Temporal analysis of ion arrival for particle quantification
The rapid transient method records time stamps of individual ion arrival for accurate identification and quantification of nanoparticles.
Duffin, Andrew M.↗
SEARCH · Engineering Papers
Results for “isotope identification”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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NEOCAM: Near Earth Object Chemical Analysis Mission: Bridging the Gulf between Telescopic Observations and the Chemical and Mineralogical Compositions of Asteroids or Diogenes A: Diagnostic Observation of the Geology of Near Earth Spectrally-Classified Asteroids
Studies of meteorites have yielded a wealth of scientific information based on highly detailed chemical and isotopic studies possible only in sophisticated terrestrial laboratories. Telescopic studies have revealed an enormous (greater than 10(exp 5)) number of physical objects ranging in size from a few tens of meters to several hundred kilometers, orbiting not only in the traditional asteroid belt between Mars and Jupiter but also throughout the inner solar system. Many of the largest asteroids are classed into taxonomic groups based on their observed spectral properties and are designated as C, D. X, S or V types (as well as a wide range in sub-types). These objects are certainly the sources far the meteorites in our laboratories, but which asteroids are the sources for which meteorites? Spectral classes are nominally correlated to the chemical composition and physical characteristics of the asteroid itself based on studies of the spectral changes induced in meteorites due to exposure to a simulated space environment. While laboratory studies have produced some notable successes (e.g. the identification of the asteroid Vesta as the source of the H, E and D meteorite classes), it is unlikely that we have samples of each asteroidal spectral type in our meteorite collection. The correlation of spectral type and composition for many objects will therefore remain uncertain until we can return samples of specific asteroid types to Earth for analyses. The best candidates for sample return are asteroids that already come close to the Earth. Asteroids in orbit near 1 A.U. have been classified into three groups (Aten, Apollo & Amor) based on their orbital characteristics. These Near Earth Objects (NEOs) contain representatives of virtually all spectral types and sub-types of the asteroid population identified to date. Because of their close proximity to Earth, NEOs are prime targets for asteroid missions such as the NEAR-Shoemaker NASA Discovery Mission to Eros and the Japanese Hyabusa Mission to Itokawa. Also due to their close proximity to Earth, NEOs constitute the most likely set of celestial objects that will impact us in the relatively near future.
Nuth, Joseph A.↗
Lunar and Planetary Science XXXVI, Part 7
Topics discussed include: Lunar Geologic Mapping: Preliminary Mapping of Copernicus Quad High-Resolution Topography of Layers in the Valles Marineris Via Thermoclinometry ; The Critical Importance of Data Reduction Calibrations in the Interpretability of S-type Asteroid Spectra; (sup 238)U-(sup 206)Pb Age and Uranium-Lead Isotope Systematics of Mare Basalt 10017; Morphological Investigations of Martian Spherules, Comparisons to Collected Terrestrial Counterparts; The Vapor Pressure of Palladium at Temperatures up to 1973K; Areas of Favorable Illumination at the Lunar Poles Calculated from Topography; An Indigenous Origin for the South Pole-Aitken Basin Thorium Anomaly; Ar-Ar Ages of Nakhlites Y000593, NWA998, and Nakhla and CRE Ages of NWA998; Experiments on the Acoustic Properties of Titan-like Atmospheres; Analysis of Downstream Transitions in Morphology and Structure of Lava Channels on Mars; Structure and Bonding of Carbon in Clays from CI Carbonaceous Chondrites; Comparison of Three Hydrogen Distributions at the Equator of Mars; An Impact Origin for the Foliation of Ordinary Chondrites; A New Micrometeorite Collection from Antarctica and Its Preliminary Characterization by Microobservation, Microanalysis and Magnetic Methods; Volcanic Plumes and Plume Deposits on Io; Results of the Alpha-Particle-X-Ray Spectrometer on Board of the Mars Exploration Rovers; Effects of Oceans on Atmospheric Loss During the Stage of Giant Impacts; and Identification of Predominant Ferric Signatures in Association to the Martian Sulfate Deposits
Source record↗
Nucleogenic noble gas components in the Cape York iron meteorite
The paper reports data on neutron capture products of the secondary cosmic ray component, the inferred proton and neutron fluences, and the identification of double beta decay of Se-82 in heavily shielded samples of the Cape York iron meteorite. One purpose of this study is to develop a new chronometer for cosmic ray exposure, based on the nuclides I-129 (16 My half-life) and Xe-129 from low energy cosmic ray reactions on Te. The abundance ratio of these two nuclides permits the determination of an (effective) exposure age of 93 + or - 16 My, which represents the first exposure age datum of Cape York. The very small concentrations of spallogenic Ar-38 = 6.5 x 10 to the -10th cu cm STP/g in the metal and troilite (per g Fe) document the heavily shielded locations of the sample. An excess of Xe-129 in the troilite is shown to be entirely due to the decay of cosmic-ray-produced I-129. On the other hand, an inclusion in the troilite reveals the presence of Xe-129 from extinct I-129 and documents its about 4.5 Gy formation age. Mono-isotopic excess of Kr-82 is identified as due to beta-beta-decay of Se-82 with an inferred half-life of 1.0 x 10 to the 20th y. This represents the first beta-beta-decay product observed in a meteorite.
