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At least 1,729 records · Page 96

Reduced graphene oxide as a filament material for thermal ionization mass spectrometry

Isotopic information can be informative as to the intended use and/or production history of special nuclear material. For uranium and plutonium samples, thermal ionization mass spectrometry (TIMS) is the benchmark technique for determining isotope ratio data. Sample utilization in thermal ionization, however, is low with typical ionization efficiencies between 0.1% and 0.5% - i.e., only 0.1% to 0.5% of the sample contributes to the detected signal. One barrier to improving the ionization efficiency is thermodynamic limits related to the work function of the ionization filament. Graphene oxide, having a tunable work function, has the potential to greatly improve ionization efficiencies over Re or W-based filaments. The bulk work function of graphene can be tuned through doping or incorporating metal particulates in the graphene oxide matrix. In the first year of this LDRD project reduced graphene oxide (RGO) filaments were constructed using 3D printing techniques and mated to commercial filament posts. The second year of this LDRD produced ultra-low U background RGO filaments and RGO-composite filaments that are more robust than Re filaments at high temperatures and high vacuum conditions. Preliminary results using a commercial TIMS instrument demonstrate a 500 % ionization enhancement for Uranium when using Re-RGO composite-based filaments over traditional Re filaments when direct loading sample solutions onto filaments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

In situ aircraft measurements of enhanced levels of N2O associated with thunderstorm lightning

A series of measurements of enhanced levels of atmospheric N2O associated with thunderstorm lightning are reported. The data were gathered by instrumentation on-board an aircraft operated as part of the NASA Storm Hazards Project. Air samples were taken both during storms and in clear conditions to have a basis for comparisons; sample bottles were filled at altitudes from 11,000-40,000 ft. Gas chromatography was employed for sample composition analyses, revealing clear air N2O concentrations of about 310 ppbv, while storm concentrations reached, for example, 490, 729, and 393 ppbv. Although the measurements did not precisely characterize the actual lightning contributions, the enhancements being present during electrically active storms did confirm that trace gases are produced by lightning. Calculations are presented to demonstrate that the 3 to greater than 12 keV X rays detected in storm clouds are of sufficient energy to drive the production of N2O from the reaction of metastable nitrogen with molecular oxygen.

Levine, J. S.↗

Wildfire Segmentation From Remotely Sensed Data Using Quantum-Compatible Conditional Vector Quantized-Variational Autoencoders

