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DOE OSTI2023

Charge Concentration Limits the Hydrogen Evolution Rate in Organic Nanoparticle Photocatalysts

Colloidal organic nanoparticles have proven to be a promising class of photocatalyst for performing the Hydrogen Evolution Reaction (HER) due to their dispersibility in aqueous environments, their strong absorption within the visible region, and the tunabilty of their component materials' redox potentials. Currently, there is little understanding of how charge generation and accumulation in organic semiconductors change when these materials are formed into nanoparticles that share a high interfacial area with water, nor is it known what mechanism limits the hydrogen evolution efficiency in recent reports on organic nanoparticle photocatalysts. Herein, we use Time-Resolved Microwave Conductivity to study aqueous-soluble organic nanoparticles and bulk thin films composed of various blend ratios of the non-fullerene acceptor EH-IDTBR and conjugated polymer PTB7-Th and examine the relationship between composition, interfacial surface area, charge carrier dynamics, and photocatalytic activity. We quantitatively measure the rate of Hydrogen Evolution Reaction by nanoparticles composed of various donor:acceptor blend ratio compositions and find that the most active blend ratio displays a Hydrogen Quantum Yield of 0.83% per photon. Moreover, we find that nanoparticle photocatalytic activity corresponds directly to charge generation, and that nanoparticles have 3x more long-lived accumulated charges relative to bulk samples of the same material composition. Here these results suggest that, under our current reaction conditions, with approximately 3x solar flux, catalytic activity by these nanoparticles is limited by the concentration of electrons and holes in operando and not a finite number of active surface cites or the catalytic rate at the interface. This provides a clear design goal for the next generation of efficient photocatalytic nanoparticles.

08 HYDROGEN↗

DOE OSTI2021

Phoenix: A Scalable Streaming Hypergraph Analysis Framework

We present Phoenix, a scalable hypergraph analytics framework for data analytics and knowledge discovery that was implemented on the leadership class computing platforms at Oak Ridge National Laboratory (ORNL). Our software framework comprises a distributed implementation of a streaming server architecture which acts as a gateway for various hypergraph generators/external sources to connect. Phoenix has the capability to utilize diverse hypergraph generators, including HyGen, a very large-scale hypergraph generator developed by ORNL. Phoenix incorporates specific algorithms for efficient data representation by exploiting hidden structures of the hypergraphs. Our experimental results demonstrate Phoenix’s scalable and stable performance on massively parallel computing platforms. Phoenix’s superior performance is due to the merging of high-performance computing with data analytic.

Kurte, Kuldeep↗

DOE OSTI2018

GPU acceleration and performance of the particle-beam-dynamics code Elegant

Elegant is an accelerator physics and particle-beam dynamics code widely used for modeling and design of a variety of high-energy particle accelerators and accelerator-based systems. We discuss a recently developed version of the code that can take advantage of CUDA-enabled graphics processing units (GPUs) to achieve significantly improved performance for a large class of simulations that are important in practice. The GPU version is largely defined by a framework that simplifies implementations of the fundamental kernel types that are used by Elegant: particle operations, reductions, particle loss, histograms, array convolutions and random number generation. Accelerated performance on the Titan Cray XK-7 supercomputer is approximately 6–10 times better with the GPU than all the CPU cores associated with the same node count. In addition to performance, the maintainability of the GPU-accelerated version of the code was considered a key design objective. Accuracy with respect to the CPU implementation is also a core consideration. Finally, four different methods are used to ensure that the accelerated code faithfully reproduces the CPU results.