Murty, S. V. S.↗
Strategies for Distinguishing Abiotic Chemistry from Martian Biochemistry in Samples Returned from Mars
A key goal in the search for evidence of extinct or extant life on Mars will be the identification of chemical biosignatures including complex organic molecules common to all life on Earth. These include amino acids, the monomer building blocks of proteins and enzymes, and nucleobases, which serve as the structural basis of information storage in DNA and RNA. However, many of these organic compounds can also be formed abiotically as demonstrated by their prevalence in carbonaceous meteorites [1]. Therefore, an important challenge in the search for evidence of life on Mars will be distinguishing between abiotic chemistry of either meteoritic or martian origin from any chemical biosignatures from an extinct or extant martian biota. Although current robotic missions to Mars, including the 2011 Mars Science Laboratory (MSL) and the planned 2018 ExoMars rovers, will have the analytical capability needed to identify these key classes of organic molecules if present [2,3], return of a diverse suite of martian samples to Earth would allow for much more intensive laboratory studies using a broad array of extraction protocols and state-of-theart analytical techniques for bulk and spatially resolved characterization, molecular detection, and isotopic and enantiomeric compositions that may be required for unambiguous confirmation of martian life. Here we will describe current state-of-the-art laboratory analytical techniques that have been used to characterize the abundance and distribution of amino acids and nucleobases in meteorites, Apollo samples, and comet- exposed materials returned by the Stardust mission with an emphasis on their molecular characteristics that can be used to distinguish abiotic chemistry from biochemistry as we know it. The study of organic compounds in carbonaceous meteorites is highly relevant to Mars sample return analysis, since exogenous organic matter should have accumulated in the martian regolith over the last several billion years and the analytical techniques previously developed for the study of extraterrestrial materials can be applied to martian samples.
Glavin, D. P.↗
Neural MUSE Analysis
Researchers at Oak Ridge National Laboratory (ORNL) created data as part of the MUSE (Multi-Agency Urban Search Experiment Detector and Algorithm Test Bed) project simulating illicit nuclear materials located in various buildings along a road. In the simulation, a truck containing a radiation detector drives down the road gathering listmode data (counting the and energy of incident gamma radiation). Building materials, source shielding, driving speed, truck direction, truck location on the road, source type, and source placement are all varied between runs of the data set. This data was created using deterministic neutron transport and Monte Carlo methods through a combination of SCALE, MAVRIC, MCNP, and GADRAS. As part of a follow-on NA-22 project, two Kaggle competitions were created to determine the best algorithms for finding and identifying gamma sources in this simulated urban environment. The winning algorithm was neural network-based and had a test accuracy of 76.4% accuracy for source identification. This work seeks to build upon this work and improve the results through the application of novel machine learning techniques. As a first step, the data was classified by a simple Convolutional Neural Network (CNN) To accomplish this, the data was first preprocessed into “waterfall plots.” These plots are composed of energy vs count plots that are stacked vertically to show progression in time. The horizontal axis indicating the particle energy incorporated user defined bin spacing with options for in linear-, logarithmic-, square root-, and user-spaced bins. The z or color dimension showed the number of counts corresponding the energy-time combination. This data was then used to generate more data, by generating a local estimate of the mean of the distribution for a bin and then randomly re-sampling that bin from a Poisson distribution. Once all of this data was generated, it was fed into a well-known CNN architecture, ResNet50. The output layer of this model was removed and replaced with layers corresponding to the shape desired isotope outputs. The provided training data was used to train the classifier and the remaining testing data was used to evaluate the model. Results are soon to be forthcoming.
