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At least 1,243 records · Page 69

Baseflow Identification via Explainable AI With Kolmogorov‐Arnold Networks

Abstract Hydrological models often involve constitutive laws that may not be optimal in every application. We propose to replace such laws with the Kolmogorov‐Arnold networks (KANs), a class of neural networks designed to identify symbolic expressions. We demonstrate KAN's potential on the problem of baseflow identification, a notoriously challenging task plagued by significant uncertainty. KAN‐derived functional dependencies of the baseflow components on the aridity index outperform their original counterparts; they demonstrate that water availability, rather than potential evapotranspiration, drives baseflow by constraining actual evapotranspiration under arid conditions. On a test set, they increase the Nash‐Sutcliffe efficiency (NSE) by 65%, decrease the root mean squared error by 29%, and increase the Kling‐Gupta efficiency by 34%. This superior performance is achieved while reducing the number of fitting parameters from three to two. Next, we use data from 378 catchments across the continental United States to refine the water‐balance equation at the mean‐annual scale. The KAN‐derived equations based on the refined water balance outperform both the current aridity index model, with up to a 105% increase in NSE, and the KAN‐derived equations based on the original water balance. While the performance of our model and tree‐based machine learning methods is similar, KANs offer the advantage of simplicity and transparency and require no specific software or computational tools. This case study focuses on the aridity index formulation, but the approach is flexible and transferable to other hydrological processes. Plain Language Summary Equations used in hydrologic model are often suboptimal, resulting in reduced prediction accuracy and efficiency. We implemented Kolmogorov‐Arnold networks (KAN), a machine learning algorithm for deriving symbolic formulations, to estimate groundwater recharge and showed that it outperforms an existing state‐of‐the‐art semi‐empirical formulation. In hydrology, Nash‐Sutcliffe efficiency (NSE), root mean squared error (RMSE), and Kling‐Gupta efficiency (KGE) are commonly used to evaluate model performance. Higher NSE and KGE values indicate better performance, while lower RMSE values are preferable. Our results show that NSE increased by 71%, RMSE decreased by 32%, and KGE improved by 25%. In addition, KAN identifies an optimal functional form and can be used to derive new analytical formulas using the prior knowledge. The KAN‐inspired equation outperformed the original formulation and reduced the fitting parameters. Furthermore, we refined the water‐balance equation at the mean‐annual scale and showed that, based on the new water‐balance equation, KAN can derive new formulations that are superior to the original aridity index formulations (up to 105% increase in NSE) and KAN‐derived equations based on the original water balance. These findings highlight the significant potential of KAN to advance the scientific understanding of a wide range of hydrologic processes. Key Points Kolmogorov‐Arnold networks (KANs) enhance interpretability of machine‐learned hydrological models KAN‐derived symbolic formulations outperform state‐of‐the‐art semi‐empirical aridity indices KAN‐identified functional form yields an analytical index with fewer fitting parameters and improved performance

baseflow↗

Chemical versus physical pressure effects on the structure transition of bilayer nickelates

The observation of high-T c superconductivity (HTSC) in concomitant with pressure-induced orthorhombic-tetragonal structural transition in bilayer La 3 Ni 2 O 7 has sparked hopes of achieving HTSC by stabilizing the tetragonal phase at ambient pressure. Chemical pressure, introduced by replacing La 3+ with smaller rare-earth R 3+ has been considered as a potential route. However, our experimental and theoretical investigation reveals that such substitutions, despite causing lattice contraction, actually produce stronger orthorhombic distortions, requiring higher pressures for the structural transition. A linear extrapolation of P c versus the average size of A-site cations (<$r_A$>), yields a putative critical value of (<$r_A$>) ≈ 1.23 Å for P c ≈ 1 bar. The negative correlation between P c and (<$r_A$>) indicates that replacing La 3+ with smaller R 3+ ions is unlikely to reduce P c to ambient pressure. Instead, substituting La 3+ with larger cations like Sr 2+ or Ba 2+ might be a feasible approach. Our results provide guidance for realizing ambient-pressure HTSC in bilayer nickelates.

