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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Machine-Learning Architecture for Ultrasonic Thermometry

Temperature distribution in solids can be inverted from the speed of sound (SOS) measurements, as has been shown feasible by timing the propagation of the excitation pulse and the train of echoes in ultrasonically segmented waveguides (WGs) and metal components. However, complicated geometries and closely-space echogenic features (EFs) create complex waveforms, from which the segmental time of flights (TOFs) are impossible to estimate using traditional methods. This work describes a machine learning architecture shown to extract temperature information from complex ultrasonic waveforms without explicit measurements of segmental TOFs. We accomplish this by using an autoencoder neural network (NN) to map ultrasonic waveforms into a low-dimensional latent space. A second NN then maps the latent space into unknown temperature distribution along the WG. The proposed architecture was tested in simulations and experimentally. The autoencoder accurately reconstructs the waveforms from their latent representation, several orders of magnitude lower in dimensionality. The obtained latent space was successfully mapped into the temperature of the propagation path.

John, Mason↗
DOE OSTI2020

Comparison of PID Shunting in Polycrystalline and Single-Crystal Silicon Modules via Multi-Scale, Multi-Technique Characterization

We used the methods we reported last year to investigate potential-induced degradation (PID). We have now applied these methods to single-crystalline silicon modules that have degraded during field deployment, as well as in minimodules stressed in the laboratory. We will compare these results to the polycrystalline results presented last year. Small cores have been removed from the modules and subjected to analysis. We use a combination of photoluminescence and dark lock-in thermography imaging, laser marking, electron-beam induced current measurements, and subsequent focused ion-beam marking to allow analysis of individual defects via time-of-flight secondary-ion mass spectrometry (TOF-SIMS) to investigate the root-cause mechanism for PID shunting. We see a direct correlation between recombination active shunts and sodium content. The sodium content in shunted areas peaks at the SiN/Si interface and is consistently observed at a concentration of 0.1%-1% in shunted areas. TOF-SIMS data taken on degraded and non-degraded single-crystalline sample areas show a similar trend as in the polycrystalline samples: more sodium is seen in the degraded areas.

14 SOLAR ENERGY↗
DOE OSTI2012

Surface characterization of Zr/Ti/Nb tri-layered films deposited by magnetron sputtering on Si(111) and stainless steel substrates

Among metallic materials, commercially pure titanium and titanium alloys are very often used as biomaterials for implants. Among these alloys, titanium-aluminum-vanadium alloy Ti-6 A-4 V is one of the most commonly used due to its excellent biocompatibility and ability to allow bone-implant integration. A new class of Ti alloys employs Zr for solid-solution hardening and Nb as {beta}-phase stabilizer. Metals such as Ti, Nb, and Zr-known as valve metals-usually have their surfaces covered by a thin oxide film that forms spontaneously in air. This oxide film constitutes a barrier between the metal and the medium. The Ti-Nb-Zr alloys have mechanical and corrosion resistance characteristics which make them suitable for use as implants. Tri-layered films of Ti-Nb-Zr were deposited on both Si(111) and stainless steel (SS) substrates using dc magnetron sputtering equipment, under an argon atmosphere according to the following methodology: a 100 nm thick layer of Nb was deposited on the substrate, followed by a 200 nm thick layer of Ti, and finally a 50 nm thick layer of Zr, on top of the multilayer stack. The morphology and chemical composition of the films were analyzed by atomic force microscopy (AFM), x-ray photoelectron spectroscopy (XPS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS). AFM images showed that the Zr/Ti/Nb tri-layer films presented nanostructured grains and low roughness. The ToF-SIMS depth profiles confirmed the formation of a three-layered film on Si(111) with well-defined and sharp interfaces between the layers, while the deposition on the stainless steel substrate caused slight intermixing at the different alloy/Nb, Nb/Ti and Ti/Zr interfaces, reflecting the greater roughness of the raw substrate. The XPS results for the Zr/Ti/Nb layers deposited on Si(111) and SS confirmed that the outermost layer consisted of Zr only, with a predominance of ZrO{sub 2}, as the metal layer is passivated in air. An oxidation treatment of 1000 Degree-Sign C in air for 1 h for the multilayer stacks caused some dewetting with Si(111) films, and alloying in the layers. The latter effect was more pronounced for the stainless steel substrate.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Studies on atomic layer deposition of IRMOF-8 thin films

