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All sources NASA NTRS DOE OSTI

DOE OSTI2021

Cometary Activity Begins at Kuiper Belt Distances: Evidence from C/2017 K2

We study the development of activity in the incoming long-period comet C/2017 K2 over the heliocentric distance range 9 ≲ r {sub H} ≲ 16 au. The comet continues to be characterized by a coma of submillimeter-sized and larger particles ejected at low velocity. In a fixed co-moving volume around the nucleus we find that the scattering cross section of the coma, C, is related to the heliocentric distance by a power law, C∝r{sub H}{sup -s}, with heliocentric index s = 1.14 ± 0.05. This dependence is significantly weaker than the r {sub H} {sup -2} variation of the insolation as a result of two effects. These are, first, the heliocentric dependence of the dust velocity and, second, a lag effect due to very slow-moving particles ejected long before the observations were taken. A Monte Carlo model of the photometry shows that dust production beginning at r {sub H} ~ 35 au is needed to match the measured heliocentric index, with only a slight dependence on the particle size distribution. Mass-loss rates in dust at 10 au are of order 10{sup 3} kg s{sup -1}, while loss rates in gas may be much smaller, depending on the unknown dust to gas ratio. Consequently, the ratio of the nongravitational acceleration to the local solar gravity, α', may, depending on the nucleus size, attain values of ~10{sup -7} ≲ α' ≲ 10{sup -5}, comparable to values found in short-period comets at much smaller distances. Nongravitational acceleration in C/2017 K2 and similarly distant comets, while presently unmeasured, may limit the accuracy with which we can infer the properties of the Oort cloud from the orbits of long-period comets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Surrogate Model Based Optimization for Finding Robust Deep Learning Model Architectures

Deep Learning (DL) models are increasingly used throughout the sciences. However, their performance and usefulness depend greatly on their architecture which is defined by hyperparameters such as the number of nodes, layers, the learning rate, etc. Tuning these hyperparameters is time-consuming because evaluating their performance requires a lengthy training step. Stochastic optimizers used in training lead to performance variability and potentially prediction reliability issues. In this talk, we will describe an automated optimization method based on surrogate models and active learning strategies for tuning DL model architectures. We take into account the prediction variability with the goal to identify architectures that make reliable and robust predictions. We demonstrate our developments on an application arising in particle physics.

deep learning↗

DOE OSTI2024

ETROC1: the first full chain precision timing prototype ASIC for CMS MTD endcap timing layer upgrade

We present the design and characterization of the first fullchain precision timing prototype ASIC, named ETL Readout Chipversion 1 (ETROC1) for the CMS MTD endcap timing layer (ETL)upgrade. The ETL utilizes Low Gain Avalanche Diode (LGAD) sensors todetect charged particles, with the goal to achieve a time resolutionof 40–50 ps per hit, and 30–40 ps per track with hits from twodetector layers. The ETROC1 is composed of a 5 × 5 pixelarray and peripheral circuits. The pixel array includes a4 × 4 active pixel array with an H-tree shaped networkdelivering clock and charge injection signals. Each active pixel iscomposed of various components, including a bump pad, a chargeinjection circuit, a pre-amplifier, a discriminator, adigital-to-analog converter, and a time-to-digital converter. Thesecomponents play essential roles as the front-end link in processingLGAD signals and measuring timing-related information. Theperipheral circuits provide clock signals and readoutfunctionalities. The size of the ETROC1 chip is7 mm× 9 mm. ETROC1 has been fabricated in a 65 nmCMOS process, and extensively tested under stimuli of chargeinjection, infrared laser, and proton beam. The time resolution ofbump-bonded ETROC1 + LGAD chipsets reaches 42–46 ps per hit in thebeam test.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Effects of negative triangularity shaping on energetic particle driven Alfvén eigenmodes in DIII-D