36 MATERIALS SCIENCE↗

The expression of genes encoding novel Sesame oleosin variants facilitates enhanced triacylglycerol accumulation in Arabidopsis leaves and seeds

Summary Triacylglycerols (TAG), accumulate within lipid droplets (LD), predominantly surrounded by OLEOSINs (OLE), that protect TAG from hydrolysis. We tested the hypothesis that identifying and removing degradation signals from OLE would promote its abundance, preventing TAG degradation and enhancing TAG accumulation. We tested whether mutating potential ubiquitin‐conjugation sites in a previously reported improved Sesamum indicum OLE ( SiO ) variant, o3‐3 Cys‐OLE ( SiCO herein), would stabilize it and increase its lipogenic potential. SiCOv1 was created by replacing all five lysines in SiCO with arginines. Separately, six cysteine residues within SiCO were deleted to create SiCOv2. SiCOv1 and SiCOv2 mutations were combined to create SiCOv3. Transient expression of SiCOv3 in Nicotiana benthamiana increased TAG by two‐fold relative to SiCO. Constitutive expression of SiCOv3 or SiCOv5 , containing the five predominant TAG‐increasing mutations from SiCOv3 , in Arabidopsis along with mouse DGAT2 ( mD ) increased TAG accumulation by 54% in leaves and 13% in seeds compared with control lines coexpressing SiCO and mD. Lipid synthesis rates increased, consistent with an increase in lipid sink strength that sequesters newly synthesized TAG, thereby relieving the constitutive BADC‐dependent inhibition of ACCase reported for WT Arabidopsis. These OLE variants represent novel factors for potentially increasing TAG accumulation in a variety of oil crops.

59 BASIC BIOLOGICAL SCIENCES↗

Effect of Quartz Aperture Covers on the Fluid Dynamics and Thermal Efficiency of Falling Particle Receivers

Falling particle receivers are an emerging technology for use in concentrating solar power systems. In this paper, quartz half-shells are investigated for use as full or partial aperture covers to reduce receiver thermal losses. Quartz half-shell aperture covers offer the ability to minimally interfere with incoming solar radiation from the heliostat field while obstructing thermal radiation and advection from leaving the receiver cavity. The fluid dynamics and heat transfer of a receiver subdomain and surrounding air are modeled using ANSYS®FLUENT We compare the percentage of total incident solar power lost due to conduction through the receiver walls, advective losses through the aperture, and radiation exiting the aperture. Contrary to expected outcomes, results show that quartz aperture covers can increase radiative losses and result in modest to nonexistent reductions in advective losses. The increased radiative losses are driven by elevated quartz half-shell temperatures and have the potential to be mitigated by active cooling and/or material selection. Quartz half-shell total transmissivity was measured experimentally using a radiometer and the National Solar Thermal Test Facility heliostat field with values up to 0.97 ± 0.01. Quartz half-shell aperture covers did not yield expected efficiency gains in numerical results due to increased radiative losses, but efficiency improvement in some numerical results and the performance of quartz half-shells subject to concentrated solar radiation suggest that quartz half-shell aperture covers should be investigated further.

14 SOLAR ENERGY↗

Rare earth elements from waste

Rare earth elements (REEs) are critical materials in electronics and clean technologies. With the diminishing of easily accessible minerals for mining, the REE recovery from waste is an alternative toward a circular economy. Present methods for REE recovery suffer from lengthy purifications, low extractability, and high wastewater streams. Here, we report an ultrafast electrothermal process (~3000°C, ~1 s) based on flash Joule heating (FJH) for activating wastes to improve REE extractability. FJH thermally degrades or reduces the hard-to-dissolve REE species to components with high thermodynamic solubility, leading to ~2× increase in leachability and high recovery yields using diluted acid (e.g., 0.1 M HCl). The activation strategy is feasible for various wastes including coal fly ash, bauxite residue, and electronic waste. The rapid FJH process is energy-efficient with a low electrical energy consumption of 600 kWh ton –1 . The potential for this route to be rapidly scaled is outlined.