Deposition of IRMOF-8 thin films by atomic layer deposition was studied at 260–320 °C. Zinc acetate and 2,6-naphthalenedicarboxylic acid were used as the precursors. The as-deposited amorphous films were crystallized in 70% relative humidity at room temperature resulting in an unknown phase with a large unit cell. An autoclave with dimethylformamide as the solvent was used to recrystallize the films into IRMOF-8 as confirmed by grazing incidence x-ray diffraction. The films were further characterized by high temperature x-ray diffraction (HTXRD), field emission scanning electron microscopy, Fourier transform infrared spectroscopy (FTIR), time-of-flight elastic recoil detection analysis (TOF-ERDA), nanoindentation, and energy-dispersive x-ray spectroscopy. HTXRD measurements revealed similar behavior to bulk IRMOF-8. According to TOF-ERDA and FTIR, composition of the films was similar to IRMOF-8. Through-porosity was confirmed by loading the films with palladium using Pd(thd){sub 2} (thd = 2,2,6,6-tetramethyl-3,5-heptanedionato) as the precursor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantitative evaluation of perfluorinated alkanethiol molecular order on gold surfaces

Self-assembled monolayers (SAMs) of perfluoroalkanethiols [CF3(CF2)xCH2CH2SH (x = 3, 5, 7, and 9)] on gold were characterized by x-ray photoelectron spectroscopy (XPS), near edge x-ray absorption fine structure (NEXAFS), and static time-of-flight secondary ion mass spectrometry (ToF-SIMS). Perfluoroalkanethiols of several chain lengths were synthesized using a known hydride reduction method for transforming commercially available perfluoroalkyliodides to corresponding perfluoroalkanethiols. This strategy provides improved product yields compared to other known routes based on hydrolysis from the common thioacetyl perfluoroalkyl intermediate. Angle-dependent XPS analysis revealed that CF3(CF2)xCH2CH2SH (x = 5, 7, and 9; F6, F8, and F10, respectively) SAMs on gold exhibited significant enrichment of the terminal CF3 group at the outer monolayer surface with the sulfur present as a metal-bound thiolate located at the monolayer-gold interface. XPS of the CF3(CF2)3CH2CH2SH (F4) monolayer revealed a thin film with a significant (>50%) amount of hydrocarbon contamination consistent with poorly organized monolayers, while the longest thiol (F10) showed XPS signals attributed to substantial ordering and anisotropy. ToF-SIMS spectra from all four SAMs contained molecular ions representative of the particular perfluorinated thiol used to prepare the monolayer. NEXAFS methods were used to determine degrees of ordering and average tilt for molecules comprising monolayers. The SAMs prepared from the longest (F10) thiols exhibited the highest degree of ordering with the molecular axis nearly perpendicular to the gold surface. The degree of ordering decreased significantly with decreasing length of the perfluorocarbon tail.

