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At least 271 records · Page 15

2D Semiconductor Nanosheets Supported on Colloidal Quantum Cubes

Two-dimensional (2D) colloidal nanocrystals bridge the physics of epitaxial quantum wells with the synthetic scalability of solution-processed nanomaterials, making them an attractive platform for future LEDs, lasers, and photodetectors. However, their strongly anisotropic 2D morphology complicates the formation of close-packed films required for electrically interfaced devices. Here, we address this limitation by introducing semiconductor quantum cubes (QCs) in which 2D CdSe nanosheets are conformally grown on six faces of CdS cubic scaffolds. This architecture preserves excitonic physics of quasi-2D nanosheets while leveraging the mechanical rigidity and self-assembly of nanocubes, enabling close-packed films with improved electronic coupling and electrical conductivity. By extending CdS/CdSe QCs into a CdS/CdSe/CdS core/shell/shell structure, we realize 2D quantum wells that exhibit unusual multiexciton behavior. In particular, CdS/CdSe/CdS QCs show repulsive exciton–exciton interactions, which decouple CdSe facets into quasi-independent emitters. This leads to the suppressed Auger recombination, long multiexciton lifetimes, and broadband optical gain. The demonstrated combination of unusual multiexciton photophysics and favorable film self-assembly characteristics in QCs presents opportunities for solution-processed optoelectronic devices.

perovskites↗

Complex Phase Transitions of Fully Rigid Sphere–Rod Amphiphiles Induced by Solvent Polarity in Dilute Solutions

Here we report complex macrophase and microphase transitions of rigid amphiphiles with spherical Keggin molecular clusters as the solvophilic block and rod-like rigid oligofluorene (OF) as the solvophobic block in mixed solvents of water and polar organic solvent. By properly adjusting the solvent polarity, the amphiphiles are found to respond accordingly by self-assembling into multilayered incomplete onion-like structures (10–25 vol % THF), single-layered vesicular structures (60 vol % THF), and an unexpected macrophase separation in the middle (40–50 vol % THF), which is due to the anomalous trends in Keggin solubility as a result of the nature of TBA + counterions. The rigidity of the OF block prevents the amphiphile from assembling by following the rule of packing parameters; instead, interdigitation among different rods leads to the formation of the solvophobic domain to achieve self-assembly. The incomplete onion structures are controlled by the interdigitation of rigid rods for the number of layers and the electrostatic interaction among Keggin head groups for the interlayer distance. When the degree of interdigitation becomes lower, the self-assembly process shows a trend that can be explained by the traditional rule of packing parameter. This study demonstrates the formation of different self-assembled structures by rigid amphiphiles and their transitions induced by solvent composition. The self-assembly (microphase separation) of rigid amphiphiles in a dilute solution could indeed represent a broad area containing complicated, uncharted rules.

36 MATERIALS SCIENCE↗

Conjunction Assessment and Deconfliction Paradigm for Co-Located Satellite Constellations With on-Spacecraft “Autonomous” Flight Dynamics Control