01 COAL, LIGNITE, AND PEAT↗

Forest carbon sequestration on the west coast, USA: Role of species, productivity, and stockability

Forest ecosystems store large amounts of carbon and can be important sources, or sinks, of the atmospheric carbon dioxide that is contributing to global warming. Understanding the carbon storage potential of different forests and their response to management and disturbance events are fundamental to developing policies and scenarios to partially offset greenhouse gas emissions. Projections of live tree carbon accumulation are handled differently in different models, with inconsistent results. We developed growth-and-yield style models to predict stand-level live tree carbon density as a function of stand age in all vegetation types of the coastal Pacific region, US (California, Oregon, and Washington), from 7,523 national forest inventory plots. We incorporated site productivity and stockability within the Chapman-Richards equation and tested whether intensively managed private forests behaved differently from less managed public forests. We found that the best models incorporated stockability in the equation term controlling stand carrying capacity, and site productivity in the equation terms controlling the growth rate and shape of the curve. RMSEs ranged from 10 to 137 Mg C/ha for different vegetation types. There was not a significant effect of ownership over the standard industrial rotation length (~50 yrs) for the productive Douglas-fir/western hemlock zone, indicating that differences in stockability and productivity captured much of the variation attributed to management intensity. Our models suggest that doubling the rotation length on these intensively managed lands from 35 to 70 years would result in 2.35 times more live tree carbon stored on the landscape. These findings are at odds with some studies that have projected higher carbon densities with stand age for the same vegetation types, and have not found an increase in yields (on an annual basis) with longer rotations. We suspect that differences are primarily due to the application of yield curves developed from fully-stocked, undisturbed, single-species, “normal” stands without accounting for the substantial proportion of forests that don’t meet those assumptions. The carbon accumulation curves developed here can be applied directly in growth-and-yield style projection models, and used to validate the predictions of ecophysiological, cohort, or single-tree style models being used to project carbon futures for forests in the region. Our approach may prove useful for developing robust models in other forest types.

Chisholm, Paul J. (ORCID:0000000238784707)↗

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗

Results from a multi-laboratory ocean metaproteomic intercomparison: effects of LC-MS acquisition and data analysis procedures

Metaproteomics is an increasingly popular methodology that provides information regarding the metabolic functions of specific microbial taxa and has potential for contributing to ocean ecology and biogeochemical studies. A blinded multi-laboratory intercomparison was conducted to assess comparability and reproducibility of taxonomic and functional results and their sensitivity to methodological variables. Euphotic zone samples from the Bermuda Atlantic Time-series Study (BATS) in the North Atlantic Ocean collected by in situ pumps and the autonomous underwater vehicle (AUV) Clio were distributed with a paired metagenome, and one-dimensional (1D) liquid chromatographic data-dependent acquisition mass spectrometry analysis was stipulated. Analysis of mass spectra from seven laboratories through a common bioinformatic pipeline identified a shared set of 1056 proteins from 1395 shared peptide constituents. Quantitative analyses showed good reproducibility: pairwise regressions of spectral counts between laboratories yielded R 2 values averaged 0.62±0.11, and a Sørensen similarity analysis of the top 1000 proteins revealed 70 %–80 % similarity between laboratory groups. Taxonomic and functional assignments showed good coherence between technical replicates and different laboratories. A bioinformatic intercomparison study, involving 10 laboratories using eight software packages, successfully identified thousands of peptides within the complex metaproteomic datasets, demonstrating the utility of these software tools for ocean metaproteomic research. Lessons learned and potential improvements in methods were described. Future efforts could examine reproducibility in deeper metaproteomes, examine accuracy in targeted absolute quantitation analyses, and develop standards for data output formats to improve data interoperability. Together, these results demonstrate the reproducibility of metaproteomic analyses and their suitability for microbial oceanography research, including integration into global-scale ocean surveys and ocean biogeochemical models.

