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Direct ladderization of cyclooctatetraene-containing, processable conjugated ladder polymers from annulated bis-zirconacyclopentadienes
Conjugated ladder polymers (CLPs) are difficult yet captivating synthetic targets due to their fully unsaturated fused backbones. Inherent challenges associated with their synthesis often lead to low yields, structural defects, and insoluble products. Here a new method to form CLPs is demonstrated, utilizing a high-yielding dimerization of annulated zirconacyclopentadienes to form cyclooctatetraene (COT) monomer units. The resulting COT-containing polymers form rapidly in a single ladderization step from the bis-zirconacyclopentadiene precursors and display M n up to 29.7 kg mol -1 . The polymers represent rare examples of CLPs with negatively curved rings, resulting in the observation of unusual properties. The rigid tub-shaped COT units embedded in the backbone imbue the polymers with microporosity, exhibiting BET surface areas up to 555 m 2 g -1 . Additionally, the remarkable solubility of these CLPs in organic solvents enables the fabrication of thin films showcasing high dielectric performance with a discharged energy density as high as 6.54 J cm -3 at 650 MV m -1 .
Rheological Behavior & Process Monitoring of Highly Filled Direct-Ink Write Pastes.
Abstract not provided.
EdgeAI: Machine learning via direct attached accelerator for streaming data processing at high shot rate x-ray free-electron lasers
We present a case for low batch-size inference with the potential for adaptive training of a lean encoder model. We do so in the context of a paradigmatic example of machine learning as applied in data acquisition at high data velocity scientific user facilities such as the Linac Coherent Light Source-II x-ray Free-Electron Laser. We discuss how a low-latency inference model operating at the data acquisition edge can capitalize on the naturally stochastic nature of such sources. We simulate the method of attosecond angular streaking to produce representative results whereby simulated input data reproduce high-resolution ground truth probability distributions. By minimizing the mean-squared error between the decoded output of the latent representation and the ground truth distributions, we ensure that the encoding layers and resulting latent representation maintains full fidelity for any downstream task, be it classification or regression. We present throughput results for data-parallel inference of various batch sizes, some with throughput exceeding 100 k images per second. We also show in situ training below 10 s per epoch for the full encoder–decoder model as would be relevant for streaming and adaptive real-time data production at our nation’s scientific light sources.
Digital Image Velocimetry
Proposed technique for production of velocity maps from sequences of photographic video images of flows seeded with small particles. In digital image velocimetry, image analyzed by digital Fourier tranformation. Process free of noise, more precise, and consumes less time. Eliminates need to process photographs, indicates directions of velocity vectors unambiguously, and offers increased dynamic ranges. Because all processing performed electronically, eventually capable of mapping flow-velocity fields in real time.
Asymptotically stable direct model reference adaptive controllers for processes not necessarily satisfying a positive real constraint
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Future directions in focal-plane signal processing for space-borne scientific imagers
The potential of focal-plane signal processing for space-borne scientific imagers is discussed. Significant improvement in image quality and consequent scientific return may be enabled through the utilization of focal-plane signal processing techniques. The possible application of focal-plane signal processing to readout noise reduction, cosmic ray circumvention, non-uniformity correction, and throughput enhancement is described. On-focal-plane analog-to-digital (A/D) conversion and micromotion stabilization are also discussed. It is the intention of this paper to stimulate further thought and efforts in this field.
Multigrid direct numerical simulation of the whole process of flow transition in 3-D boundary layers
A new technology was developed in this study which provides a successful numerical simulation of the whole process of flow transition in 3-D boundary layers, including linear growth, secondary instability, breakdown, and transition at relatively low CPU cost. Most other spatial numerical simulations require high CPU cost and blow up at the stage of flow breakdown. A fourth-order finite difference scheme on stretched and staggered grids, a fully implicit time marching technique, a semi-coarsening multigrid based on the so-called approximate line-box relaxation, and a buffer domain for the outflow boundary conditions were all used for high-order accuracy, good stability, and fast convergence. A new fine-coarse-fine grid mapping technique was developed to keep the code running after the laminar flow breaks down. The computational results are in good agreement with linear stability theory, secondary instability theory, and some experiments. The cost for a typical case with 162 x 34 x 34 grid is around 2 CRAY-YMP CPU hours for 10 T-S periods.