Shape variations from positive to negative triangularity may lead to improved performance regimes in a tokamak with a reduction in microturbulence as well as improved thermal confinement. The motivation of this investigation is to model and compare the neutral beam driven Alfvén eigenmode (AE) activity in two DIII-D discharges with positive and negative triangularity shaping of plasma. The simulations are performed using the linear version of the FAR3d code, which solves the reduced MHD equations for thermal plasma with addition of moment equations for the energetic ion density and parallel velocity with appropriate Landau closure relations. Overall, our numerical results indicate that for similar physical parameters, the unstable AEs observed in the negative triangularity case have lower growth rates as compared to the positive triangularity regime. Our findings may be useful to analyze the influence of the reverse-D like geometry on the AE instabilities in DIII-D and may lead to better configurations for minimizing fast ion losses in a tokamak device.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Enhancing the inherent catalytic activity and stability of TiO 2 supported Pt single-atoms at CeO x –TiO 2 interfaces

Single-atoms (SAs) with atomically coordinated reaction centers are considered the next generation of catalysts that can exhibit exceptional catalytic efficiency. However, the general concern about thermodynamic vulnerabilities of SAs questions their practical value. Moreover, whether the inherent catalytic nature of SAs is superior compared with that of larger nanoparticles is still under debate. Here, we address two controversies by a comparative study using two catalysts: Pt/TiO 2 and Pt/CeO x –TiO 2 . Based on a hierarchical study of density functional theory, time-resolved catalysis performance test, in situ infrared spectroscopy, and operando X-ray absorption spectroscopy, we could unveil the catalytic nature of Pt-SAs and their stability. By utilizing the heterogeneous interface formed between TiO 2 supporting particles and CeO x clusters formed on the surface of TiO 2 , we preferentially synthesized Pt-SAs pinned at the CeO x –TiO 2 interfaces on CeO x –TiO 2 hybrid-oxide supports. The strong electronic coupling between the Pt-SAs and the Ce ions at the CeO x –TiO 2 interfaces enhanced the catalytic activity toward CO oxidation of Pt-SAs and improved the long-term stability under CO oxidation conditions. The CO oxidation activity of Pt-SAs stabilized at CeO x –TiO 2 was improved by 13.5 times at 200 °C compared with the Pt-SAs on TiO 2 . The results present how to easily improve the activity and stability of Pt-SAs using a simple interface control method. Moreover, we demonstrate that the catalytic activity and the stability of Pt-SAs can be monitored through the chemical state of the interfaces. Finally, our study provides comprehensive understanding about the catalytic nature as well as a novel strategy toward applications of Pt-SAs, enabling sustainable use of Pt in heterogeneous catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Certifying the Performance of Fixative Technologies under Open Air Demolition Activities for D and D - 20096

Department of Energy (DOE) facilities undergoing deactivation and decommissioning (D and D) activities struggle with safety concerns of residual radioactive contamination leftover after gross decontamination efforts have concluded. The positive effects of implementing fixative technologies for decommissioning and maintenance is known across the DOE complex. However, there is no standardized metric in place that quantifies the performance of these technologies such as incombustible fixative platforms that immobilize the contamination in a solid polymer material under normal operating conditions or when exposed to stressors. The primary focus of this research is to provide the empirical data necessary to properly characterize the effects of implementing fixative technologies on mitigating the release of contamination. In addition, this effort has been used to identify and establish uniform testing protocols to quantify operational parameters of fixating platforms and properly credit such systems under a variety of operational conditions and stressors that can arise during open air demolition efforts (e.g. impact, water, thermal, etc.). The established protocols will be provided to the ASTM International E10.03 Subcommittee on Radiological Protection for Decontamination and Decommissioning of Nuclear Facilities and Components for the potential of formal standardization. Attributes to be addressed during testing are material compromise from impact stress, thermal stress for incombustible fixative materials, and immobilization factors (how well an immobilizing platform is capable of retaining fixated material during thermal and impact stressors). In developing these test methods, a greater understanding of the material's behavior under anticipated and unanticipated events, such as decommissioning activities and contingency events as outlined in the Basis of Interim Operations (BIO), can be successfully characterized. There are several key components of the experimental methodology that is essential in empirically certifying fixative technologies. A surrogate contaminant with a unique signature has been utilized with the implementation of a uniform contamination process of test coupons that is quantifiable and replicable for direct fixative comparisons. A modular test chamber has also been used to apply the various stressors of interest. Collection of released contamination that includes airborne and resettled contaminant particles and analyzed using mass spectrometry. This research directly supports DOE complex-wide concerns in terms of final disposition of nuclear facilities and the considerations made during their time between ceasing facility operation and final disposition. The results of this effort aims to provide a standardized road map and logical decision flow to better facilitate fixative technologies into D and D activities required to achieve the desired facility end state. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Elucidating the factors controlling the methanol synthesis from CO 2 on ZnPd-ZnO/TiO 2 catalysts prepared by direct/inverse impregnation