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

Differences in toxicity of anionic and cationic PAMAM and PPI dendrimers in zebrafish embryos and cancer cell lines

Dendrimers are an emerging class of polymeric nanoparticles with beneficial biomedical applications like early diagnostics, in vitro gene transfection or controlled drug delivery. However, the potential toxic impact of exposure on human health or the environment is often inadequately defined. Thus, polyamidoamine (PAMAM) dendrimers of generations G3.0, 3.5, 4.0, 4.5 and 5.0 and polypropylenimine (PPI) dendrimers G3.0, 4.0 and 5.0 were tested in zebrafish embryos for 96 h and human cancer cell lines for 24 h, to assess and compare developmental in vivo toxicity with cytotoxicity. The zebrafish embryo toxicity of cationic PAMAM and PPI dendrimers increased over time, with EC50 values ranging from 0.16 to just below 1.7 μM at 24 and 48 hpf. The predominant effects were mortality, plus reduced heartbeat and blood circulation for PPI dendrimers. Apoptosis in the embryos increased in line with the general toxicity concentration-dependently. Hatch and dechorionation of the embryos increased the toxicity, suggesting a protective role of the chorion. Lower generation dendrimers were more toxic in the embryos whereas the toxicity in the HepG2 and DU145 cell lines increased with increasing generation of cationic PAMAMs and PPI dendrimers. HepG2 were less sensitive than DU145 cells, with IC50 values ≥ 402 μM (PAMAMs) and ≤ 240 μM (PPIs) for HepG2 and ≤ 13.24 μM (PAMAMs) and ≤ 12.84 μM (PPIs) for DU145. Neither in fish embryos nor cells toxicity thresholds were determinable for anionic PAMAM G3.5 and G4.5. The study demonstrated that the cytotoxicity underestimated the in-vivo toxicity of the dendrimers in the fish embryos. - Highlights: • Zebrafish embryo toxicity of cationic PAMAM and PPI dendrimers increased over time. • Zebrafish embryo toxicity of cationic dendrimers did not increase with generation. • Cationic dendrimers induced apoptosis in zebrafish embryos. • Toxicity of cationic dendrimers was lower in HepG2 and DU145 than zebrafish embryos. • Anionic PAMAM dendrimers showed little to no toxicity in fish embryos and cells.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2026

Atomic-Scale Imaging Reveals Polar-π Interactions in Two-Dimensional Molecular Superlattices

Controlling coassembly of synthetic oligomers into binary superlattices at the atomic level is challenging. Here, we report a strategy for programming polar-π interactions in oligomeric peptoids, a class of sequence-defined peptidomimetics, facilitating the formation of homogeneous two-dimensional (2D) superlattices. N-2-phenylethyl and N-(2-perfluorophenyl)ethyl side chains, similar in size, but with contrasting electrostatic characteristics, were introduced at defined sequence positions to generate favorable dipolar aromatic interactions. The resulting nanosheets exhibit different crystal motifs depending on the side chain interactions: systems containing only one type of aromatic side chain form a parallel V-shaped motif driven by π-π interactions, whereas a combination of both types of aromatic side chains, either within one backbone or through the coassembly of two distinct peptoids, adopt an antiparallel V-shaped superlattice with higher thermal stability, driven by polar-π interactions. Cryogenic transmission electron microscopy directly resolved the packing arrangement of perfluorophenyl and phenyl rings in individual nanosheet superlattices, confirming that intermolecular polar-π interaction dominates the superlattice motifs and increases lattice stability. Molecular dynamics simulations and density functional theory calculations further substantiate the energetic favorability of polar-π interactions over π-π interactions, rationalizing the formation of homogeneous superlattices with enhanced thermal stability. Our discoveries establish a design principle for binary coassembly using sequence-defined oligomers, which enables control over unit cell geometry, lattice stability, and molecular registration through aromatic side chain polarization and sequence control. This ability to program atomic-scale binary superlattices opens new avenues for designing functional 2D soft materials.