Encryption for Remote Control via Internet or Intranet
A data-communication protocol has been devised to enable secure, reliable remote control of processes and equipment via a collision-based network, while using minimal bandwidth and computation. The network could be the Internet or an intranet. Control is made secure by use of both a password and a dynamic key, which is sent transparently to a remote user by the controlled computer (that is, the computer, located at the site of the equipment or process to be controlled, that exerts direct control over the process). The protocol functions in the presence of network latency, overcomes errors caused by missed dynamic keys, and defeats attempts by unauthorized remote users to gain control. The protocol is not suitable for real-time control, but is well suited for applications in which control latencies up to about 0.5 second are acceptable. The encryption scheme involves the use of both a dynamic and a private key, without any additional overhead that would degrade performance. The dynamic key is embedded in the equipment- or process-monitor data packets sent out by the controlled computer: in other words, the dynamic key is a subset of the data in each such data packet. The controlled computer maintains a history of the last 3 to 5 data packets for use in decrypting incoming control commands. In addition, the controlled computer records a private key (password) that is given to the remote computer. The encrypted incoming command is permuted by both the dynamic and private key. A person who records the command data in a given packet for hostile purposes cannot use that packet after the public key expires (typically within 3 seconds). Even a person in possession of an unauthorized copy of the command/remote-display software cannot use that software in the absence of the password. The use of a dynamic key embedded in the outgoing data makes the central-processing unit overhead very small. The use of a National Instruments DataSocket(TradeMark) (or equivalent) protocol or the User Datagram Protocol makes it possible to obtain reasonably short response times: Typical response times in event-driven control, using packets sized .300 bytes, are <0.2 second for commands issued from locations anywhere on Earth. The protocol requires that control commands represent absolute values of controlled parameters (e.g., a specified temperature), as distinguished from changes in values of controlled parameters (e.g., a specified increment of temperature). Each command is issued three or more times to ensure delivery in crowded networks. The use of absolute-value commands prevents additional (redundant) commands from causing trouble. Because a remote controlling computer receives "talkback" in the form of data packets from the controlled computer, typically within a time interval < or =1 s, the controlling computer can re-issue a command if network failure has occurred. The controlled computer, the process or equipment that it controls, and any human operator(s) at the site of the controlled equipment or process should be equipped with safety measures to prevent damage to equipment or injury to humans. These features could be a combination of software, external hardware, and intervention by the human operator(s). The protocol is not fail-safe, but by adopting these safety measures as part of the protocol, one makes the protocol a robust means of controlling remote processes and equipment by use of typical office computers via intranets and/or the Internet.
4D imaging of lithium-batteries using correlative neutron and X-ray tomography with a virtual unrolling technique
The temporally and spatially resolved tracking of lithium intercalation and electrode degradation processes are crucial for detecting and understanding performance losses during the operation of lithium-batteries. Here, high-throughput X-ray computed tomography has enabled the identification of mechanical degradation processes in a commercial Li/MnO 2 primary battery and the indirect tracking of lithium diffusion; furthermore, complementary neutron computed tomography has identified the direct lithium diffusion process and the electrode wetting by the electrolyte. Virtual electrode unrolling techniques provide a deeper view inside the electrode layers and are used to detect minor fluctuations which are difficult to observe using conventional three dimensional rendering tools. Moreover, the 'unrolling' provides a platform for correlating multi-modal image data which is expected to find wider application in battery science and engineering to study diverse effects e.g. electrode degradation or lithium diffusion blocking during battery cycling.
Standard Materials and Processes Requirements for Spacecraft
This NASA Technical Standard is directed toward materials and processes (M&P) used in the design, fabrication, and testing of space program flight hardware for NASA, including but not limited to crewed, uncrewed, robotic, launch vehicle, lander, in-space and surface systems, and spacecraft program/project hardware elements. All spaceflight hardware is covered by the M&P requirements of this document, including vendor-designed, off-the-shelf, and vendor-furnished items. M&P used in interfacing ground support equipment (GSE), test equipment, hardware processing equipment, hardware packaging, and hardware shipment is covered by the M&P requirements of this NASA Technical Standard only to the extent required to prevent damage to or contamination of spaceflight hardware (see section 4). M&P used in NASA aircraft and aircraft operations are not covered by the M&P requirements of this document.