Wildfires represent a critical environmental hazard with multifaceted implications for ecosystems, communities, and public health [1]. The escalating frequency and intensity of wildfires globally have intensified the urgency for robust segmentation methodologies to facilitate effective mitigation, response, and recovery strategies [2]. Accurate wildfire segmentation is pivotal for delineating fire boundaries, assessing progression patterns, and prioritizing resource allocation during emergency scenarios. Furthermore, precise segmentation enables stakeholders, including policymakers, environmental scientists, and emergency responders, to formulate evidence-based strategies, thereby minimizing socio-economic disruptions and ecological degradation. Consequently, advancing wildfire segmentation techniques through innovative technological interventions remains a paramount research imperative. Although foundational in wildfire segmentation, traditional deterministic models exhibit inherent limitations that compromise their efficacy in dynamic and uncertain environments. These models often operate on rigid algorithms prioritizing deterministic classifications, thereby overlooking the inherent complexities and uncertainties associated with wildfire behavior and satellite data variability. Such deterministic frameworks tend to produce oversimplified representations that fail to capture the intricate nuances of evolving fire dynamics, spatial heterogeneity, and environmental interactions [1]. Consequently, the deterministic approach’s propensity for uncertainty collapsing [1, 3] hampers the accuracy, reliability, and applicability of segmentation outcomes in real-world scenarios. Contrastingly, stochastic models offer a more nuanced and adaptable framework for wildfire segmentation. By integrating probabilistic elements into the modeling paradigm, stochastic approaches, particularly probabilistic approaches such as variational auto encoders (VAEs) [4], facilitate comprehensive uncertainty assessment, enabling researchers to quantify and incorporate uncertainties into segmentation outcomes effectively. This probabilistic nature empowers stochastic models to encapsulate variability, account for data inconsistencies, and adapt to evolving environmental conditions, enhancing segmentation accuracy, reliability, and robustness. Embracing stochastic methodologies thus catalyzes advancements in wildfire science by fostering a more holistic, adaptive, and resilient segmentation framework. Despite VAEs demonstrating significant promise in various applications, they come with inherent limitations that have garnered attention within the machine learning community. One of the primary drawbacks lies in their reliance on static priors, which essentially assume a fixed distribution for latent variables, thereby limiting the model’s flexibility to capture complex data structures effectively [5]. This static nature leads to suboptimal representations, especially when dealing with complex and high-dimensional data. Additionally, VAEs often struggle with generating sharp and realistic samples, a phenomenon commonly referred to as mode collapse [5, 7, 6]. Furthermore, the optimization process in VAEs, which involves balancing the reconstruction loss and the regularization term, can sometimes be challenging to fine-tune [7]. In recent efforts to address these shortcomings, alternative approaches like Vector Quantized Variational Auto encoders(VQ-VAEs) [7], address the challenges by incorporating discrete latent variables and leveraging techniques that enhance the quality and diversity of generated samples while maintaining efficient training dynamics. VQ-VAEs propose a dynamic prior distribution generation mechanism that diverges from the static priors commonly associated with traditional VAEs. This dynamic approach allows for more adaptive and context-aware latent variable representations, thereby potentially capturing complex data structures more effectively. Unlike autoregressive prior models such as PixelCNN, which, despite their ability to model dependencies across data dimensions, suffer from significant computational inefficiencies and lack flexibility in handling diverse datasets. In our work, we propose to use a generative quantum-compatible approach to help alleviate the shortcomings of autoregressive prior model in VQ-VAEs. Restricted Boltzmann Machines (RBMs) are a viable alternative prior model that can learn prior distributions in a faster and more flexible manner. In this research endeavor, we meticulously curate a state-of-the-art dataset leveraging satellite MODIS data in conjunction with VIIRS fire masks, derived from Fire Radiative Power (FRP), thereby encapsulating diverse wildfire scenarios and environmental contexts. We developed a conditional VQ-VAE architecture with the RBM prior model that is trained in a supervised manner for segmenting wildfire masks. This innovative approach synergistically harnesses deep learning capabilities, enabling the generation of segmentation maps characterized by heightened precision, granularity, and contextual relevance. Furthermore, replacing the autoregressive prior learning method proposed by the original VQ-VAE with a prior density approximation via quantum-compatible RBM facilitates expedited inference processes, augments flexibility in prior sampling, optimizes computational efficiency and establishes a groundbreaking benchmark in wildfire segmentation methodologies.

quantum machine learning↗

Selectivity enhancement in photoacoustic gas analysis via phase-sensitive detection at high modulation frequency

A method for detecting a target fluid in a fluid sample comprising a first fluid and the target fluid using photoacoustic spectroscopy (PAS), comprises a) providing a light source configured to introduce an optical signal having at least one wavelength into the fluid sample; b) modulating the optical signal at a desired modulation frequency such that the optical signal generates an acoustic signal in the fluid sample; c) measuring the acoustic signal in a resonant acoustic detector; and d) using the phase of the acoustic signal to detect the presence of the target fluid.

Kosterev, Anatoliy↗

Aerial Lidar and Geomorphic Change Detection Software- Tools for Monitoring Canyon Sediments at LANL - 18668