Lee, Yen Jea [Lawrence Berkeley National Laborator↗

DOE OSTI2022

Efficient Clustering of Software Vulnerabilities using Self Organizing Map (SOM)

The common vulnerabilities and exposures (CVE) database was created with a mission to ``identify, define, and catalog publicly disclosed cybersecurity vulnerabilities''. This rich body of information can be used to enable rapid and efficient response to secure and defend cyber operations and protect critical cyber infrastructure. The main goal of this paper is to develop a visual analytics tool to enable deep analysis of CVEs using unsupervised clustering techniques. We enhance our analysis by first mapping CVEs to hierarchical-classes in Common Weakness Enumeration (CWE) using information in the National Vulnerability Database (NVD). Both the mapping and the numerical representation of CVEs are enabled by V2W-BERT, which uses natural language processing of the extensive information in NVD to generate a large tabular database of 137,226 CVE entries from 1999 to 2020, where each CVE is represented by a vector of 768 numerical features. The vectorized data is processed by Self-Organizing Maps (SOM), which is an unsupervised machine learning technique for dimensionality reduction, visual representation and clustering. Using a Torus map of 6417 units, we achieve ~10-fold data compression of ~140k CVEs using SOM. The trained map is further clustered using standard K-means clustering into 138 clusters of CVEs. We conducted a brief investigation of the rich mapping of CVEs to best-matching-units to K-means clusters, as well as CVEs to CWEs. For example, this novel mapping provided insight into the role of CWE-59 and CWE-264 in several CVEs that is otherwise hard to explore in the original data. We conclude that our this novel approach will not only enable deep analysis of the complex relationships between CVEs and CWEs, but also a mechanism to quickly respond to and design mitigation actions for rapidly evolving vulnerabilities that have not been mapped to existing CWEs.

Panchal, Khyati↗

DOE OSTI2021

Accelerator Real-time Edge AI for Distributed Systems (READS) (Proposal)

Over the last decade, Machine Learning (ML) technologies have slowly made their way into the accelerator community. Rapid advances in recent years in deep learning, particularly reinforcement learning for control system applications and the accessibility of deep learning in embedded hardware, have generated renewed interest and spawned a number of applications. The Fermilab Accelerator Complex, shown in Fig. 1, has provided High Energy Physics (HEP) experiments with proton beams for nearly fifty years. The current focus of the laboratory is its world-class experimental program at the intensity frontier. While increasing beam intensity certainly presents its own challenges, preserving beam size while minimizing beam losses – particles lost through interactions with the beam vacuum pipe – turns out to be, in many ways, the main challenge. The accelerator is controlled via a complex system of hundreds of thousands of devices. Enabling fine tuning and real-time optimization of their parameters using ML methods and stepping beyond experience-based reasoning of human operators are key to the success of future intensity upgrades. Our objective will be to integrate ML into accelerator operations and furthermore, provide an accessible framework, which can also be used by a broad range of other accelerator systems with dynamic tuning needs.

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Factors That Control the Formation of Dendrites and Other Morphologies on Lithium Metal Anodes

Lithium metal is a promising anode material for next-generation rechargeable batteries, but non-uniform electrodeposition of lithium is a significant barrier. These non-uniform deposits are often referred to as lithium “dendrites,” although their morphologies can vary. We have surveyed the literature on lithium electrodeposition through three classes of electrolytes: liquids, polymers and inorganic solids. We find that the non-uniform deposits can be grouped into six classes: whiskers, moss, dendrites, globules, trees, and cracks. These deposits were obtained in a variety of cell geometries using both unidirectional deposition and cell cycling. The main result of the study is a figure where the morphology of electrodeposited lithium is plotted as a function of two variables: shear modulus of the electrolyte and current density normalized by the limiting current density. We show that specific morphologies are confined to contiguous regions on this two-dimensional plot.

25 ENERGY STORAGE↗

DOE OSTI2023

Evolutionary flexibility and rigidity in the bacterial methylerythritol phosphate (MEP) pathway