61 RADIATION PROTECTION AND DOSIMETRY↗
Constraining Clouds and Convective Parameterizations in A Climate Model Using Paleoclimate Data
Cloud and convective parameterizations strongly influence uncertainties in equilibrium climate sensitivity. We provide a proof-of-concept study to constrain these parameterizations in a perturbed parameter ensemble of the atmosphere-only version of the Goddard Institute for Space Studies Model E2.1 simulations by evaluating model biases in the present-day runs using multiple satellite climatologies and by comparing simulated δ 18 O of precipitation (δ 18 O p ), known to be sensitive to parameterization schemes, with a global database of speleothem δ 18 O records covering the Last Glacial Maximum (LGM), mid-Holocene (MH) and pre-industrial (PI) periods. Relative to modern interannual variability, paleoclimate simulations show greater sensitivity to parameter changes, allowing for an evaluation of model uncertainties over a broader range of climate forcing and the identification of parts of the world that are parameter sensitive. Certain simulations reproduced absolute δ 18 O p values across all time periods, along with LGM and MH δ 18 O p anomalies relative to the PI, better than the default parameterization. No single set of parameterizations worked well in all climate states, likely due to the non-stationarity of cloud feedbacks under varying boundary conditions. Future work that involves varying multiple parameter sets simultaneously with coupled ocean feedbacks will likely provide improved constraints on cloud and convective parameterizations.
cloud and convective parameterization↗
Interlaboratory comparison of secondary ion mass spectrometry analysis results from the 7th international technical nuclear forensics working group collaborative material exercise
A review and interlaboratory comparison of secondary ion mass spectrometry (SIMS) data obtained by laboratories participating in the International Technical Nuclear Forensics Working Group (ITWG) 7th Collaborative Material Exercise (CMX-7) has been conducted. The analyzed materials were two uranium compounds in powder form and two pieces of uranium metal. The instruments used in this comparison were a small-geometry (SG) SIMS, CAMECA IMS 7f from the Research Centre Rez, and a large-geometry (LG) SIMS, CAMECA IMS 1280 from Los Alamos National Laboratory. Despite the differences in instruments and analytical procedures, e.g., sample preparation, SIMS setups, and data post-processing, there was good agreement for the 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios in the analyzed materials. The main difference was in the precision, which was, as expected, higher for the LG-SIMS. In addition, a comparison between the laboratories was also made for the image processing algorithms applied to raw data acquired in automated particle measurement (APM) mode. In conclusion, the result of this comparison has led to identification of best practices for setting up parameters of the APM software.
and nuclear chemistry↗
Striking Graphite Bearing Clasts Found in Two Ordinary Chondrite Samples; NWA6169 and NWA8330
Meteorites play an integral role in understanding the history of the solar system. Not only can they contain some of the oldest material found in the solar system they also can contain material that is unique. Many lithologies are only found as foreign clasts within distinctly different host meteorites. In this investigation two foreign clasts within the meteorites, NWA6169 and NWA8330 were studied. The purpose of this investigation was to examine the mineralogy and petrography of the clasts within the samples. From there an identification and possible origin were to be inferred. NWA6169 is an unclassified ordinary chondrite that has a presumed petrologic type of L3. NWA8330 is a classified ordinary chondrite that has a petrologic type of LL3. Both meteorites were found to contain clasts that were similar; both modally were comprised of about 5% acicular graphite. Through SEM and Raman Spectroscopy it was found that they contained olivine, pyroxene, plagioclase, Fe-Ni sulfides, graphite, and metals. They were found to portray an igneous texture with relationships that suggest concurrent growth. Analytical microprobe results for NWA6169 revealed mineral compositions of Fa31-34, Fs23-83, and Ab7-85. For NWA8330 these were Fa28-32, Fs10-24, and Ab4-83. Only one similar material has been reported, in the L3 chondrite Krymka (Semenenko & Girich, 1995). The clast they described exhibited similar mineralogies including the unusual graphite. Krymka data displayed compositional values of Fa28.5-35.0 and Fs9-25.9. These ranges are fairly similar to that of NWA6169 and NWA8330. These samples may all be melt clasts, probably of impact origin. Two possibilities are (1) impact of a C-type asteroid onto the L chondrite parent asteroid, and (2) a piece of proto-earth ejected from the moon-forming collision event. These possibilities present abundant questions, and can be tested. The measurement of oxygen isotope compositions from the clasts should reveal the original source of the melt clasts. It may also be possible to perform Ar dating of the plagioclase present. Former analyses are now being performed.