The Los Alamos National Laboratory Environmental Remediation program has conducted extensive geomorphic surveys of sediment deposits in the canyon bottoms within and surrounding the facility. The goal of the geomorphic surveys was to provide basic information needed to characterize chemical inventories of the sediments downstream of historical release sites. Sediment units were mapped based on depositional setting and age. Representative characterization samples were collected for each unit and submitted for chemical analysis. Chemical inventories were estimated by calculating the total volume of each depositional unit and multiplying by average chemical concentration. This method of characterization provides a spatial distribution of chemical data based on fluvial processes. In general, for the canyon bottom sediments, the higher concentrations of industrial chemicals were associated with fine-grained floodplain deposits closest to the source. Since initial characterization, many of the reaches have undergone changes in response to post-wildfire floods and severe rain events. These events impacted the channel and floodplain deposits. Much of the elevated concentrations are confined to the over-bank deposits distal from the primary channel. In order to ensure that the sediment units containing elevated chemical concentrations are stable, repeat aerial light detection and ranging (LiDAR) surveys are conducted and changes are assessed using the Geomorphic Change Detection (GCD) plug-in for ArcGIS. These tools provide high confidence uncertainty estimates and extensive areal coverage. This is a valuable method for long-term monitoring of surface sediments with low-level but widespread contaminant distributions. All of the monitored canyon bottom reaches pass risk assessment and present technically infeasible sediment removal options. Following the 2014 monsoon season, aerial LiDAR data has been collected annually and the resulting digital elevation models (DEMs) processed using the GCD method. Changes are identified using GCD and are verified by field walk downs. If erosion is identified in areas which are vulnerable to mobilizing contaminated sediment, enhanced controls can be installed to stabilize banks or other areas with high erosion potential. Annual sediment monitoring samples are collected where there is evidence for flow and deposition within the past year. Since 2014, no severe floods have been catalogued using the LiDAR surveys and GCD software. The recent rainfall/runoff events have not caused major changes to the canyon bottom channels and floodplains. Geomorphic processes identified in the monitoring results include channel aggradation and incision that over the course of a monsoon season results in minor changes to the system. Other active processes contributing to observed changes are minor slides, flows, slumps, and falls of unconsolidated sediment on steep bedrock or soil surfaces. A comprehensive baseline has been established by geomorphic mapping and characterization sampling. Periodic monitoring consists of LiDAR surveys and GCD analysis which offers an effective and defensible methodology for documenting stability of surface sediments. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

De-Stressing Biofuel Microalgae: Leveraging Beneficial Microbiomes to Alleviate Harmful Conditions that Reduce Algal Growth

Industrial-scale production of algal biofuels is hampered by two major stressors: environmental and biological. Specifically, high light intensities and temperatures combined with microbial predators can wipe out entire crops of microalgae, which increases prices (Shurin et al., 2013). We are examining interactions between Desmodesmus sp. CO46, a species of microalgae used in biofuel production, and its microbiomes (also known as bacterial communities) that attach to its cell periphery. This work seeks to establish and monitor bacterial species that beneficially interact with Desmodesmus to enhance its growth by mitigating the negative effects of high light, high temperature, and pathogen attack. Algal cells were cultivated with samples of diluted microbiome bacteria in sterile artificial seawater (F/2 media), and algal growth was measured via chlorophyll-a fluorometry. By monitoring samples of Desmodesmus cultured with simplified microbiomes under high light cycled incubation, we find an array of algal growth responses ranging from highly beneficial to severely negative. Utilizing this library of helpful microbiomes will assist with the reliable, larger scale cultivation of Desmodesmus for biofuels and bioproducts and provide cheaper renewable energy. Future experimentation is intended to compare bulk algal dry weight between the microbiomes when grown in largescale, to see whether combining beneficial simplified microbiomes would result in an additive effect on algal growth enhancement, and to investigate more closely the specific metabolic exchanges between mutualistic bacteria and Desmodesmus. Eventually, the beneficial bacteria will also be identified through DNA sequencing.