Terpenoids are a diverse class of compounds with wide-ranging uses including as industrial solvents, pharmaceuticals, and fragrances. Efforts to produce terpenoids sustainably by engineering microbes for fermentation are ongoing, but industrial production still largely relies on nonrenewable sources. The methylerythritol phosphate (MEP) pathway generates terpenoid precursor molecules and includes the enzyme Dxs and two iron–sulfur cluster enzymes: IspG and IspH. IspG and IspH are rate limiting-enzymes of the MEP pathway but are challenging for metabolic engineering because they require iron–sulfur cluster biogenesis and an ongoing supply of reducing equivalents to function. Therefore, identifying novel alternatives to IspG and IspH has been an on-going effort to aid in metabolic engineering of terpenoid biosynthesis. We report here an analysis of the evolutionary diversity of terpenoid biosynthesis strategies as a resource for exploration of alternative terpenoid biosynthesis pathways. Using comparative genomics, we surveyed a database of 4,400 diverse bacterial species and found that some may have evolved alternatives to the first enzyme in the pathway, Dxs making it evolutionarily flexible. In contrast, we found that IspG and IspH are evolutionarily rigid because we could not identify any species that appear to have enzymatic routes that circumvent these enzymes. The ever-growing repository of sequenced bacterial genomes has great potential to provide metabolic engineers with alternative metabolic pathway solutions. With the current state of knowledge, we found that enzymes IspG and IspH are evolutionarily indispensable which informs both metabolic engineering efforts and our understanding of the evolution of terpenoid biosynthesis pathways.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Census of the Young Stellar Population in the Galactic H ii Region Sh2-242

We present here identification and characterization of the young stellar population associated with an active star-forming site Sh2-242. We used our own new optical imaging and spectroscopic observational data, as well as several archival catalogs, e.g., Pan-STARRS 1, Gaia DR2, IPHAS, Wide-field InfraRed Camera, 2MASS, and Spitzer. Slit spectroscopic results confirm the classification of the main ionizing source BD+26 980 as an early-type star of spectral type B0.5 V. The spectrophotometric distance of the star is estimated as 2.08 ± 0.24 kpc, which confirms the source as a member of the cluster. An extinction map covering a large area (diameter ∼50′) is generated with H and K photometry toward the region. From the map, three distinct locations of peak extinction complexes (A {sub V} ≃ 7–17 mag) are identified for the very first time. Using the infrared color excess, a total of 33 Class I and 137 Class II young objects are classified within the region. The IPHAS photometry reveals classification of 36 Hα emitting sources, which might be class II objects. Among 36 Hα emitting sources, 5 are already identified using infrared excess emission. In total, 201 young objects are classified toward S242 from this study. The membership status of the young sources is further windowed with the inclusion of parallax from the Gaia DR2 catalog. Using the optical and infrared color–magnitude diagrams, the young stellar objects are characterized with an average age of ∼1 Myr and masses in the range 0.1–3.0 M {sub ☉}. The census of the stellar content within the region is discussed using combined photometric and spectroscopic data.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

A RECONNECTION-DRIVEN MODEL OF THE HARD X-RAY LOOP-TOP SOURCE FROM FLARE 2004 FEBRUARY 26

A compact X-class flare on 2004 February 26 showed a concentrated source of hard X-rays at the tops of the flare’s loops. This was analyzed in previous work and interpreted as plasma heated and compressed by slow magnetosonic shocks (SMSs) generated during post-reconnection retraction of the flux. That work used analytic expressions from a thin flux tube (TFT) model, which neglected many potentially important factors such as thermal conduction and chromospheric evaporation. Here we use a numerical solution of the TFT equations to produce a more comprehensive and accurate model of the same flare, including those effects previously omitted. These simulations corroborate the prior hypothesis that slow-mode shocks persist well after the retraction has ended, thus producing a compact, loop-top source instead of an elongated jet, as steady reconnection models predict. Thermal conduction leads to densities higher than analytic estimates had predicted, and evaporation enhances the density still higher, but at lower temperatures. X-ray light curves and spectra are synthesized by convolving the results from a single TFT simulation with the rate at which flux is reconnected, as measured through motion of flare ribbons, for example. These agree well with light curves observed by RHESSI and GOES and spectra from RHESSI . An image created from a superposition of TFT model runs resembles one produced from RHESSI observations. This suggests that the HXR loop-top source, at least the one observed in this flare, could be the result of SMSs produced in fast reconnection models like Petschek’s.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1980

A tensor approach to modeling of nonhomogeneous nonlinear systems

Model following control methodology plays a key role in numerous application areas. Cases in point include flight control systems and gas turbine engine control systems. Typical uses of such a design strategy involve the determination of nonlinear models which generate requested control and response trajectories for various commands. Linear multivariable techniques provide trim about these motions; and protection logic is added to secure the hardware from excursions beyond the specification range. This paper reports upon experience in developing a general class of such nonlinear models based upon the idea of the algebraic tensor product.