Johnson, Jessica M.↗
Annotation of DOM metabolomes with an ultrahigh resolution mass spectrometry molecular formula library
Current approaches to analyzing metabolomic data often rely on matching MS/MS fragmentation data to sparse libraries or databases. This approach results in limited identification of features, often with less than 10% of the dataset being annotated. A complementary approach is to assign molecular formula to features based on accurate mass measurements, but the platforms commonly used for metabolomics do not have the needed accuracy or resolving power to do this robustly, particularly for larger molecules. Using our newly modified analysis tool, CoreMS, we generated a library of molecular formula from pooled samples analyzed with LC-21T FT-ICR MS. This library successfully annotated approximately 53.2% of features identified from the exometabolome of marine diatom Phaeodactylum tricornutum – a nearly ten-fold increase over the 5.9% annotation rate achieved using a conventional MS/MS library matching approach. Using this FT-ICR MS library approach, we were able to differentiate differences in the exometabolome of P. tricornutum in iron replete and iron limited conditions, with 668 metabolites being differentially expressed (p < 0.05, 2 x intensity difference) under these conditions. The traditional MS/MS fragmentation-based annotation approach only annotated 61 of these metabolites, while our novel pipeline annotated 450 metabolites and revealed 12 metabolites that were significantly more abundant under low iron conditions. Our results demonstrate the utility of ultrahigh resolution mass spectrometry for generating more comprehensive and confident molecular annotations.
21T-FTICR-MS, CoreMS↗
Quantitative Assessment for Advanced Reactor Radioisotope Screening Utilizing a Heat Pipe Reactor Inventory
This report documents a method for the quantitative identification of radionuclides of potential interest for accident consequence analysis involving advanced nuclear reactors. Based on previous qualitative assessments of radionuclide inventories for advanced reactors coupled with the review of a radiological inventory developed for a heat pipe reactor, a 1 Ci activity airborne release was calculated for 137 radionuclides using the MACCS 4.1 code suite. Several assumptions regarding release conditions were made and discussed herein. The potential release of a heat pipe reactor inventory was also modeled following the same assumptions. Results provide an estimation of the relative EARLY and CHRONC phase dose contribution from advanced reactor radionuclides and are normalized to doses from equivalent releases of I-131 and Cs-137, respectively. Ultimately, a list of 69 radionuclides with EARLY or CHRONC dose contributions at least 1/100th that of I-131 or Cs-137, respectively – 48 of which are currently considered for LWR consequence analyses – was identified of being of potential importance for analyses involving a heat pipe reactor.
