally, tantalum oxide contains only a single suboxide (TaO), in contrast to niobium's two suboxides (NbO and NbO2). The suboxide of tantalum contributes minimally to the total oxide content and shows a relative increase with temperature. Understanding the oxide’s behavior will open new pathways for optimizing coherence times in tantalum qubits.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