59 BASIC BIOLOGICAL SCIENCES↗

Atomic Layer Deposition for Spatial Control of Redox Reaction Selectivity

Photocatalytic water splitting holds great potential in the pursuit of the U.S. Department of Energy's Hydrogen Shot initiative to bring the cost of H2 to $1/kg by 2031. A key challenge in the development of photocatalysts is increasing their overall solar-to-hydrogen efficiency by enhancing charge separation yields and redox selectivity. In this work, we use area selective ALD of oxide films to develop tunable interphase layers for selective oxidation and reduction reactions on a single substrate. This presentation details initial synthesis and characterization of Pt- and Au-based planar thin film electrodes in which Au regions were deactivated towards ALD growth through self-assembled thiol monolayers. The suppression of TiO2 ALD selectivity of thiols was assessed through ellipsometry, X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry. A patterned planar sample comprised of interdigitated arrays of Au and Pt, used as a surrogate for a photocatalyst particle containing two different co-catalysts, was exposed to ALD growth and removal of the inhibitor species. Scanning electrochemical microscopy (SECM) was used then to probe the local activity of different regions of the patterned surface towards the hydrogen evolution reaction (HER) and iron oxidation and correlated with the ionic and e- blocking effects of the area selective ALD coating. We will also detail the application of these findings to the ongoing development of 3D, particle-based photocatalysts.

atomic layer deposition↗

Closed‐Loop Recyclable Vitrimer Plastics from PET Waste: A Design for Circularity

Plastics are essential to modern society, but their low recycling rates and inefficient end-of-life management pose a significant environmental challenge. Herein, the efficient strategy for upcycling postconsumer poly(ethylene terephthalate) (PET) waste into robust, closed-loop recyclable vitrimer plastics and composites is presented to address this issue. The catalyst-free aminolysis utilizes readily available amines to deconstruct diverse PET wastes into macromonomers, which are upcycled into vitrimers, exhibiting superior mechanical properties and exceeding the ultimate tensile stress and Young's Modulus of virgin PET by 80% and 150% respectively. These vitrimers exhibit excellent healability, shape memory, thermal reprocessability, and closed-loop chemical recyclability, enabling quantitative macromonomer recovery even from mixed plastic waste streams and glass/carbon fiber reinforced vitrimer (G/CFRV) composites. Furthermore, the vitrimer resin yields robust GFRV and CFRV composites with tensile strengths exceeding those of traditional epoxy composites by 100% and 80%, respectively, while maintaining complete chemical recyclability of both constituent materials. A preliminary technoeconomic analysis confirms the costeffectiveness and competitiveness of the facile PET deconstruction approach, which is potentially adaptable to other condensation polymers. Further, this study presents a facile approach to upcycling plastic waste into circular plastics and composites, offering a sustainable solution to global plastic waste management and fostering a circular economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-throughput screening tools facilitate calculation of a combined exposure-bioactivity index for chemicals with endocrine activity