09 BIOMASS FUELS↗

Star Formation in Galaxies at z ∼ 4–5 from the SMUVS Survey: A Clear Starburst/Main-sequence Bimodality for Hα Emitters on the SFR–M* Plane

We study a large galaxy sample from the Spitzer Matching Survey of the UltraVISTA ultra-deep Stripes (SMUVS) to search for sources with enhanced 3.6 μm fluxes indicative of strong Hα emission at z=3.9--4.9. We find that the percentage of “Hα excess” sources reaches 37%–40% for galaxies with stellar masses log{sub 10}(M{sup ∗}/M{sub ⊙})≈9--10 and decreases to <20% at log{sub 10}(M{sup ∗}/M{sub ⊙})∼10.7. At higher stellar masses, however, the trend reverses, although this is likely due to active galactic nucleus contamination. We derive star formation rates (SFR) and specific SFR (sSFR) from the inferred Hα equivalent widths of our “Hα excess” galaxies. We show, for the first time, that the “Hα excess” galaxies clearly have a bimodal distribution on the SFR–M* plane: they lie on the main sequence of star formation (with log{sub 10}(sSFR/yr{sup −1})<−8.05) or in a starburst cloud (with log{sub 10}(sSFR/yr{sup −1})>−7.60). The latter contains ∼15% of all the objects in our sample and accounts for >50% of the cosmic SFR density at z=3.9--4.9, for which we derive a robust lower limit of 0.066 M{sub ⊙} yr{sup −1} Mpc{sup −3}. Finally, we identify an unusual >50σ overdensity of z=3.9--4.9 galaxies within a 0.20×0.20 arcmin{sup 2} region. We conclude that the SMUVS unique combination of area and depth at mid-IR wavelengths provides an unprecedented level of statistics and dynamic range that are fundamental to revealing new aspects of galaxy evolution in the young universe.

79 ASTRONOMY AND ASTROPHYSICS↗

Robust long-range magnetic correlation across antiphase domain boundaries in Sr 2 CrReO 6

Here, we report a resonant elastic x-ray scattering study of a thin-film sample of Sr 2 CrReO 6 , which has one of the highest ferrimagnetic transition temperatures among ordered double perovskites.We found resonantly enhanced magnetic Bragg peaks at Q = (odd, odd, odd) at both the rhenium L 2 and L 3 edges, which coincide with the structural Bragg peaks of Sr 2 CrReO 6 . By analyzing the widths of these Bragg peaks, we extracted very different structural and magnetic correlation lengths. The former is about 15 nm, while the latter is constrained by the instrumental resolution to be at least 90 nm. We argue that a finite structural correlation length is consistent with the existence of antiphase nanodomains in our sample. On the other hand, a much larger magnetic correlation length indicates that the magnetic correlation extends far beyond the boundaries of individual domains and is consistent with strong antiferromagnetic coupling between different antiphase domains. Last, from the azimuthal dependence of the magnetic intensity, we show that the magnetic moments lie perpendicular to the c axis, which explains the earlier bulk magnetization data.

36 MATERIALS SCIENCE↗

Field demonstration of DNAPL dehalogenation using emulsified zero-valent iron

This paper describes the results of the first field-scale demonstration conducted to evaluate the performance of nanoscale emulsified zero-valent iron (EZVI) injected into the saturated zone to enhance in situ dehalogenation of dense, nonaqueous phase liquids (DNAPLs) containing trichloroethene (TCE). EZVI is an innovative and emerging remediation technology. EZVI is a surfactant-stabilized, biodegradable emulsion that forms emulsion droplets consisting of an oil-liquid membrane surrounding zero-valent iron (ZVI) particles in water. EZVI was injected over a five day period into eight wells in a demonstration test area within a larger DNAPL source area at NASA's Launch Complex 34 (LC34) using a pressure pulse injection method. Soil and groundwater samples were collected before and after treatment and analyzed for volatile organic compounds (VOCs) to evaluate the changes in VOC mass, concentration and mass flux. Significant reductions in TCE soil concentrations (>80%) were observed at four of the six soil sampling locations within 90 days of EZVI injection. Somewhat lower reductions were observed at the other two soil sampling locations where visual observations suggest that most of the EZVI migrated up above the target treatment depth. Significant reductions in TCE groundwater concentrations (57 to 100%) were observed at all depths targeted with EZVI. Groundwater samples from the treatment area also showed significant increases in the concentrations of cis-1,2-dichloroethene (cDCE), vinyl chloride (VC) and ethene. The decrease in concentrations of TCE in soil and groundwater samples following treatment with EZVI is believed to be due to abiotic degradation associated with the ZVI as well as biodegradation enhanced by the presence of the oil and surfactant in the EZVI emulsion.