Biophysics↗
DOE OSTI2020

Results from the Advanced Scintillator Compton Telescope (ASCOT) Balloon Payload

The Advanced Scintillator Compton Telescope (ASCOT) is a medium-energy gamma-ray Compton telescope flown on NASA’s high-altitude scientific balloon from Palestine, TX on 5th July 2018. It uses commercially available highperformance scintillators like Cerium Bromide (CeBr3) and p-terphenyl along with compact readout devices - silicon photomultipliers (SiPMs) - for an improved instrument response. ASCOT was built to address the existing need for observations in the gamma-ray energy range of 0.4 - 20 MeV. Operating stably throughout the mission, it reached an altitude of 120,000 ft and observed the Crab Nebula at MeV energies for ~5 hours. Built on the legacy of COMPTEL (onboard CGRO), along with the hardware advancement ASCOT also makes use of the Time-of-Flight (ToF) background rejection technique for effective imaging. Presented here is the Energy and ToF calibrated flight data with optimal data cuts (Earth Horizon Cut, Pulse Shape Discrimination Cut). The growth curves generated using this data from 5 to 100 g/cm2 of residual atmosphere in conjunction with the Monte Carlo simulations of the instrument response have been used to obtain the Cosmic Diffuse Gamma-ray (CDG) flux value of (1.28 ± 0.37)×10 -5 photons/cm 2 /s/sr/keV for 0.4 – 0.7 MeV energy range. The 3σ upper limit for CDG flux is 1.8×10-5 photons/cm 2 /s/sr/keV for 0.7-1.5 MeV and 2×10-6 photons/cm2/s/sr/keV for 1.5-2.5 MeV. The analysis of the Crab Nebula from flight observation is underway

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2012

Fast time-of-flight camera based surface registration for radiotherapy patient positioning

Purpose: This work introduces a rigid registration framework for patient positioning in radiotherapy, based on real-time surface acquisition by a time-of-flight (ToF) camera. Dynamic properties of the system are also investigated for future gating/tracking strategies. Methods: A novel preregistration algorithm, based on translation and rotation-invariant features representing surface structures, was developed. Using these features, corresponding three-dimensional points were computed in order to determine initial registration parameters. These parameters became a robust input to an accelerated version of the iterative closest point (ICP) algorithm for the fine-tuning of the registration result. Distance calibration and Kalman filtering were used to compensate for ToF-camera dependent noise. Additionally, the advantage of using the feature based preregistration over an ''ICP only'' strategy was evaluated, as well as the robustness of the rigid-transformation-based method to deformation. Results: The proposed surface registration method was validated using phantom data. A mean target registration error (TRE) for translations and rotations of 1.62 {+-} 1.08 mm and 0.07 deg. {+-} 0.05 deg., respectively, was achieved. There was a temporal delay of about 65 ms in the registration output, which can be seen as negligible considering the dynamics of biological systems. Feature based preregistration allowed for accurate and robust registrations even at very large initial displacements. Deformations affected the accuracy of the results, necessitating particular care in cases of deformed surfaces. Conclusions: The proposed solution is able to solve surface registration problems with an accuracy suitable for radiotherapy cases where external surfaces offer primary or complementary information to patient positioning. The system shows promising dynamic properties for its use in gating/tracking applications. The overall system is competitive with commonly-used surface registration technologies. Its main benefit is the usage of a cost-effective off-the-shelf technology for surface acquisition. Further strategies to improve the registration accuracy are under development.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

SU-E-J-184: Stereo Time-Of-Flight System for Patient Positioning in Radiotherapy

Purpose: The objective of this work is to test the advantage of using the surface acquired by two stereo Time-of-Flight (ToF) cameras in comparison of the use of one camera only for patient positioning in radiotherapy. Methods: A first step consisted on validating the use of a stereo ToFcamera system for positioning management of a phantom mounted on a linear actuator producing very accurate and repeatable displacements. The displacements between two positions were computed from the surface point cloud acquired by either one or two cameras thanks to an iterative closest point algorithm. A second step consisted on determining the displacements on patient datasets, with two cameras fixed on the ceiling of the radiotherapy room. Measurements were done first on voluntary subject with fixed translations, then on patients during the normal clinical radiotherapy routine. Results: The phantom tests showed a major improvement in lateral and depth axis for motions above 10 mm when using the stereo-system instead of a unique camera (Fig1). Patient measurements validate these results with a mean real and measured displacement differences in the depth direction of 1.5 mm when using one camera and 0.9 mm when using two cameras (Fig2). In the lateral direction, a mean difference of 1 mm was obtained by the stereo-system instead of 3.2 mm. Along the longitudinal axis mean differences of 5.4 and 3.4 mm with one and two cameras respectively were noticed but these measurements were still inaccurate and globally underestimated in this direction as in the literature. Similar results were also found for patient subjects with a mean difference reduction of 35%, 7%, and 25% for the lateral, depth, and longitudinal displacement with the stereo-system. Conclusion: The addition of a second ToF-camera to determine patient displacement strongly improved patient repositioning results and therefore insures better radiation delivery.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2014