Satellite constellations that employ on-spacecraft flight dynamics and conjunction assessment (CA) approaches face particular challenges. First, they must arrange to obtain and upload to the constellation satellite close approach information, such as Conjunction Data Messages, so that their on-board systems will have the data they need to make informed CA decisions. Second, given current latencies in obtaining CA screening information, such systems often cannot obtain dedicated screenings of their proposed maneuvers before they are executed. Third, they usually cannot engage in real time with owner/operators (O/Os) with whom they may come into conjunction, relying instead on pre-arranged courses of action that may or may not fit a given situation well. Despite these difficulties, it is nonetheless possible, as operators such as SpaceX have demonstrated, to operate safely using on-board CA calculations, in the presence of a largely collaborative operating environment. The situation breaks down, however, when two constellations that operate with such a paradigm are placed in the same orbital region and will experience conjunctions with each other. Each may have a vague idea of where the other’s satellites are, or perhaps even a somewhat precise idea if they exchange O/O ephemerides, but neither will know the other’s more immediate maneuver intentions, especially for situations in which they are in a high-risk conjunction with each other and a mitigation maneuver is required. As there is no formalized way for these automated systems to ascertain each other’s intentions for this type of conjunction, it is quite possible that each spacecraft may choose a maneuver that results in the two objects’ colliding. An opportunity to develop a solution to this problem was presented by the NASA “Starling” project, a small experimental constellation developed to demonstrate autonomous satellite control and constellation reconfiguration and for which a launch was obtained that, serendipitously, will place this constellation close to the SpaceX Starlink constellation. Because the NASA constellation is experimental, an extended mission part of the mission has been negotiated to implement and test mechanisms for resolving the problem of co-located constellations with on-board flight dynamics control. For the last eighteen months, a consortium among NASA Ames (the Starling satellite providers), NASA CARA (the Agency organization responsible for conjunction assessment), Space X, and the Department of Commerce (in observer status) has met regularly to assemble a concept of operations for a robust solution to this problem and has developed a prototype ground node that will serve as a needed CA screening and information dispensary. The approach and methods, as well as the active employment of the developed ground node, will be tested both in simulation before actual use and then in actual spacecraft operations, which are anticipated to begin in January 2024. This paper will describe the co-located autonomously-controlled constellation problem and the developed solution in detail, outlining what ground node (i.e., government) infrastructure and features are required, what particular capabilities are needed by the constellations themselves in order to make use of this deconfliction paradigm, and the migration path forward to allow such a capability set to be incorporated by the Department of Commerce’s space traffic coordination system.

Conjunction Assessment↗

A process for preparing an assembly of an article and a polyimide which resists dimensional change, delamination, and debonding when exposed to changes in temperature

An assembly of an article and a polyimide composition is prepared. The assembly resists dimensional change, delamination, or debonding when exposed to changes to temperature. An article is provided. A polyamic acid solution which yields a polyimide having a low coefficient of thermal expansion (CTE) was prepared. Equimolar quantities of an aromatic diamine and an aromatic dianhydride were reacted in a solvent medium to form a polyamic acid solution. A metal ion containing additive was added to the solution. Examples of this additive are: TbCl3, DyCl3, ErCl3, TmCl3, Al(C5H7O2)3, and Er2S3. The polyamic acid solution was imidized and is combined with the article to form the assembly.

Stoakley, Diane M.↗

Advanced Technology Blade testing on the XV-15 Tilt Rotor Research Aircraft

The XV-15 Tilt Rotor Research Aircraft has just completed the first series of flight tests with the Advanced Technology Blade (ATB) rotor system. The ATB are designed specifically for flight research and provide the ability to alter blade sweep and tip shape. A number of problems were encountered from first installation through envelope expansion to airplane mode flight that required innovative solutions to establish a suitable flight envelope. Prior to operation, the blade retention hardware had to be requalified to a higher rated centrifugal load, because the blade weight was higher than expected. Early flights in the helicopter mode revealed unacceptably high vibratory control system loads which required a temporary modification of the rotor controls to achieve higher speed flight and conversion to airplane mode. The airspeed in airplane mode was limited, however, because of large static control loads. Furthermore, analyses based on refined ATB blade mass and inertia properties indicated a previously unknown high-speed blade mode instability, also requiring airplane-mode maximum airspeed to be restricted. Most recently, a structural failure of an ATB cuff (root fairing) assembly retention structure required a redesign of the assembly. All problems have been addressed and satisfactory solutions have been found to allow continued productive flight research of the emerging tilt rotor concept.