Water Pollutants/isolation & purification↗

Occurrence, leaching, and degradation of Cry1Ab protein from transgenic maize detritus in agricultural streams

The insecticidal Cry1Ab protein expressed by transgenic (Bt) maize can enter adjacent water bodies via multiple pathways, but its fate in stream ecosystems is not as well studied as in terrestrial systems. In this study, we used a combination of field sampling and laboratory experiments to examine the occurrence, leaching, and degradation of soluble Cry1Ab protein derived from Bt maize in agricultural streams. We surveyed 11 agricultural streams in northwestern Indiana, USA, on 6 dates that encompassed the growing season, crop harvest, and snowmelt/spring flooding, and detected Cry1Ab protein in the water column and in flowing subsurface tile drains at concentrations of 3–60 ng/L. In a series of laboratory experiments, submerged Bt maize leaves leached Cry1Ab into stream water with 1% of the protein remaining in leaves after 70 d. Laboratory experiments suggested that dissolved Cry1Ab protein degraded rapidly in microcosms containing water-column microorganisms, and light did not enhance breakdown by stimulating assimilatory uptake of the protein by autotrophs. Here, the common detection of Cry1Ab protein in streams sampled across an agricultural landscape, combined with laboratory studies showing rapid leaching and degradation, suggests that Cry1Ab may be pseudo-persistent at the watershed scale due to the multiple input pathways from the surrounding terrestrial environment.

59 BASIC BIOLOGICAL SCIENCES↗

Low-field magnetoresistance up to 400 K in double perovskite Sr{sub 2}FeMoO{sub 6} synthesized by a citrate route

A wet-chemistry technique, namely the citrate route, has been used to prepare high-quality polycrystalline samples of double perovskite Sr{sub 2}FeMoO{sub 6}. We report on the evolution of magnetic and magnetoresistive properties of the synthesized samples as a function of three parameters (i) the pH of the starting solution, (ii) the decomposition temperature of the citrate precursors and (iii) the sintering conditions. The low-field magnetoresistance (LFMR) value of our best samples is as high as 5% at room temperature for an applied magnetic field of 1 kOe. Additionally, the distinguishing feature of these samples is the persistence of LFMR, with a reasonably large value, up to 400 K which is a crucial parameter for any practical application. Our study indicates that the enhancement of LFMR observed is due to a good compromise between the grain size distribution and their magnetic polarization. -- Graphical abstract: The microstructure (left panel) and corresponding low-field magnetoresistance of one of the Sr{sub 2}FeMoO{sub 6} samples synthesized in the course of this work. Highlights: • Samples of Sr{sub 2}FeMoO{sub 6} are prepared using a citrate route under varying conditions. • Magnetoresistive properties are improved and optimized. • Low-field magnetoresitence values as large as 5% at 300 K/1 kOe are reported. • Persistence of low-field magnetoresistance up to 400 K.

36 MATERIALS SCIENCE↗

Ultralow Thermal Conductivity and Thermoelectric Properties of Rb 2 Bi 8 Se 13

Complex bismuth chalcogenides are narrow band gap semiconductors with intrinsic low thermal conductivity, which exhibit high potential as highly efficient thermoelectric materials. Here, we assess the basic thermoelectric properties of polycrystalline Rb 2 Bi 8 Se 13 in the temperature range 300-823 K as well as performance-optimizing strategies. We find that the as-made bulk samples are single phase with the monoclinic crystal structure (P2 1 /m) and crystallize in layer morphology. The pristine sample exhibits an exceedingly low lattice thermal conductivity of 0.6- 0.46 W·m -1 ·K -1 at 300-823 K, which derives from strong lattice anharmonicity, large Grüneisen parameters, and low phonon velocities induced by the complex crystal structure with heavy atom Bi and a large unit cell. Here, the Cl doping successfully enhances the carrier concentration in Rb 2 Bi 8 Se 13 with a negligible impact on the electronic band structure, displaying common doping behaviors. Se vacancy, on the contrary, leads to n-type doping and enhances the effective mass and power factors more significantly. Consequently, a maximum ZT of ~0.75 at 823 K for the 0.3% Se-vacancy-doped sample is obtained.