The 5-(4-Ethynylophenoxy) isophthalic chloride
Sulfone-ester polymers containing pendent ethynyl groups and a direct and multistep process for preparing them are disclosed. The multistep process involves the conversion of a pendent bromo group to the ethynyl group while the direct route involves reating hydroxy-terminated sulfone oligomer or polymers with a stoichiometric amount of 5-(4-ethynylphenoxy) isophthaloyl chloride. The 5-(4-ethynylphenoxy) isophthaloyl chloride and the process for preparing it are also disclosed.
Direct Recycling of End-of-Life Cathode Material Through Redox Chemistry Mediators
Lithium-ion batteries (LIBs) are ideal for electric vehicles and electronic devices because of their high-power density and outstanding cycle life. The need for recycled LIBs material is pivotal for the sustainability of the renewable energy industry. The recycling process needs to be both economically and environmentally conscious. Direct recycling is cheaper and generates the least amount of waste compared to pyrometallurgical and hydrometallurgical processes. Direct recycling explored in this work is useful for reclaiming precious minerals from the End-of-Life (EOL) LIBs material. The EOL material has varying lithium deficiency, hence, redox mediator relithiation restores the lithium content rapidly and at low cost. The redox mechanism relithiate EOL cathode material by shuttling charges very fast between lithium metal and EOL cathode material. The redox mediator is oxidized to create lithium rich solvent and reduced to relithiate EOL cathode material. However, the process is sensitive to pH changes. The redox reaction creates acidic solvent, which may cause lithium leaching. Therefore, use of lithium hydroxide (LiOH) to remove impurities on the surface of the EOL material and as a lithium source creates a basic solution to prevent lithium leaching and relithiate EOL material. This approach will potentially pave way for fast quality cathode material recovery at a low cost.
Technoeconomic Analysis of a Direct Air Capture System Utilizing a Looped CaCO3/Ca(OH)2 Process
This presentation reports preliminary results from a screening level techno-economic analysis of a looped CaCO3/Ca(OH)2 direct air capture process. Preliminary results reveal that the looped CaCO3/Ca(OH)2 process may be cost competitive with solvent- and sorbent-based DAC technologies. Results from a detailed sensitivity analysis revealing multiple avenues for system optimization and cost reduction are presented.
Direct Observation of Two-Step, Stratified Crystallization and Morphology in Conjugated Polymer Thin Films
A two-step stratified crystallization process has been directly observed during cooling of poly(3-hexylthiophene) (P3HT) thin films of thickness h = 20-250 nm: a thin (<20 nm) layer at the free surface crystallizes ~25 °C higher than the bulk crystallization temperature (T C,bulk ), whereas the rest of the film (i.e. the underlayer) crystallizes near T C,bulk . In-situ measurements of films with and without a free surface unequivocally ascribe the high-temperature crystallization to a surface-induced process, which correlates with the formation of large birefringent structures and highly oriented edge-on crystallites at the air–polymer interface. In contrast, crystallization of the bulk-like underlayer leads to mostly edge-on-oriented crystallites in thinner films and becomes increasingly isotropic in thicker films. For h < 20 nm, free-surface effects dominate and only high-temperature crystallization is observed. These results highlight the potential of melt crystallization to tailor morphology and orientation across thin film thickness for specific electronic applications.
Radiocarbon analysis of soil microbial biomass via direct chloroform extraction
Microbial processing of soil organic matter is a significant driver of C cycling, yet we lack an understanding of what shapes the turnover of this large terrestrial pool. In part, this is due to limited options for accurately identifying the source of C assimilated by microbial communities. Laboratory incubations are the most common method for this; however, they can introduce artifacts due to sample disruption and processing and can take months to produce sufficient CO 2 for analysis. We present a biomass extraction method which allows for the direct 14 C analysis of microbial biomolecules and compare the results to laboratory incubations. In the upper 50 cm soil depths, the Δ 14 C from incubations was indistinguishable from that of extracted microbial biomass. Below 50 cm, the Δ 14 C of the biomass was more depleted than that of the incubations, either due to the stimulation of labile C decomposition in the incubations, the inclusion of biomolecules from non-living cells in the biomass extractions, or differences in C used for assimilation versus respiration. Our results suggest that measurement of Δ 14 C of microbial biomass extracts can be a useful alternative to soil incubations.