A system to detect cerebral aneurysms in multimodality angiographic data sets

Purpose: The early detection of cerebral aneurysms plays a major role in preventing subarachnoid hemorrhage. The authors present a system to automatically detect cerebral aneurysms in multimodal 3D angiographic data sets. The authors’ system is parametrizable for contrast-enhanced magnetic resonance angiography (CE-MRA), time-of-flight magnetic resonance angiography (TOF-MRA), and computed tomography angiography (CTA). Methods: Initial volumes of interest are found by applying a multiscale sphere-enhancing filter. Several features are combined in a linear discriminant function (LDF) to distinguish between true aneurysms and false positives. The features include shape information, spatial information, and probability information. The LDF can either be parametrized by domain experts or automatically by training. Vessel segmentation is avoided as it could heavily influence the detection algorithm. Results: The authors tested their method with 151 clinical angiographic data sets containing 112 aneurysms. The authors reach a sensitivity of 95% with CE-MRA data sets at an average false positive rate per data set (FP{sub DS}) of 8.2. For TOF-MRA, we achieve 95% sensitivity at 11.3 FP{sub DS}. For CTA, we reach a sensitivity of 95% at 22.8 FP{sub DS}. For all modalities, the expert parametrization led to similar or better results than the trained parametrization eliminating the need for training. 93% of aneurysms that were smaller than 5 mm were found. The authors also showed that their algorithm is capable of detecting aneurysms that were previously overlooked by radiologists. Conclusions: The authors present an automatic system to detect cerebral aneurysms in multimodal angiographic data sets. The system proved as a suitable computer-aided detection tool to help radiologists find cerebral aneurysms.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

CHERENCUBE: Concept definition and implementation challenges of a Cherenkov-based detector block for PET

Purpose: A new concept for a depth-of-interaction (DOI) capable time-of-flight (TOF) PET detector is defined, based only on the detection of Cherenkov photons. The proposed “CHERENCUBE” consists of a cubic Cherenkov radiator with position-sensitive photodetectors covering each crystal face. By means of the spatial distribution of the detected photons and their time of arrival, the point of interaction of the gamma-ray in the crystal can be determined. This study analyzes through theoretical calculations and Monte Carlo simulations the potential advantages of the concept toward reaching a Cherenkov-only detector for TOF-PET with DOI capability. Furthermore, an algorithm for the DOI estimation is presented and the requirements for a practical implementation of the proposed concept are defined. Methods: The Monte Carlo simulations consisted of a cubic crystal with one photodetector coupled to each one of the faces of the cube. The sensitive area of the detector matched exactly the crystal size, which was varied in 1 mm steps between 1 × 1 × 1 mm{sup 3} and 10 × 10 × 10 mm{sup 3}. For each size, five independent simulations of ten thousand 511 keV gamma-rays were triggered at a fixed distance of 10 mm. The crystal chosen was PbWO{sub 4}. Its scintillation properties were simulated, but only Cherenkov photons were analyzed. Photodetectors were simulated having perfect photodetection efficiency and infinite time resolution. For every generated particle, the analysis considered its creation process, parent and daughter particles, energy, origin coordinates, trajectory, and time and position of detection. The DOI determination is based on the distribution of the emission time of all photons per event. These values are calculated as a function of the coordinates of detection and origin for every photon. The common origin is estimated by finding the distribution with the most similar emission time-points. Results: Detection efficiency increases with crystal size from 8.2% (1 × 1 × 1 mm{sup 3}) to 58.6% (10 × 10 × 10 mm{sup 3}) and decreases applying a photon detection threshold of 5/10/20 photons to 6.3%/4.3%/0.7% and 49.3%/30.4%/2.8%, respectively. The detection rate in the six photodetectors is uniform due to the nearly isotropic cone emission. Most cones originated after a photoelectric effect interaction, with two dominating peaks for the kinetic energy of the electron at 422.99 and 441.47 keV. The detection distance between same-event photons defines the spatial resolution of the detector required for individual photon recognition, with 20% of the detected photons having their closest neighbor within a distance of 5% of the length of the cube. Same-event photons are detected within a time window whose width is determined by the crystal size, with values of 30 and 150 ps for a 1 × 1 × 1 mm{sup 3} and a 10 × 10 × 10 mm{sup 3} cube, respectively. The DOI reconstruction has an accuracy of approximately 23% of the length of the cube, with an average value of 2.2 mm for a 10 × 10 × 10 mm{sup 3} CHERENCUBE. Conclusions: The proposed concept requires a detector with high photodetection efficiency. The structure of the sensitive surface of the detector should be a two dimensional array of microcells, able to provide individual detection coordinates and time stamps. The microcell size determines the ability to recognize individual photons, influencing detection efficiency. The 3D DOI recognition relies on the accuracy of the time stamps and detection coordinates, without the need for a recognition of the projected patterns of photons. The refractive index of the material defines a detector intrinsic energy-based rejection of scattered PET events at the cost of reduced sensitivity.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Investigating the limits of PET/CT imaging at very low true count rates and high random fractions in ion-beam therapy monitoring