High-throughput and computational tools provide a new opportunity to calculate combined bioactivity of exposure to diverse chemicals acting through a common mechanism. We used high throughput in vitro bioactivity data and exposure predictions from the U.S. EPA’s Toxicity and Exposure Forecaster (ToxCast and ExpoCast) to estimate combined estrogen receptor (ER) agonist activity of non-pharmaceutical chemical exposures for the general U.S. population. High-throughput toxicokinetic (HTTK) data provide conversion factors that relate bioactive concentrations measured in vitro (µM), to predicted population geometric mean exposure rates (mg/kg/day). These data were available for 22 chemicals with ER agonist activity and were estimated for other ER bioactive chemicals based on the geometric mean of HTTK values across chemicals. For each chemical, ER bioactivity across ToxCast assays was compared to predicted population geometric mean exposure at different levels of in vitro potency and model certainty. Dose additivity was assumed in calculating a Combined Exposure-Bioactivity Index (CEBI), the sum of exposure/bioactivity ratios. Combined estrogen bioactivity was also calculated in terms of the percent maximum bioactivity of chemical mixtures in human plasma using a concentration-addition model. Estimated CEBIs vary greatly depending on assumptions used for exposure and bioactivity. In general, CEBI values were <1 when using median of the estimated general population chemical intake rates, while CEBI were ≥1 when using the upper 95th confidence bound for those same intake rates for all chemicals. Concentration-addition model predictions of mixture bioactivity yield comparable results. Based on current in vitro bioactivity data, HTTK methods, and exposure models, combined exposure scenarios sufficient to influence estrogen bioactivity in the general population cannot be ruled out. Future improvements in screening methods and computational models could reduce uncertainty and better inform the potential combined effects of estrogenic chemicals.

54 ENVIRONMENTAL SCIENCES↗

Towards the sustainable conversion of corn stover into bioenergy and bioproducts through biochemical route: Technical, economic and strategic perspectives

Corn stover (CS) is one of the most abundant agricultural wastes and is ubiquitous around the world that is left over after grain harvest and accounts for 47–50% dry mass of the total grain yield. The global CS yield is 1661.25 million tons/year, which is 27.2% of the total agricultural waste. CS consists of about 34.5% stems, 32.3% leaves, 14.3% husks, 12.3% cobs and 6.6% flowers, with up to 45% cellulose, 30% hemicellulose and 20% lignin. Further, due to its favorable economic and environmental potential, CS is considered an ideal raw material for producing biofuels and biobased chemicals, which can largely be divided into carbohydrate and lignin platforms. However, the techno-economic perspectives of CS-based biorefineries have remained questionable due to the inadequate supply chain logistics, lack of cost-effective conversion technologies, limited scale-up of the product-specific technologies, and lower competitiveness in the market compared to their counterparts, such as sugar and starch-based biorefineries. While CS is converted by thermochemical and biochemical approaches, the latter is considered to be more sustainable for its selective conversion under mild conditions using microorganisms. This review aimed to critically discuss the latest research and developments on the biochemical conversion of CS into biofuels and chemicals. In particular, this paper covers the market potential of biofuels and chemicals to which CS can make a significant contribution, technological developments in the microbial conversion of CS, major biofuels and chemicals produced from CS-derived carbohydrates and lignin, and the technoeconomic perspectives of CS-based biorefinery.

09 BIOMASS FUELS↗

Errors introduced in fission neutron spectrum measurements using a single reference

Measurements of physical quantities are often made relative to a reference quantity, simplifying the interpretation of the measurement and its uncertainties. However, if applied without careful considerations, this technique can carry with it a significant and complex systematic error that is usually ignored. For example, measurements of continuous neutron spectra relative to a reference spectrum yield a result that does not properly include the important effects of neutron scattering in the experimental environment. These effects act to distort the measured spectrum shape and create notable errors in spectrum-integrated quantities. While this effect is one of a series of known potential sources of systematic error including, but not limited to target impurities, angular distributions, incident beam flux, and others, the error introduced from differences in environmental scattering effects between the reference and desired spectra are frequently overlooked. In this work, we demonstrate the origin of this error using simulated data corresponding to measurements of the neutron-induced prompt fission neutron spectra of 233 U, 235 U, 238 U, and 239 Pu as well as the spontaneous fission neutron spectrum of 252 Cf. Errors in the spectrum shape can be as high as 10%–15% depending on the combination of incident and outgoing neutron energy. The spectrum integral and average spectrum energy also contain errors that change with incident neutron energy and can be as high as ~2%. Although this study is based on simulated data, we also show a method for proving that this error exists in an experimental data set and we show a correction that can be applied to results of this type to obtain a more accurate result, thereby largely removing systematic errors from environmental scattering effects. The potential for these kinds of errors should be considered in measurements producing continuous neutron spectra.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Chemical recycling of post-consumer polyester wastes using a tertiary amine organocatalyst