The direct hydrogenation of CO 2 to methanol over supported ZnPd intermetallic catalysts remains a challenge due to the complex nature of the active sites, which are highly dependent on both the dispersion of ZnPd intermetallics and their proximity to ZnO. This study investigates the effect of the Pd and Zn incorporation order on methanol synthesis over TiO 2 -supported ZnPd catalysts. Catalysts were prepared via direct (Pd/Zn), inverse (Zn/Pd), and co-impregnation (Pd+Zn) methods using anatase TiO 2 as the support. Comprehensive characterization by XRD, HRTEM, CO-DRIFTS and XPS revealed that the formation of small and crystalline intermetallic β-ZnPd particles and their interaction with ZnO/ZnO x depends on the sequence of Pd and Zn incorporation. It was found that, under the reaction conditions, the ZnO x species plays a critical role in facilitating the formation of the intermetallic ZnPd through the interactions between Pd and ZnO x . In addition, ZnO x species have also been shown to modulate key catalytic properties, such as CO 2 activation and methanol selectivity. Specifically, the ZnPd/Pd surface ratio, determined by Pd dispersion and proximity to ZnO/ZnO x , was shown to determine the methanol production from CO 2 directly or via a CO intermediate. The Pd/Zn catalyst showed superior selectivity due to the in-situ formation of intermetallic species facilitated by Pd-ZnO x interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

ML-based calibration and control of the GlueX Central Drift Chamber

The GlueX Central Drift Chamber (CDC) in Hall D at Jefferson Lab, used for detecting and tracking charged particles, is calibrated and controlled during data taking using a Gaussian process. The system dynamically adjusts the high voltage applied to the anode wires inside the chamber in response to changing environmental and experimental conditions such that the gain is stabilized. Control policies have been established to manage the CDC's behavior. These policies are activated when the model's uncertainty exceeds a configurable threshold or during human-initiated tests during normal production running. Finally, we demonstrate the system reduces the time detector experts dedicate to calibration of the data offline, leading to a marked decrease in computing resource usage without compromising detector performance.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

The Twomey effect brightens clouds by increasing aerosol concentrations, which activates more droplets and decreases cloud supersaturation in response to more competition for water vapor. To quantify this competition response, we used marine low cloud observations in clean and smoky conditions at Ascension Island in the tropical South Atlantic during the Layered Aerosol Smoke Interactions with Cloud (LASIC) campaign. These observations show similar increases in droplet number for increased accumulation-mode particles from surface-based and satellite cloud retrievals, demonstrating the importance of below-cloud aerosol measurements for retrieving aerosol–cloud interactions (ACI) in clean and smoky aerosol conditions. Four methods for estimating cloud supersaturation from aerosol–cloud measurements were compared, with cloud scene-based and parcel-based methods showing sufficient variability for a strong dependence on both aerosol accumulation number concentration and cloud-base updraft velocities. Decomposing aerosol-related changes in cloud albedo and optical depth shows the calculated competition response accounts for dampening the activation response by 12 to 35%, explaining the diminished Twomey effect at high aerosol concentrations observed for smoky conditions at LASIC and previously around the world. This result was consistent for independent supersaturation retrievals by cloud scene-based droplet number and cloud condensation nuclei and parcel-based multimode size-resolving Lagrangian methods. Translating aerosol effects to local radiative forcing with clean conditions as a proxy for preindustrial and smoky conditions for present-day showed that the competition response reduces cooling from the Twomey radiative forcing by 12 to 35%, providing an essential process-specific constraint for improving the representation of aerosol competition in climate model simulation of indirect aerosol forcing.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Abstract Understanding structure–function relationships enables the design of materials with tailored functionalities. The long‐standing challenge is to design materials with high active volume to improve efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. This study reports a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in 3D and creating a significantly higher active volume. Such a structure in anatase is obtained and tuned by phase transformation during the heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