Wellman, Brent↗

Process for preparing an assembly of an article and a polyimide which resists dimensional change, delamination and debonding when exposed to changes in temperature

An assembly of an article and a polyimide composition is prepared. The assembly resists dimensional change, delamination, or debonding when exposed to changes in temperature. An article is provided. A polyamic acid solution which yields a polyimide having a low coefficient of thermal expansion (CTE) was prepared. Equimolar quantities of an aromatic diamine and an aromatic dianhydride were reacted in a solvent medium to form a polyamic acid solution. A metal ion-containing additive was added to the solution. Examples of this additive are: TbCl3, DyCl3, ErCl3, TmCl3, Al(C5H7O2)3, and Er2S3. The polyamic acid solution was imidized and is combined with the article to form the assembly.

Stoakley, Diane M.↗

Structural Characterization of the Platinum Nanoparticle Hydrogen-Evolving Catalyst Assembled on Photosystem I by Light-Driven Chemistry

Directed assembly of abiotic catalysts onto biological redox protein frameworks is of interest as an approach for the synthesis of biohybrid catalysts that combine features of both synthetic and biological materials. In this report, we provide a multiscale characterization of the platinum nanoparticle (NP) hydrogen-evolving catalysts that are assembled by light-driven reductive precipitation of platinum from an aqueous salt solution onto the photosystem I protein (PSI), isolated from cyanobacteria as trimeric PSI. The resulting PSI-NP assemblies were analyzed using a combination of X-ray energy-dispersive spectroscopy (XEDS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), small-angle X-ray scattering (SAXS), and high-energy X-ray scattering with atomic pair distribution function (PDF) analyses. The results show that the PSI-supported NPs are approximately 1.8 nm diameter disk-shaped particles that assemble at discrete sites with 145 Å separation. This separation is too large to be consistent with NP nucleation and growth at a site adjacent to the F B cofactor site. Instead, we suggest a mechanism for NP growth at hydrophobic sites on the PSI stromal surface. The NPs photoreductively assembled on the PSI stromal surface are found to be analogous to the nanostructures produced by successive cycles of atomic layer deposition (ALD) of platinum onto 40 nm porous anodic alumina oxide supports, although the mechanisms for nucleation appear to differ. In conclusion, this work establishes a foundation for the investigation of the reductive assembly of abiotic metal catalysts at sites connected to photochemically reducing equivalent production in PSI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Internal Microstructure Dictates Interactions of Polymer-grafted Nanoparticles in Solution

Understanding the effects of polymer brush architecture on particle interactions in solution is requisite to enable the development of functional materials based on self-assembled polymer-grafted nanoparticles (GNPs). Static and dynamic light scattering of polystyrene-grafted silica particle solutions in toluene reveals that the pair interaction potential, inferred from the second virial coefficient, A 2 , is strongly affected by the grafting density, σ, and degree of polymerization, N, of tethered chains. In the limit of intermediate σ (~0.3 to 0.6 nm -2 ) and high N, A 2 is positive and increases with N. This confirms the good solvent conditions and can be qualitatively rationalized on the basis of a pair interaction potential derived for grafted (brush) particles. In contrast, for high σ > 0.6 nm -2 and low N, A 2 displays an unexpected reversal to negative values, thus indicating poor solvent conditions. These findings are rationalized by means of a simple analysis based on a coarse-grained brush potential, which balances the attractive core-core interactions and the excluded volume interactions imparted by the polymer grafts. The results suggest that the steric crowding of polymer ligands in dense GNP systems may fundamentally alter the interactions between brush particles in solution and highlight the crucial role of architecture (internal microstructure) on the behavior of hybrid materials. The effect of grafting density also illustrates the opportunity to tailor the physical properties of hybrid materials by altering geometry (or architecture) rather than a variation of the chemical composition.