Purpose: External beam radiotherapy with protons and heavier ions enables a tighter conformation of the applied dose to arbitrarily shaped tumor volumes with respect to photons, but is more sensitive to uncertainties in the radiotherapeutic treatment chain. Consequently, an independent verification of the applied treatment is highly desirable. For this purpose, the irradiation-induced β{sup +}-emitter distribution within the patient is detected shortly after irradiation by a commercial full-ring positron emission tomography/x-ray computed tomography (PET/CT) scanner installed next to the treatment rooms at the Heidelberg Ion-Beam Therapy Center (HIT). A major challenge to this approach is posed by the small number of detected coincidences. This contribution aims at characterizing the performance of the used PET/CT device and identifying the best-performing reconstruction algorithm under the particular statistical conditions of PET-based treatment monitoring. Moreover, this study addresses the impact of radiation background from the intrinsically radioactive lutetium-oxyorthosilicate (LSO)-based detectors at low counts. Methods: The authors have acquired 30 subsequent PET scans of a cylindrical phantom emulating a patientlike activity pattern and spanning the entire patient counting regime in terms of true coincidences and random fractions (RFs). Accuracy and precision of activity quantification, image noise, and geometrical fidelity of the scanner have been investigated for various reconstruction algorithms and settings in order to identify a practical, well-suited reconstruction scheme for PET-based treatment verification. Truncated listmode data have been utilized for separating the effects of small true count numbers and high RFs on the reconstructed images. A corresponding simulation study enabled extending the results to an even wider range of counting statistics and to additionally investigate the impact of scatter coincidences. Eventually, the recommended reconstruction scheme has been applied to exemplary postirradiation patient data-sets. Results: Among the investigated reconstruction options, the overall best results in terms of image noise, activity quantification, and accurate geometrical recovery were achieved using the ordered subset expectation maximization reconstruction algorithm with time-of-flight (TOF) and point-spread function (PSF) information. For this algorithm, reasonably accurate (better than 5%) and precise (uncertainty of the mean activity below 10%) imaging can be provided down to 80 000 true coincidences at 96% RF. Image noise and geometrical fidelity are generally improved for fewer iterations. The main limitation for PET-based treatment monitoring has been identified in the small number of true coincidences, rather than the high intrinsic random background. Application of the optimized reconstruction scheme to patient data-sets results in a 25% − 50% reduced image noise at a comparable activity quantification accuracy and an improved geometrical performance with respect to the formerly used reconstruction scheme at HIT, adopted from nuclear medicine applications. Conclusions: Under the poor statistical conditions in PET-based treatment monitoring, improved results can be achieved by considering PSF and TOF information during image reconstruction and by applying less iterations than in conventional nuclear medicine imaging. Geometrical fidelity and image noise are mainly limited by the low number of true coincidences, not the high LSO-related random background. The retrieved results might also impact other emerging PET applications at low counting statistics.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2016