Ren, Peng↗

DOE OSTI2021

Tracking the phase changes in micelle-based NiGa nanocatalysts for methanol synthesis under activation and working conditions

The hydrogenation of CO 2 into high energy density fuels such as methanol, where the required H 2 is obtained from renewable sources, is of utmost importance for a sustainable society. In recent years, NiGa alloys have attracted attention as promising catalyst material systems for the hydrogenation of CO 2 into methanol at ambient pressures. They thus represent an energy-saving alternative to the Cu-based catalysts employed in today's catalytic industry that require high pressures for the CO 2 hydrogenation. However, the underlying reaction mechanisms for the NiGa system are still under debate. One of the challenges here is to unravel the evolution and coexistence of the different species in the heterogeneous NiGa catalyst system under activation and reaction conditions. To shed light on their evolution under activation in H 2 and their catalytic roles under CO 2 hydrogenation working conditions on well-defined Ni 3 Ga 1 and Ni 5 Ga 3 nanoparticle (NP) catalysts, we employed a multi-probe approach in this study. It included advanced machine learning-based analysis of operando X-ray absorption spectroscopy data combined with operando powder X-ray diffraction and near ambient pressure X-ray photoelectron spectroscopy measurements, as well as reactivity studies using bed-packed mass flow reactors. In addition, we employed atomic force microscopy and scanning transmission electron microscopy for structural characterization. Under H 2 activation at 1 bar total pressure, we concluded the formation of metallic Ni, starting for Ni 3 Ga 1 at 300 °C, and for Ni 5 Ga 3 at 400 °C. At higher temperatures, the formation of NiGa alloys follows. The α'-Ni 3 Ga 1 alloy phase is predominantly formed for the Ni 3 Ga 1 NPs, while the coexistence of α'-Ni 3 Ga 1 , δ-Ni 5 Ga 3 and Ga 2 O 3 phases is observed for the Ni 5 Ga 3 NPs after the H 2 activation. The formation of the Ga 2 O 3 phase also results in the presence of excess metallic Ni. Under CO 2 hydrogenation reaction conditions, Ga partially oxidizes again to form a Ga 2 O 3 -rich particle shell for both NP compositions, yet, to a larger extent for the Ni 3 Ga 1 NPs, which, in turn, feature a higher amount of excess Ni. We reveal that metallic Ni is responsible for the high selectivity of the Ni 3 Ga 1 NPs towards the production of methane in our catalytic tests. In contrast, the Ni 5 Ga 3 NPs display a strong selectivity toward methanol production (>92%), more than one order of magnitude higher than that for the Ni 3 Ga 1 NPs, which we ascribe to the presence of the δ-Ni 5 Ga 3 phase.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Diffused trenches for high fill-factor Low-Gain Avalanche Diodes