07 ISOTOPE AND RADIATION SOURCES↗
Ion Acceleration in Solar Flares
Solar flares are among the most energetic and interesting phenomena in the Solar system, releasing up to 1032 ergs of energy on timescales of several tens of seconds to several tens of minutes. Much of this energy is in the form of suprathermal electrons and ions, which remain trapped at the Sun and produce a wide variety of radiations, as well as escape into interplanetary space, where they can be directly observed. The radiation from trapped particles consists in general of (1) continuum emission; (2) narrow gamma-ray nuclear deexcitation lines; and (3) high-energy neutrons observed in space or by ground-based neutron monitors. The particles that escape into space consist of both electrons and ions, which often have compositions quite different than that of the ambient solar atmosphere. Flares thus present many diagnostics of the particle acceleration mechanism(s), the identification of which is the ultimate goal of flare research. Moreover, flares in fact offer the only opportunity in astrophysics to study the simultaneous energization of both electrons and ions. Hopefully, an understanding of flares with their wealth of diagnostic data will lead to a better understanding of particle acceleration at other sites in the Universe. It is now generally accepted that flares are roughly divided into two classes: impulsive and gradual. Gradual events are large, occur high in the corona, have long-duration soft and hard X-rays and gamma rays, are electron poor, are associated with Type II radio emission and coronal mass ejections (CMEs), and produce energetic ions with coronal abundance ratios. Impulsive events are more compact, occur lower in the corona, produce short-duration radiation, and exhibit dramatic abundance enhancements in the energetic ions. Their He-3/He-4 ratio is - 1, which is a huge increase over the coronal value of about 5 x 10(exp -4), and they also posses smaller but still significant enhancements of Ne, Mg, Si, and Fe relative to He-4, C, N, and O. Specifically, above about 1 MeV nucleon(exp -1), the ratio of Fe to O is about 8 times larger than in the corona or in gradual flares, while the ratio of Ne, Mg, and Si to O is about 3 times higher; He-4, C, N, and 0 are not enchanced with respect to each other. In addition to these elemental enhancements, Ne and Mg have isotopic enhancements as well. The general scenario that has emerged from these (and other) observations is that energetic particles in gradual events are accelerated by a CME-driven shock, while those particles in impulsive events are accelerated by another mechanism(s).
Miller, James A.↗
Integration of the QMSFRG Database into the HZETRN Code
Accurate nuclear interaction data bases are needed for describing the transport of space radiation in matter including space craft structures, atmospheres, and tissues. Transport models support the identification and development of new material concepts for human and electronic part protection. Quantum effects are manifested in nuclear reactions in several ways including interference effects between terms in the multiple scattering series, the many-body nuclear wave functions (for e.g. the roles of shell structure and Fermi momentum) and nuclear clustering. The quantum multiple scattering fragmentation model (QMSFRG) is a comprehensive model for generating nuclear interaction databases for galactic cosmic ray (GCR) transport. Other nuclear databases including the NUCFRG model and Monte-Carlo simulation codes such as FLUKA, LAHET, HETC, and GEANT ignore quantum effects. These codes fail to describe many important features of nuclear reactions and are thus inaccurate for the evaluation of materials for radiation protection. Previously we have shown that quantum effects are manifested through constructive interference in forward production spectra, the effects of Fermi momentum on production spectra, cluster nuclei knockout, and the nuclear response function. Quantum effects are especially important for heavy ions with mass numbers less than 20 that dominate radiation transport in human tissues and for the materials that are expected to be superior in space radiation protection. We describe the integration of the QMSFRG model into the HZETRN transport code. Integration milestones include proper treatment of odd-even charge-mass effects in nuclear fragmentation and the momentum distribution of nucleon production from GCR primary heavy ions. We have also modified the two-body amplitudes in the model to include nuclear medium effects. In order to include a comprehensive description of the GCR isotopic composition in materials, we have described the isotopic composition of the GCR by extending the 59-isotope version of HZETRN to an 120-isotope version. The isotopic composition of most primary GCR elements (including H, He, C, N, O, Ne, Mg, Si, Ar, Ca, Cr, and Fe) are included in the extended model. We discuss results for the high-energy neutron composition inside materials, and the charge and mass distribution for benchmark GCR problems.