Recycling diverse waste plastics poses challenges due to complex sorting and processing, resulting in high costs and inefficiency. To tackle this, we present a metal-free catalytic sorting method for targeted deconstruction of polyester from post-consumer plastic waste, encompassing textiles, plastic mixtures, and multilayer packaging materials. This method employs N-methylpiperidine, a tertiary amine catalyst in methanol, to depolymerize polyethylene terephthalate (PET). Operating under these conditions (160°C, 1 h), we achieve 100% yields of dimethyl terephthalate and ethylene glycol. This technique also effectively breaks down other polyesters, including polylactic acid, polycarbonate, and polybutylene terephthalate, yielding high-yield monomers at relatively low temperatures. Through comprehensive nuclear magnetic resonance (NMR) analysis, we propose that N-methylpiperidine’s role is in enhancing methanol nucleophilicity and activating PET’s ester bond. Our insights advance the chemical recycling of post-consumer plastic waste, offering a potentially simple and efficient path to closing the polyester production loop.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Predicted Fracture Tendency of Naturally Occurring Aluminum Surface Coatings under Tensile Loading

Naturally occurring coatings on aluminum metal, such as its oxide or hydroxide, serve to protect the material from corrosion. Understanding the conditions under which these coatings mechanically fail is therefore expected to be an important aspect of predictive models for aluminum component lifetimes. To this end, we develop and apply a molecular dynamics (MD) modeling framework for conducting tension tests that is capable of isolating factors governing the mechanical strength as a function of coating chemistry, defect morphology, and variables associated with the loading path. We consider two representative materials, including γ-Al 2 O 3 and γ-Al(OH) 3 (i.e., oxide and hydroxide), both of which form readily as aluminum surface coatings. Our results indicate that defects have a significant bearing on the strength of aluminum oxide, with grain boundaries serving to reduce the strain at failure from ε zz = 0.300 to 0.219, relative to perfect single crystal. Our simulations also predict that porosity lowers the elastic stiffness and yield strength of the oxide. Relative to perfect crystal, we find porosity factors of 5%, 10% and 20% decrease the yield stress by 26%, 36% and 53%, respectively. MD predicts that perfect hydroxide and oxide single crystal have respective strains at failure of 0.08 and 0.31 under tensile uniaxial strain loading, and that the corresponding yield stresses are respectively 1.6 and 11.1 GPa. These data indicate that the hydroxide is substantially more susceptible to mechanical failure than the oxide. Our results, coupled with literature findings that indicate hot and humid conditions favor formation of hydroxide and defective oxide coatings, indicate the potential for a complicated dependence of aluminum corrosion susceptibility and stress corrosion cracking on aging history.

36 MATERIALS SCIENCE↗

Electrochemical Recovery of Iron from Spent Pickle Liquor by Chloride-Based Molten Salt Electrolysis

Spent pickle liquor (SPL) is a waste stream generated in the steel industry that presents both a disposal challenge and a potential resource for metal recovery. This study investigates the electrochemical extraction of high-purity iron metal from SPL using chloride-based molten salt electrolysis (CMSE). Electrochemical characterization of diluted SPL confirmed Fe 2+ as the dominant species. Thermal dehydration of SPL under inert atmosphere yielded FeCl 2 -rich solids, which were directly employed as feedstock for electrolysis in LiCl–KCl eutectic melts at 500 °C. Cyclic voltammetry of FeCl 2 in this melt revealed well-defined Fe 2+ /Fe 0 redox behavior within the electrochemical stability window of the supporting electrolyte. High coulombic efficiency (>85%) electrodeposition was achieved demonstrating that iron metal can be produced from dehydrated SPL by CMSE. The electrodeposited iron exhibited >98 wt% purity, which was further enhanced to 99.9 wt% via arc melting. The resulting iron powder was ferromagnetic, and its size distribution was found to be suitable for powder metallurgy applications. This work demonstrates a scalable, energy-efficient pathway for valorizing SPL into high-purity iron metal, advancing circular economy strategies in the steel industry.