Low-Gain Avalanche Diodes (LGADs) are a class of silicon detectors that have been specifically designed for the fast detection of minimum ionizing particles (mips) in High-Energy Physics experiments. While they provide timing resolution on the order of a few tens of picoseconds, they cannot achieve high spatial resolution due to the intrinsic characteristics of their structures. Thus, active R&D is on-going to develop detectors based on LGADs to improve their spatial resolution while maintaining the timing performance of the LGADs. Such devices are, for example, AC-coupled LGADs and Deep-Junction LGADs. Another device option is the Trench-Isolated LGAD (TI LGAD), where trenches etched at the periphery of the pixels isolate them while providing a high fill-factor. Here, in this paper, we present a variation of this latter approach, demonstrating its feasibility by means of 2-dimensional TCAD simulations.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Surface Oxygen Depletion of Layered Transition Metal Oxides in Li-Ion Batteries Studied by Operando Ambient Pressure X-ray Photoelectron Spectroscopy

A new operando spectro-electrochemical setup was developed to study oxygen depletion from the surface of layered transition metal oxide particles at high degrees of delithiation. An NCM111 working electrode was paired with a chemically delithiated LiFePO 4 counter electrode in a fuel cell-inspired membrane electrode assembly (MEA). A propylene carbonate-soaked Li-ion conducting ionomer served as an electrolyte, providing both good electrochemical performance and direct probing of the NCM111 particles during cycling by ambient pressure X-ray photoelectron spectroscopy. The irreversible emergence of an oxygen-depleted phase in the O 1s spectra of the layered oxide particles was observed upon the first delithiation to high state-of-charge, which is in excellent agreement with oxygen release analysis via mass spectrometry analysis of such MEAs. By comparing the metal oxide-based O 1s spectral features to the Ni 2p 3/2 intensity, we can calculate the transition metal-to-oxygen ratio of the metal oxide close to the particle surface, which shows good agreement with the formation of a spinel-like stoichiometry as an oxygen-depleted phase. This new setup enables a deeper understanding of interfacial changes of layered oxide-based cathode active materials for Li-ion batteries upon cycling.

25 ENERGY STORAGE↗

DOE OSTI2025

Overview of the front-end electronics of CMS HGCal - including readout and powering

The end-cap calorimeters of CMS will be upgraded to a single High Granularity Calorimeter (HG-Cal) for the HL-LHC, including both silicon sensors and scintillator tiles with on-tile SiPMs as active elements. The readout of the active elements is performed by an ASIC (HGCROC in 130 nm CMOS technology) that measures the amplitude and arrival time of the signals. The amplitude is measured over a large dynamic range to allow calibration with single particles and the measurement of TeV showers. The time of arrival of high-energy showers will be measured with a precision of around 30 ps. A second pair of “concentrator” ASICs - ECON-T and ECON-D - takes the data from the HGCROC channels and packages them for transmission via optical links to the off-detector electronics. The ECON-T transmits trigger data at 40 MHz, to form part of the level-1 trigger. The ECON-D transmits concentrated data packets at up to 1 MHz, upon reception of a level-1 trigger signal. In addition to these ASICs, HGCal will use modified versions of common HL-LHC electronics developments, for the power chain and the optical control and readout. The dense nature of the HGCal provides additional challenges for the electronic boards and cabling. In this proceedings the overall HGCal front electronics scheme, including the latest performance of the HGCROC and ECON ASICs is presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Specific absorbed fractions for a revised series of the UF/NCI pediatric reference phantoms: internal photon sources