Cucinotta, F. A.↗
Detection and Quantification of Nitrogen Compounds in Martian Solid Samples by the Sample Analysis at Mars (SAM) Instrument Suite
The Sample Analysis at Mars (SAM) instrument suite on the Mars Science Laboratory (MSL) Curiosity Rover detected both reduced and oxidized nitrogen-bearing compounds during the pyrolysis of surface materials from three sites at Gale Crater. Preliminary detections of nitrogen species include NO, HCN, ClCN, CH3CN, and TFMA (trifluoro-Nmethyl-acetamide). On Earth, nitrogen is a crucial bio-element, and nitrogen availability controls productivity in many environments. Nitrogen has also recently been detected in the form of CN in inclusions in the Martian meteorite Tissint, and isotopically heavy nitrogen (delta N-15 approx +100per mille) has been measured during stepped combustion experiments in several SNC meteorites. The detection of nitrogen-bearing compounds in Martian regolith would have important implications for the habitability of ancient Mars. However, confirmation of indigenous Martian nitrogen bearing compounds will require ruling out their formation from the terrestrial derivatization reagents (e.g. N-methyl-N-tert-butyldimethylsilyl-trifluoroacetamide, MTBSTFA and dimethylformamide, DMF) carried for SAM's wet chemistry experiment that contribute to the SAM background. The nitrogen species we detect in the SAM solid sample analyses can also be produced during laboratory pyrolysis experiments where these reagents are heated in the presence of perchlorate, a compound that has also been identified by SAM in Mars solid samples. However, this does not preclude a Martian origin for some of these compounds, which are present in nanomolar concentrations in SAM evolved gas analyses. Analysis of SAM data and laboratory breadboard tests are underway to determine whether nitrogen species are present at higher concentrations than can be accounted for by maximum estimates of nitrogen contribution from MTBSTFA and DMF. In addition, methods are currently being developed to use GC Column 6, (functionally similar to a commercial Q-Bond column), to separate and identify unretained compounds such as NO, N2O, and NO2, which are difficult to detect by EGA-MS due to mass interferences at 30, 44 and 46, respectively. Here we present evolved gas analysis-mass spectrometry (EGA-MS) and gas chromatography mass spectrometry (GC-MS) data on the identification and quantification of these nitrogen-bearing compounds, and suggestions for their origins
Stern, Jennifer C.↗
Volatile-rich Asteroids in the Inner Solar System
Bennu (101195), target of the Origins, Spectral Interpretation, Resource Identification, Security, Regolith Explorer (OSIRIS-REx) mission, is a type-B asteroid with abundant spectral evidence for hydrated silicates, low thermal inertia “boulders” and frequent bursts of particle emission. We suggest that Bennu’s parent body formed in the outer solar system before it was perturbed into the asteroid belt and then evolved into a near-Earth object. We show that this is consistent with models of planetesimal evolution. Bennu has many characteristics expected for a dormant comet, and could potentially contain a minimum of 1 wt.% adsorbed water if its gross mineralogy is consistent with the Orgueil meteorite. This is in addition to any ice or water contained within the hydrous minerals themselves. Based on this hypothesis, we predict the properties of the samples that will be returned to Earth by the OSIRIS-REx mission, including abundant phyllosilicate minerals, amorphous hydrated silicates and low-density, very high-porosity aggregates, already observed by the OSIRIS-REx instrument suite. We predict enrichments in D/H and 15N/14N, high C/Mg ratios (>∼7 wt%), and a greater range of organic compositions than found in meteorites, including an organic component poor in aromatics, and a more labile organic fraction. Ammonium salts, ranging from NH4Cl to ammonium–organic acid salts could carry much of the nitrogen in comets, yet only NH4CH3COO and heavier salts are sufficiently stable to be found in these returned samples. Water adsorbed onto highly porous grains should also be detected provided that the sample return capsule remains below 300 K during Earth return, and this water should be isotopically heavy.