A combined time-of-flight and depth-of-interaction detector for total-body positron emission tomography

Purpose: In support of a project to build a total-body PET scanner with an axial field-of-view of 2 m, the authors are developing simple, cost-effective block detectors with combined time-of-flight (TOF) and depth-of-interaction (DOI) capabilities. Methods: This work focuses on investigating the potential of phosphor-coated crystals with conventional PMT-based block detector readout to provide DOI information while preserving timing resolution. The authors explored a variety of phosphor-coating configurations with single crystals and crystal arrays. Several pulse shape discrimination techniques were investigated, including decay time, delayed charge integration (DCI), and average signal shapes. Results: Pulse shape discrimination based on DCI provided the lowest DOI positioning error: 2 mm DOI positioning error was obtained with single phosphor-coated crystals while 3–3.5 mm DOI error was measured with the block detector module. Minimal timing resolution degradation was observed with single phosphor-coated crystals compared to uncoated crystals, and a timing resolution of 442 ps was obtained with phosphor-coated crystals in the block detector compared to 404 ps without phosphor coating. Flood maps showed a slight degradation in crystal resolvability with phosphor-coated crystals; however, all crystals could be resolved. Energy resolution was degraded by 3%–7% with phosphor-coated crystals compared to uncoated crystals. Conclusions: These results demonstrate the feasibility of obtaining TOF–DOI capabilities with simple block detector readout using phosphor-coated crystals.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Deciphering the effect of traps on electronic charge transport properties of methylammonium lead tribromide perovskite

Halide perovskites have undergone remarkable developments as highly efficient optoelectronic materials for a variety of applications. Several studies indicated the critical role of defects on the performance of perovskite devices. However, the parameters of defects and their interplay with free charge carriers remain unclear. In this study, we explored the dynamics of free holes in methylammonium lead tribromide (MAPbBr 3 ) single crystals using the time-of-flight (ToF) current spectroscopy. By combining ToF spectroscopy and Monte Carlo simulation, three energy states were detected in the bandgap of MAPbBr 3 . In addition, we found the trapping and detrapping rates of free holes ranging from a few microseconds to hundreds of microseconds. Contrary to previous studies, we revealed a strong detrapping activity of traps. We showed that these traps substantially affect the transport properties of MAPbBr 3 , including mobility and mobility-lifetime product. Our results provide an insight on charge transport properties of perovskite semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Imaging Bragg Edge Analysis TooLs for Engineering Structures (iBeatles)

The Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL) provides pulsed neutrons with energies varying from epithermal to cold. In preparation for VENUS, the neutron imaging beamline to be located at beam port 10, we have performed a series of experiments focused on wavelength-dependent radiography and computed tomography for a broad range of applications, from materials science to biological tissues.One of the time-of-flight (TOF) techniques that is of interest to the scientific community is the 2-dimensional mapping of phases and average crystalline plane orientation in samples both ex-situ and during applied stresses such as tensile loading and heating. This technique is known as Bragg edgeimaging and relies on the identification of changes of transmission values, fitting of the edge to measure its displacement, and thus identify the shift in lattice parameter due to stresses. One of the challenges of TOF imaging measurements is the amount of data and the inability to observe Bragg edge shifts in real time during an experiment. Thus, we have been focusing on creating a Python-based interface that allows fast data processing and instantaneous mapping and fitting of the Bragg edges, and their evolution through time. Python libraries and Jupyter notebooks have been implemented to facilitate decision making during an experiment. The advantage of the notebooks is the possibility to guide an experiment as they can quickly process and display Bragg edge data. These notebooks can be used independently, or can be combined in a Python Graphical User Interface (GUI) tool called iBeatles. This interface permits visualization and fitting of the Bragg edges, and ultimately back-projects the fitting results onto the radiographs to display a strain map. Assuming data collection has sufficient statistics, the strain mapping analysis can be performed on a pixel-by-pixel basis. This development is a step forward toward a better user experience at the future VENUS beamline in terms of live feedback and productivity. Analysis that used to take days of switching between different applications can now be done in minutes within the