36 MATERIALS SCIENCE↗

Method for Making a Fuel Cell from a Solid Oxide Monolithic Framework

The invention is a novel solid oxide fuel cell (SOFC) stack comprising individual bi-electrode supported fuel cells in which a thin electrolyte is supported between electrodes of essentially equal thickness. Individual cell units are made from graded pore ceramic tape that has been created by the freeze cast method followed by freeze drying. Each piece of graded pore tape later becomes a graded pore electrode scaffold that subsequent to sintering, is made into either an anode or a cathode by means of appropriate solution and thermal treatment means. Each cell unit is assembled by depositing of a thin coating of ion conducting ceramic material upon the side of each of two pieces of tape surface having the smallest pore openings, and then mating the coated surfaces to create an unsintered electrode scaffold pair sandwiching an electrolyte layer. The opposing major outer exposed surfaces of each cell unit is given a thin coating of electrically conductive ceramic, and multiple cell units are stacked, or built up by stacking of individual cell layers, to create an unsintered fuel cell stack. Ceramic or glass edge seals are installed to create flow channels for fuel and air. The cell stack with edge sealants is then sintered into a ceramic monolithic framework. Said solution and thermal treatments means convert the electrode scaffolds into anodes and cathodes. The thin layers of electrically conductive ceramic become the interconnects in the assembled stack.

Cable, Thomas L.↗

Key Intermediate Nanostructures in the Self-Assembly of Amphiphilic Polypeptoids Revealed by Cryo-TEM

Amphiphilic copolypeptoids are known to form a variety of nanostructures (fibers, tubes, sheets, etc.), but the assembly mechanisms and key intermediates remain underexplored. This study investigates the intermediate structures formed during the early stages of self-assembly in diblock copolypeptoids using cryo-transmission electron microscopy (cryo-TEM). Here we focused on two diblock copolypeptoids, one with a free N-terminus and the other with a capped N-terminus, which ultimately form less-ordered nanofibers and well-ordered nanosheets, respectively. Through cryo-TEM imaging of vitrified solutions at various time points during the self-assembly process, the study identified micelles and vesicles as key intermediate structures. Notably, the formation of vesicles as intermediates is unusual in crystallization-driven self-assembly and suggests a unique pathway in polypeptoid self-assembly. The study provides direct imaging evidence of key intermediates in polypeptoid self-assembly, advancing the understanding of their self-assembly mechanisms.

59 BASIC BIOLOGICAL SCIENCES↗

Gratings Fabricated on Flat Surfaces and Reproduced on Non-Flat Substrates

A method has been developed for fabricating gratings on flat substrates, and then reproducing the groove pattern on a curved (concave or convex) substrate and a corresponding grating device. First, surface relief diffraction grating grooves are formed on flat substrates. For example, they may be fabricated using photolithography and reactive ion etching, maskless lithography, holography, or mechanical ruling. Then, an imprint of the grating is made on a deformable substrate, such as plastic, polymer, or other materials using thermoforming, hot or cold embossing, or other methods. Interim stamps using electroforming, or other methods, may be produced for the imprinting process or if the same polarity of the grating image is required. The imprinted, deformable substrate is then attached to a curved, rigid substrate using epoxy or other suitable adhesives. The imprinted surface is facing away from the curved rigid substrate. As an alternative fabrication method, after grating is imprinted on the deformable substrate as described above, the grating may be coated with thin conformal conductive layer (for example, using vacuum deposition of gold). Then the membrane may be mounted over an opening in a pressured vessel in a manner of a membrane on a drum, grating side out. The pressure inside of the vessel may be changed with respect to the ambient pressure to produce concave or convex membrane surface. The shape of the opening may control the type of the surface curvature (for example, a circular opening would create spherical surface, oval opening would create toroidal surface, etc.). After that, well-known electroforming methods may be used to create a replica of the grating on the concave or convex membrane. For example, the pressure vessel assembly may be submerged into an electro-forming solution and negative electric potential applied to the metal coated membrane using an insulated wire. Positive electric potential may be then applied to a nickel or other metal plate submerged into the same solution. Metal ions would transfer from the plate through the solution into the membrane, producing high fidelity metal replica of the grating on the membrane. In one variation, an adhesive may be deposited on the deformable substrate, and then cured without touching the rigid, curved substrate. Edges of the deformable substrate may be attached to the rigid substrate to ensure uniform deformation of the deformable substrate. The assembly may be performed in vacuum, and then taken out to atmospheric pressure conditions to ensure that no air is trapped between the deformable and rigid substrates. Alternatively, a rigid surface with complementary curvature to the rigid substrate may be used to ensure uniform adhesion of the deformable substrate to the rigid substrate. Liquid may be applied to the surface of the deformable substrate to uniformly distribute pressure across its surface during the curing or hardening of the adhesive, or the film may be pressed into the surface using a deformable object or surface. After the attachment is complete, the grooves may be coated with reflective or dielectric layers to improve diffraction efficiency.