36 MATERIALS SCIENCE↗

Field Demonstration of DNAPL Dehalogenation Using Emulsified Zero-Valent Iron

This paper describes the results of the first field-scale demonstration conducted to evaluate the performance of nano-scale emulsified zero-valent iron (EZVI) injected into the saturated zone to enhance in situ dehalogenation of dense, non-aqueous phase liquids (DNAPLs) containing trichloroethene (TCE). EZVI is an innovative and emerging remediation technology. EZVI is a surfactant-stabilized, biodegradable emulsion that forms emulsion droplets consisting of an oil-liquid membrane surrounding zero-valent iron (ZVI) particles in water. EZVI was injected over a five day period into eight wells in a demonstration test area within a larger DNAPL source area at NASA's Launch Complex 34 (LC34) using a pressure pulse injection method. Soil and groundwater samples were collected before and after treatment and analyzed for volatile organic compounds (V005) to evaluate the changes in VOC mass, concentration and mass flux. Significant reductions in TCE soil concentrations (>80%) were observed at four of the six soil sampling locations within 90 days of EZVI injection. Somewhat lower reductions were observed at the other two soil sampling locations where visual observations suggest that most of the EZVI migrated up above the target treatment depth. Significant reductions in TCE groundwater concentrations (57 to 100%) were observed at all depths targeted with EZVI. Groundwater samples from the treatment area also showed significant increases in the concentrations of cis-1,2-dichloroethene (cDCE), vinyl chloride (VC) and ethene. The decrease in concentrations of TCE in soil and groundwater samples following treatment with EZVI is believed to be due to abiotic degradation associated with the ZVI as well as biodegradation enhanced by the presence of the oil and surfactant in the EZVI emulsion.

Quinn, Jacqueline↗

Resonant ultrasound spectroscopy for materials with high damping and samples of arbitrary geometry

This paper describes resonant ultrasound spectroscopy (RUS) as a powerful and established technique for measuring elastic constants of a material with general anisotropy. The first step of this technique consists of extracting resonance frequencies and damping from the vibrational frequency spectrum measured on a sample with free boundary conditions. An inversion technique is then used to retrieve the elastic tensor from the measured resonance frequencies. As originally developed, RUS has been mostly applicable to (i) materials with small damping such that the resonances of the sample are well separated and (ii) samples with simple geometries for which analytical solutions exist. In this paper, these limitations are addressed with a new RUS approach adapted to materials with high damping and samples of arbitrary geometry. Resonances are extracted by fitting a sum of exponentially damped sinusoids to the measured frequency spectrum. The inversion of the elastic tensor is achieved with a genetic algorithm, which allows searching for a global minimum within a discrete and relatively wide solution space. First, the accuracy of the proposed approach is evaluated against numerical data simulated for samples with isotropic symmetry and transversely isotropic symmetry. Subsequently, the applicability of the approach is demonstrated using experimental data collected on a composite structure consisting of a cylindrical sample of Berea sandstone glued to a large piezoelectric disk. In the proposed experiments, RUS is further enhanced by the use of a 3-D laser vibrometer allowing the visualization of most of the modes in the frequency band studied.