Bilheux, JeanChristophe [Oak Ridge National Labora↗
DOE OSTI2024

Acoustic sensing and autoencoder approach for abnormal gas detection in a spent nuclear fuel canister mock-up

Currently, spent nuclear fuel (SNF) from commercial nuclear power plants is stored in stainless-steel canisters for interim dry storage. To provide an inert environment, these canisters are backfilled with helium after vacuum drying. However, the helium environment may be contaminated during extended storage because of the material degradation. For example, the heavier fission gas xenon may be released from the fuel rods into the canister cavity should the fuel cladding be breached. Other gases such as air and water vapor may also be present as a result of leakage caused by chloride-induced stress corrosion cracking on the canister walls or by insufficient vacuum drying. Therefore, monitoring the gas composition can provide critical information about the health of SNF canisters. In this study, noninvasive testing was conducted on a 2/3-scaled SNF canister mock-up using acoustic sensing. Ultrasonic transducers were placed on the exterior surface of the canister to probe the gas composition. A dataset was collected by sealing the canister mock-up and introducing up to 1.53% argon or 1.29% air into the helium background gas. Three methods were used to detect changes in the gas composition: the time-of-flight (TOF) method, the differential method, and the autoencoder method. Results showed that the TOF method had sufficient resolution to detect abnormal gas concentrations of less than 1.0%. The differential method demonstrated a periodic in-phase and out-of-phase behavior between the benchmark (i.e., pure helium) and abnormal (i.e., with argon or air) state signals. The variational autoencoder (VAE) and the Wasserstein autoencoder (WAE) were trained on the benchmark data and were applied directly to the abnormal state data. It was found that both the unsupervised VAE and the WAE were able to distinguish the benchmark and abnormal states of the canister mock-up based on the reconstruction error.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Locating Methyl-Etherified and Methyl-Esterified Uronic Acids in the Plant Cell Wall Pectic Polysaccharide Rhamnogalacturonan II

Rhamnogalacturonan II (RG-II) is a structurally complex pectic polysaccharide that exists as a borate ester cross-linked dimer in the cell walls of all vascular plants. The glycosyl sequence of RG-II is largely conserved, but there is evidence that galacturonic acid (GalA) methyl etherification and glucuronic acid (GlcA) methyl esterification vary in the A sidechain across plant species. Methyl esterification of the galacturonan backbone has also been reported but not confirmed. Here we describe a new procedure, utilizing aq. sodium borodeuteride (NaBD4)-reduced RG-II, to identify the methyl esterification status of backbone GalAs. Our data suggest that up to two different GalAs are esterified in the RG-II backbone. We also adapted a procedure based on methanolysis and NaBD4 reduction to identify 3-, 4-, and 3,4-O-methyl GalA in RG-II. These data, together with matrix-assisted laser desorption/ionization–time-of-flight mass spectrometry (MALDI-TOF) MS analysis of sidechain A generated from selected RG-IIs and their NaBD4-reduced counterparts, suggest that methyl etherification of the ß-linked GalA and methyl esterification of the GlcA are widespread. Nevertheless, the extent of these modifications varies between plant species. Our analysis of the sidechain B glycoforms in RG-II from different dicots and nonpoalean monocots suggests that this sidechain has a minimum structure of an O-acetylated hexasaccharide (Ara-[MeFuc]-Gal-AceA-Rha-Api-). To complement these studies, we provide further evidence showing that dimer formation and stability in vitro is cation and borate dependent. Taken together, our data further refine the primary sequence and sequence variation of RG-II and provide additional insight into dimer stability and factors controlling dimer self-assembly.

BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Initial experience with a SiPM-based PET/CT scanner: influence of acquisition time on image quality

Background: A newly introduced PET/CT scanner (Discovery Meaningful Insights—DMI, GE Healthcare) includes the silicon photomultiplier (SiPM) with timeof-flight (TOF) technology first used in the GE SIGNA PET/MRI. In this study, we investigated the impact of various acquisition times on image quality using this SiPM-based PET/CT. Methods: We reviewed data from 58 participants with cancer who were scanned using the DMI PET/CT scanner. The administered dosages ranged 295.3–429.9 MBq (mean ± SD 356.3 ± 37.4) and imaging started at 71–142 min (mean ± SD 101.41 ± 17. 52) after administration of the radiopharmaceutical. The patients’ BMI ranged 19.79–46. 16 (mean ± SD 26.55 ± 5.53). We retrospectively reconstructed the raw TOF data at 30, 60, 90, and 120 s/bed and at the standard image acquisition time per clinical protocol (180 or 210 s/bed depending on BMI). Each reconstruction was reviewed blindly by two nuclear medicine physicians and scored 1–5 (1—poor, 5—excellent quality). The liver signal-to-noise ratio (SNR) was used as a quantitative measure of image quality. Results: The average scores ± SD of the readers were 2.61 ± 0.83, 3.70 ± 0.92, 4.36 ± 0.82, 4.82 ± 0.39, and 4.91 ± 0.91 for the 30, 60, 90, and 120 s/bed and at standard acquisition time, respectively. Inter-reader agreement on image quality assessment was good, with a weighted kappa of 0.80 (95% CI 0.72–0.81). In the evaluation of the effects of time per bed acquisition on semi-quantitative measurements, we found that the only time point significantly different from the standard time were 30 and 60 s (both with P < 0.001). The effects of dose and BMI were not statistically significant (P = 0.195 and 0.098, respectively). There was a significant positive effect of time on SNR (P < 0.001), as well as a significant negative effect of weight (P < 0.001). Conclusions: Our results suggest that despite significant delays from injection to imaging (due to comparison with standard PET/CT) compared to standard clinical operations and even in a population with average BMI > 25, images can be acquired as fast as 90 s/bed using the SiPM PET/CT and still result in very good image quality (average score > 4).

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2020

Data from A Mass Spectrometry-Based High-Throughput Screening Method for Engineering Fatty Acid Synthases with Improved Production of Medium Chain Fatty Acids

Microbial cell factories have been extensively engineered to produce free fatty acids (FFAs) as key components of crucial nutrients, soaps, industrial chemicals, and fuels. However, our ability to control the composition of microbially synthesized FFAs is still limited, particularly, for producing medium‐chain fatty acids (MCFAs). This is mainly due to the lack of high‐throughput approaches for FFA analysis to engineer enzymes with desirable product specificity. Here we report a mass spectrometry (MS)‐based method for rapid profiling of MCFAs in Saccharomyces cerevisiae by using membrane lipids as a proxy. In particular, matrix‐assisted laser desorption/ionization time‐of‐flight (MALDI‐ToF) MS was used to detect shorter acyl chain phosphatidylcholines from membrane lipids and a higher m/z peak ratio at 730 and 758 was used as an indication for improved MCFA production. This colony‐based method can be performed at a rate of ~2 s per sample, representing a substantial improvement over gas chromatography‐MS (typically >30 min per sample) as the gold standard method for FFA detection. To demonstrate the power of this method, we performed site‐saturation mutagenesis of the yeast fatty acid synthase and identified nine missense mutations that resulted in improved MCFA production relative to the wild‐type strain. Colony‐based MALDI‐ToF MS screening provides an effective approach for engineering microbial fatty acid compositions in a high‐throughput manner.

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