Content, David↗

Ionic liquid mediated one-step perpendicular assembly in block copolymer thin films for ultrafiltration membrane applications

The rapid rise of oil and gas, petrochemical, food processing, and pharmaceutical industries has added a complex mixture of contaminants like oil, particulates, metals, and other organic compounds to wastewater. Multipurpose membranes with precise pore structure can offer a solution to this problem and block copolymers (BCP) can be used to achieve such structures. Achieving vertical assembly of BCP domains provides a perfect template for developing uniform through film channels for separation and transport of material, besides being useful for the rectification of defects in photolithography patterns. Producing such morphologies may require extensive film/substrate processing and is not always feasible for scale-up. With this article, we demonstrate a facile solution casting method to induce vertical domain assembly in as-cast diblock copolymer thin films in the presence of an ionic liquid (IL) additive that preferentially segregates to one block and neutralizes interfacial interactions. We also show the tunability of domain sizes by controlling the additive concentration. These vertically aligned morphologies are important for the development of next-generation lithographic techniques and form excellent templates for ultrafiltration membranes with uniform pore sizes. In conclusion, this article demonstrates how IL additives can be used to obtain stable non-equilibrium morphologies in as-cast BCP films and the effect of BCP molecular mass, block volume fractions, and IL content on self-assembly.

59 BASIC BIOLOGICAL SCIENCES↗

Towards the specification of consecutive steps in macromolecular lignin assembly

When Pinus taeda cell suspension cultures are exposed to 8% sucrose solution, the cells undergo significant intracellular disruption, irregular wall thickening/lignification with concomitant formation of an 'extracellular lignin precipitate. However, addition of potassium iodide (KI), an H202 scavenger, inhibits this lignification response, while the ability to synthesize the monolignols, p-coumaryl and coniferyl alcohols, is retained. Lignin synthesis (i.e. polymerization) is thus temporarily correlated with H202 generation, strongly implying a regulatory role for the latter. Time course analyses of extracellular metabolites leading up to polymer formation reveal that coniferyl alcohol, but not p-coumaryl alcohol, undergoes substantial coupling reactions to give various lignans. Of these, the metabolites, dihydrodehydrodiconiferyl alcohol, shonanin (divanillyl tetrahydrofuran) and its apparent aryl tetralin derivative, cannot be explained simply on the basis of phenolic coupling. It is proposed that these moieties are the precursors of so-called reduced substructures in the lignin macromolecule. This adds a new perspective to the lignin assembly mechanism.

Non-NASA Center↗

Developing Benzodithiophene-Free donor polymer for 19.36% efficiency Green-Solvent-Processable organic solar cells

Here, in this work, a newly benzodithiophene-free D-A polymer donor, named PDTP-BDD, was developed for realizing green-solvent processed high-performance OSCs. By bridging two electron-rich unit of dithieno[3,2-b:2',3'-d]pyridin-5(4H)-one (DTP) and electron-deficient benzo[1,2-c:4,5c']dithiophene-4,8-dione (BDD) with thiophene units, PDTP-BDD possesses high absorption in the short wavelength range and a deep HOMO energy level. The rigid building blocks also make PDTP-BDD has strong aggregation and poor solubility in common halogen-free solvents (such as o-xylene) at room temperature, but it is readily dissolved and disaggregated at high temperature (120 °C). After cooling down to a lower temperature (60 °C), PDTP-BDD self-assembled and pre-aggregated slowly in the solution at a long time. By employing a delayed processing strategy in the layer-by-layer processed OSCs (LbL-OSCs), an optimized fibril network of the underling layer was realized, enabling the permeation of acceptor into the donor network. The optimized PDTP-BDD/L8-BO-based LbL-OSCs realized a high PCE of 18.42 %. By adding a small amount of D18 to further optimize the PDTP-BDD fibril network, an impressive PCE of 19.36 % was achieved finally in the resulting ternary LbL-OSCs, which is the highest value for OSCs processed by halogen-free solvents.