Materials science↗

Comparing Pr 3+ and Nd 3+ for deactivating the Er 3+ : 4 I 13/2 level in lanthanum titanate glass

Erbium lanthanum titanate glasses were prepared by levitation melting for the spectroscopic study of ways to promote the mid-infrared fluorescence. Two series of heavily erbium doped glasses (15 wt%) were prepared with the addition of either Pr 3+ or Nd 3+ in amounts relative to Er 3+ of 0.05, 0.1, and 0.2. Both ions quench the lower Er 3+ laser level with the Pr 3+ doing so more rapidly. Although high co-dopant concentrations result in higher energy transfer, as clearly evidenced in upconversion and downconversion fluorescence measurements, the mid-infrared lifetime also suffers a reduction and, therefore, a balance must be struck in the co-dopant concentration. Lifetime and spectral measurements indicate that, at a fixed relative co-dopant amount, Pr 3+ is more effective than Nd 3+ at removing the bottleneck of the Er 3+ 4 I 13/2 level. Moreover, consideration of the lifetimes alongside the absorption data of the individual ions indicates that despite the large absorption cross-section of Nd 3+ at 808 nm, the concentration needed to yield more absorbed power than utilizing direct 976 nm excitation of Er 3+ results in unfavorable lifetimes of the mid-infrared transition. In the end, Pr 3+ prevails as the superior co-dopant in terms of the effects on fluorescence lifetimes as well as potential laser system design considerations. In a unique self-doping approach, a reducing melt atmosphere of Ar instead of O 2 creates a small fraction of Ti 3+ . In 5Er 2 O 3 -12La 2 O 3 -83TiO 2 glass, the presence of Ti 3+ quenches the 4 I 13/2 emission about 2.6 times more than the 4 I 11/2 when lifetimes are compared to an O 2 melt environment. As an additional means of increasing the mid-infrared emission, the effect of temperature on the mid- and near- infrared lifetimes of a lightly doped lanthanum titanate composition is investigated between 77-300 K. The mid-infrared lifetime increases by ∼30% while the near-infrared lifetime increases by ∼10%, which suggests in addition to co-doping, active cooling of the gain media will further enhance performance.

Materials Science↗

Active Activation Diagnostics for High Energy X-ray and Neutron Measurements

Nuclear activation is a vital tool for diagnosing the properties of high-energy particles and photons. We investigate several potential reactions and suitable activation materials that could be used to simultaneously measure both neutrons and high-energy bremsstrahlung x-rays using one detector. Such a diagnostic would be valuable and practical for several facilities capable of creating such high-energy neutrons and x-rays. Laser-generated sources, such as NIF(-ARC) or Omega(-EP), have been shown to be capable of creating high-energy x-rays via high-intensity laser interactions and neutrons via DT fusion reactions. Furthermore, current laser technology is driving the demand for higher repetition rate diagnostics, hence we further constrain reaction/activation selections to accommodate high-repletion rate experiments. Our investigation will concentrate on identifying potential short half-life activation materials associated with high-energy x-ray reactions that could be incorporated into the existing realtime neutron activation detectors (RTNADs), an array of 48 activation detectors positioned around the NIF target chamber used to measure the DT neutron yield isotropy. We have identified two materials, gold and neodymium, that appear to be the best candidates to complement the RTNADs, by adding a new high-energy x-ray measurement capability.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