36 MATERIALS SCIENCE↗

Simultaneous Improvement of Resolving Power and Signal-to-Noise Ratio Using a Modified Hadamard Transform-Inverse Ion Mobility Spectrometry Technique

In order to improve the resolving power (RP) and signal-to-noise ratio (SNR) of ion mobility spectrometry (IMS) simultaneously, a modified Hadamard transform-inverse ion mobility spectrometry (MHT-IIMS) technique was developed. In this novel technique, a series of isolating codes were appended to each element of the pseudo random binary sequence (PRBS), and then the modified modulation sequence was formed and used to control the ion gate of the inverse IMS (IIMS). Experimental results demonstrate that the MHT-IIMS technique can significantly enhance the resolving power and SNR simultaneously by measuring the spectra of reaction ions. Furthermore, the gas sample CCl{sub 4} and CHCl{sub 3} were measured for evaluating the capability of detecting those samples which have single and multiple product ions. The results show that this novel technique is able to simultaneously improve the resolving power and SNR notablely for the real sample detection without any significant instrumental changes. .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

CO oxidation over ceria supported Au 22 nanoclusters: Shape effect of the support

Gold (Au) nanoclusters have recently emerged as ideal models for understanding Au catalysis, because the nanosized Au particles have precise atomic numbers and uniform size. Here, in this work, we studied for the first time the support shape effect on the catalysis of Au nanoclusters by using CO oxidation as a model reaction. Au 22 (L 8 ) 6 (L = 1,8-bis(diphenylphosphino) octane) nanoclusters were supported on CeO 2 rods or cubes, then pretreated at different temperatures (up to 673 K), allowing the gradual removal of the organic phosphine ligands. CO oxidation test over these differently pretreated samples shows that CeO 2 rods are much better supports than cubes for Au 22 nanoclusters in enhancing the reaction rate. In situ IR spectroscopy coupled with CO adsorption indicates that the shape of CeO 2 support can impact the nature and quantity of exposed Au sites, as well as the efficiency of organic ligand removal. Although CeO 2 rods are helpful in exposing a greater percentage of total Au sites upon ligands removal, the percentage of active Au sites (denoted by Au δ+ , 0 < δ < 1) is lower than that on CeO 2 cubes. The in situ extended X-ray absorption spectroscopy (EXAFS) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) results show that the Au nanoclusters bound more strongly to the CeO 2 rods than to the cubes where the Au nanoclusters show more sintering. Considering the typical redox mechanism for CO oxidation over supported Au nanoclusters and nanoparticles, it is concluded that the reactivity of the lattice oxygen of CeO 2 is the determining factor for CO oxidation over Au 22 /CeO 2 . Lastly, CeO 2 rods offer more reactive lattice oxygen and abundant oxygen vacancies than the cubes and thus make the rods a superior support for Au nanoclusters in catalyzing low temperature CO oxidation.

36 MATERIALS SCIENCE↗

Multi-fidelity classification using Gaussian processes: Accelerating the prediction of large-scale computational models

We report that machine learning techniques typically rely on large datasets to create accurate classifiers. However, there are situations when data is scarce and expensive to acquire. This is the case of studies that rely on state-of-the-art computational models which typically take days to run, thus hindering the potential of machine learning tools. In this work, we present a novel classifier that takes advantage of lower fidelity models and inexpensive approximations to predict the binary output of expensive computer simulations. We postulate an autoregressive model between the different levels of fidelity with Gaussian process priors. We adopt a fully Bayesian treatment for the hyper-parameters and use Markov Chain Monte Carlo samplers. We take advantage of the probabilistic nature of the classifier to implement active learning strategies. We also introduce a sparse approximation to enhance the ability of the multi-fidelity classifier to handle a large amount of low fidelity samples. We test these multi-fidelity classifiers against their single-fidelity counterpart with synthetic data, showing a median computational cost reduction of 23% for a target accuracy of 90%. In an application to cardiac electrophysiology, the multi-fidelity classifier achieves an F1 score, the harmonic mean of precision and recall, of 99.6% compared to 74.1% of a single-fidelity classifier when both are trained with 50 samples. In general, our results show that the multi-fidelity classifiers outperform their single-fidelity counterpart in terms of accuracy in all cases. Finally, we envision that this new tool will enable researchers to study classification problems that would otherwise be prohibitively expensive. Source code is available at https://github.com/fsahli/MFclass.

97 MATHEMATICS AND COMPUTING↗