Assessment of radiation absorbed dose to internal organs of the body from the intake of radionuclides, or in the medical setting through the injection of radiopharmaceuticals, is generally performed based upon reference biokinetic models or patient imaging data, respectively. Biokinetic models estimate the time course of activity localized to source organs. The time-integration of these organ activity profiles are then scaled by the radionuclide S-value, which defines the absorbed dose to a target tissue per nuclear transformation in various source tissues. S-values are computed using established nuclear decay information (particle energies and yields), and a parameter termed the specific absorbed fraction (SAF). The SAF is the ratio of the absorbed fraction—fraction of particle energy emitted in the source tissue that is deposited in the target tissue—and the target organ mass. While values of the SAF may be computed using patient-specific or individual-specific anatomic models, they have been more widely available through the use of computational reference phantoms. In this study, we report on an extensive series of photon SAFs computed in a revised series of the University of Florida and the National Cancer Institute pediatric reference phantoms which have been modified to conform to the specifications embodied in the ICRP reference adult phantoms of Publication 110 (e.g. organs modeled, organ ID numbers, blood contribution to elemental compositions). Following phantom anatomical revisions, photon radiation transport simulations were performed using MCNPX v2.7 in each of the ten phantoms of the series—male and female newborn, 1 year old, 5 year old, 10 year old, and 15 year old—for 60 different tissues serving as source and/or target regions. A total of 25 photon energies were considered from 10 keV to 10 MeV along a logarithm energy grid. Detailed analyses were conducted of the relative statistical errors in the Monte Carlo target tissue energy deposition tallies at low photon energies and over all energies for source–target combinations at large intra-organ separation distances. Based on these analyses, various data smoothing algorithms were employed, including multi-point weighted data smoothing, and log–log interpolation at low energies (1 keV and 5 keV) using limiting SAF values based upon target organ mass to bound the interpolation interval. The final dataset is provided in a series of ten electronic supplemental files in MS Excel format. Finally, the results of this study were further used as the basis for assessing the radiative component of internal electron source SAFs as described in our companion paper (Schwarz et al 2021) for this same pediatric phantom series.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2021

Specific absorbed fractions for a revised series of the UF/NCI pediatric reference phantoms: internal electron sources

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Cluster structure of 3⁢𝛼+𝑝 states in 13 N

Cluster states in 13 N are extremely difficult to measure due to the unavailability of 9 B +𝛼 elastic-scattering data. Using 𝛽-delayed charged-particle spectroscopy of 13 O, clustered states in 13 N can be populated and measured in the 3⁢𝛼+𝑝 decay channel. One-at-a-time implantation and decay of 13 O was performed with the Texas Active Target Time Projection Chamber. 149⁢𝛽⁢3⁢𝛼⁢𝑝 decay events were observed and the excitation function in 13 N reconstructed. Four previously unknown 𝛼-decaying excited states were observed in 13 N at an excitation energy of 11.3, 12.4, 13.1, and 13.7 MeV decaying via the 3⁢𝛼+𝑝 channel. These states are seen to have a [ 9 B ⁡(g.s) ⁢⨂𝛼/𝑝 + 12 C ⁡(0$^+_2$)], [ 9 B ⁡($\frac{1}{2}$ + )⁢ ⨂𝛼], [ 9 B ⁡($\frac{5}{2}$ + )⁢ ⨂𝛼], and [ 9 B⁡ ($\frac{5}{2}$) ⁢⨂𝛼] structure, respectively. A previously seen state at 11.8 MeV was also determined to have a [𝑝+ 12 C ⁡(g.s.)/𝑝+ 12 C ⁡(0$^+_2$)] structure. The overall magnitude of the clustering is not able to be extracted, however, due to the lack of a total width measurement. Clustered states in 13 N (with unknown magnitude) seem to persist from the addition of a proton to the highly 𝛼-clustered 12 C . Evidence of the $\frac{1}{2}$ + state in 9 B was also seen to be populated by decays from 13 N ★ .

Physics↗

DOE OSTI2022

Role of Local Structure in the Enhanced Dynamics of Deformed Glasses

External stress can accelerate molecular mobility of amorphous solids by several orders of magnitude. The changes in mobility are commonly interpreted through the Eyring model, which invokes an empirical activation volume. Here, we analyze constant-stress molecular dynamics simulations and propose a structure-dependent Eyring model, connecting activation volume to a machine-learned field, softness. We show that stress has a heterogeneous effect on the mobility that depends on local structure through softness. The barrier impeding relaxation reduces more for well-packed particles, which explains the narrower distribution of relaxation time observed under stress.

74 ATOMIC AND MOLECULAR PHYSICS↗