Joseph A. Nuth, III↗
Explaining machine-learning models for gamma-ray detection and identification
As more complex predictive models are used for gamma-ray spectral analysis, methods are needed to probe and understand their predictions and behavior. Recent work has begun to bring the latest techniques from the field of Explainable Artificial Intelligence (XAI) into the applications of gamma-ray spectroscopy, including the introduction of gradient-based methods like saliency mapping and Gradient-weighted Class Activation Mapping (Grad-CAM), and black box methods like Local Interpretable Model-agnostic Explanations (LIME) and SHapley Additive exPlanations (SHAP). In addition, new sources of synthetic radiological data are becoming available, and these new data sets present opportunities to train models using more data than ever before. In this work, we use a neural network model trained on synthetic NaI(Tl) urban search data to compare some of these explanation methods and identify modifications that need to be applied to adapt the methods to gamma-ray spectral data. We find that the black box methods LIME and SHAP are especially accurate in their results, and recommend SHAP since it requires little hyperparameter tuning. We also propose and demonstrate a technique for generating counterfactual explanations using orthogonal projections of LIME and SHAP explanations.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Thermally Stable Co@C3N4 Single-Atom Catalysts for CO Oxidation: Atomic-Level Insights into Structure and Activity
Single Co atoms supported on C3N4 (Co@C3N4) have demonstrated high activity and selectivity in photocatalysis. However, the investigation of structure–function relationships and reaction mechanisms under photocatalytic conditions is very challenging due to the complex conditions of light absorption, charge transfer, and catalysis. In this study, we employed thermal CO oxidation as a prototypical probe reaction to benchmark the intrinsic catalytic performance and track the active-site evolution of Co@C3N4. Single Co atoms were identified and shown to be the catalytically active sites for CO oxidation based on control experiments and isotope-labeling experiments. The Co sites remained atomically dispersed before, during, and after the reaction with temperatures up to 400 °C, as established by in situ X-ray absorption fine structure (XAFS) combined with density functional theory (DFT), FDMNES simulations, and dynamic-time-warping (DTW)-assisted X-ray absorption near edge structure (XANES) matching. Together with theoretical calculations, the integrated analysis reveals a stable coordination environment under reaction conditions, which correlates with sustained activity, establishing Co@C3N4 single-atom catalysts as thermally stable CO oxidation catalysts. Beyond these findings, the current study provides a workflow for unambiguously assigning active sites in Co@C3N4 for thermal CO oxidation. This workflow will aid the understanding of their behavior in photocatalysis in the future, where light-driven dynamics obscure direct structure–function links. Notably, this study provides fundamental insights for the rational design of robust single-atom catalysts and a foundation for the broader application of Co@C3N4 catalysts in oxidation reactions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Time projection chamber for GADGET II
The established Gaseous Detector with Germanium Tagging (GADGET) detection system is used to measure weak, low-energy 𝛽-delayed proton decays. It consists of the Gaseous Proton Detector equipped with a MICROMEGAS (MM) readout to detect protons and other charged particles calorimetrically, surrounded by the Segmented Germanium Array (SeGA) for high-resolution detection of prompt 𝛾 rays. To upgrade GADGET's Proton Detector to operate as a compact time projection chamber (TPC) for the detection, three-dimensional imaging and identification of low-energy 𝛽-delayed single- and multiparticle emissions mainly of interest to astrophysical studies. A new high granularity MM board with 1024 pads has been designed, fabricated, installed, and tested. A high-density data acquisition system based on generic electronics for TPCs (GET) has been installed and optimized to record and process the gas avalanche signals collected on the readout pads. The TPC's performance has been tested using a 220 Rn 𝛼-particle source and cosmic-ray muons. In addition, decay events in the TPC have been simulated by adapting the attpcroot data analysis framework. Furthermore, a novel application of two-dimensional convolutional neural networks for GADGET II event classification is introduced. The optimization of data throughput is also addressed. The GADGET II TPC is capable of detecting and identifying 𝛼 particles as well as measuring their track direction, range, and energy. The extracted energy resolution of the GADGET II TPC using P10 gas is about 5.4% at 6.288 MeV ( 220 Rn 𝛼 events), computed using charge integration. Based on a systematic simulation study, we estimated the detection efficiency of the GADGET II TPC for protons and 𝛼 particles, respectively. It has also been demonstrated that the GADGET II TPC is capable of tracking minimum-ionizing particles (i.e., cosmic-ray muons). From these measurements, the electron drift velocity was measured under typical operating conditions. In addition to being one of the first generation of micropattern gaseous detectors (MPGDs) to utilize a resistive anode applied to low-energy nuclear physics, the GADGET II TPC will also be the first TPC surrounded by a high-efficiency array of high-purity germanium 𝛾-ray detectors. As a result, the TPC of GADGET II has been designed, fabricated, and tested and is ready for operation at the Facility for Rare Isotope Beams for radioactive-beam-line experiments.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