36 MATERIALS SCIENCE↗

Tetrapodal textured Janus textiles for accessible menstrual health

Menstruating individuals without access to adequate hygiene products often improvise with alternatives that pose health risks and limit their participation in society. We describe here a menstrual hygiene product based on low-cost materials, which are integrated onto fabrics to imbue unidirectional permeability. A body-facing "Janus" fabric top layer comprising ZnO tetrapods spray-coated onto polyester mosquito netting imparts hierarchical texturation, augmenting the micron-scale texturation derived from the weave of the underlying fabric. The asymmetric coating establishes a gradient in wettability, which underpins flash spreading and unidirectional permeability. The hygiene product accommodates a variety of absorptive media, which are sandwiched between the Janus layer and a second outward-facing coated densely woven fabric. An assembled prototype demonstrates outstanding ability to wick saline solutions and a menstrual fluid simulant while outperforming a variety of commercially alternatives. The results demonstrate a versatile menstrual health product that provides a combination of dryness, discretion, washability, and safety.

60 APPLIED LIFE SCIENCES↗

Verification of the ENDF/B-VII.1 Based MC 2 -3 Library Rev.1

The MC 2 -3 code, developed by Argonne National Laboratory under the DOE-NE NEAMS program, is a multigroup cross section generation code for fast reactor applications. Last year, the ENDF/B-VII.0 (E70) MC 2 -3 library, which has been extensively used, verified, and validated over a long period, was intensively reverified and updated to support the commercial grade dedication (CGD) requirement of the TerraPower Natrium project. This year, the ENDF/B-VII.1 (E71) MC 2 -3 library, the preliminary version of which was generated several years ago, was regenerated and rigorously verified to support the Natrium project as well as the completion of verification of the E71 library. The E71 library was verified using the process developed during the verification of the E70 library, including comparisons of cross sections with the NJOY-generated cross sections, comparisons of the resolved resonance cross sections with those using the PEDNF library, and comparison of total cross sections with the sum of partial cross sections. Additional verifications were conducted to ensure that the benchmark problem solutions with the E71 library are reasonable compared to the corresponding Monte Carlo solutions. Furthermore, the E71 gamma library was generated, which includes data for prompt gamma, delayed gamma, and delayed beta as well as neutron and gamma heating. The gamma library was verified at the level of individual isotopes. The EBR-II core solutions from MC 2 -3/ DIF3D and MCNP were compared, demonstrating that those solutions in terms of k-effective and assembly powers were in good agreement.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Calibration and performance of the energetic X-ray imaging telescope experiment

The final integration and testing of the Energetic X-ray Imaging Telescope Experiment (EXITE) are described. The detector and telescope as finally assembled are described, and problems as well as solutions are detailed. The preflight calibration of the position-sensitive NaI detector revealed unanticipated effects in the energy spectra. In particular, an effect due to surface roughness (lack of firm optical polishing) on the crystal was found and calibrated. The radial variation of gain and resolution in the detector was also measured, and so-called flat fielding methods have been derived to analyze the data. The integration of the EXITE detector and gondola systems is described. Several novel features were developed for the EXITE gondola, most notably a shock absorber system. The performance of the detector and gondola systems was evaluated on a first balloon flight from Australia (May 1988) and a second flight from Ft. Sumner, New Mexico (October 1988).

Braga, Joao↗