Yurkovich, S.↗

NASA NTRS1990

Are extremely luminous far-infrared galaxies the result of merging quasar cores

Extremely Luminous far-infrared galaxies (ELFs) are a class of galaxy discovered independently by several groups. The class is characterized by a quasar-like total luminosity (10(exp 11) to 10(exp 13) solar luminosity) which is radiated almost entirely in the far-infrared. It has been suggested that obscured quasar cores may be responsible for generating this luminosity. Here the author demonstrates that ELFs appear in several guises which can be characterized by the number of quasar cores they contain (zero, one or two). The author develops a unified model to account for these differences.

Norris, R. P.↗

NASA NTRS1991

Experimental demonstration of a classical approach for flexible space structure control: NASA CSI testbeds

The results of active control experiments performed for the Mini-Mast truss structure are presented. The primary research objectives were: (1) to develop active structural control concepts and/or techniques; (2) to verify the concept of robust non-minimum-phase compensation for a certain class of non-colocated structural control problems through ground experiments; (3) to verify a 'dipole' concept for persistent disturbance rejection control of flexible structures; and (4) to identify CSI (Control Structure Interaction) issues and areas of emphasis for the next generation of large flexible spacecraft. The classical SISO (Single Input and Single Output) control design approach was employed.

Bond, Wie↗

NASA NTRS1995

Mapping Vegetative Ground Cover From Polarimetric SAR Data

Three-frequency quad-polarization data used to distinguish among different types of cover. MAPVEG computer program performs first-level classification of NASA/JPL AIRSAR polarimetric synthetic-aperture-radar (SAR) data into simple ground-cover types. Classification images generated used to separate vegetated from nonvegetated areas; useful in determining soil moisture in areas free of vegetation. Classification separates forests from surrounding vegetation, and used to identify clear-cut areas. Urban areas and potential marshlands examples of other identifiable classes. Written in FORTRAN 77.

Chapman, Bruce↗

NASA NTRS2014

Guaranteed Road Network Search with Small Unmanned Aircraft

The use of teams of small unmanned aircraft in real-world rapid-response missions is fast becoming a reality. One such application is search and detection of an evader in urban areas. This paper draws on results in graph-based pursuit-evasion, developing mappings from these abstractions to primitive motions that may be performed by aircraft, to produce search strategies providing guaranteed capture of road-bound targets. The first such strategy is applicable to evaders of arbitrary speed and agility, offering a conservative solution that is insensitive to motion constraints pursuers may possess. This is built upon to generate two strategies for capture of targets having a known speed bound that require searcher teams of much smaller size. The efficacy of these algorithms is demonstrated by evaluation in extensive simulation using realistic vehicle models across a spectrum of environment classes.

unmanned aircraft systems↗

NASA NTRS2018

Beamforming P-Band Synthetic Aperture Radar for Planetary Applications

The Space Exploration Synthetic Aperture Radar (SESAR) is an advanced P-band beamforming radar instrument concept to enable a new class of observations suitable to meet multiple Decadal Survey science goals for planetary exploration. The radar is capable of providing unprecedented surface and near subsurface measurements at full polarimetry and fine (meter scale) resolution, and achieves beam agility through programmable waveform generation and digital beamforming. The radar’s highly flexible modular architecture employs a novel low power, lightweight design approach to meet stringent planetary instrument requirements, all while minimizing cost and development time.

Rincon, Rafael F.↗

NASA NTRS2023

Evolutionary Flexibility and Rigidity in the Bacterial Methylerythritol Phosphate (Mep) Pathway

Bailey Marshall↗