Non-Equilibrium Matter - The Next Decade and Beyond in Space Materials Research
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Designing a Dynamic Material via Interlocking Kraft Lignin with Ultrahigh Molecular Weight Poly(ethylene oxide)
The environmental issues stemming from plastic waste and the excessive use of petroleum-based chemicals are both concerning and urgent. To effectively address this problem, we need to adopt a comprehensive approach involving developing more sustainable and renewable materials. These materials should be capable of demonstrating similar or even better performance than functional polymers synthesized from petroleum-based chemicals. Our research aims to develop more sustainable materials by leveraging the intrinsic characteristics of a natural polymer, lignin, a byproduct of the biorefinery industries. We utilized the three-dimensional branching structure of lignin as a material framework. We employed an approach to co-reactive melt processing of kraft lignin with aliphatic flexible chains of soft cross-linkers through the reaction of the cross-linker epoxy chain ends with lignin functional groups. Our study demonstrates that the interlocked structure formed from the co-blending of kraft lignin with ultrahigh molecular weight poly(ethylene oxide) and the cross-linking of lignin chains through a solvent-free process can manipulate the macromolecular interactions and relaxation. This manipulation results in materials that exhibit a wide range of thermomechanical properties and self-healing and shape memory effects, with drastically improved stiffness in a single material. We have explored the fundamental understanding of the macromolecular chain relaxation dynamics originating from the interlocking structure formation. In conclusion, this investigation utilized various techniques, including thermal, mechanical, rheology, and quasi-elastic neutron scattering.
36 MATERIALS SCIENCE↗
Shear-free mixing to achieve accurate temporospatial nanoscale kinetics through scanning-SAXS: ion-induced phase transition of dispersed cellulose nanocrystals
Time-resolved in situ characterization of well-defined mixing processes using small-angle X-ray scattering (SAXS) is usually challenging, especially if the process involves changes of material viscoelasticity. In specific, it can be difficult to create a continuous mixing experiment without shearing the material of interest; a desirable situation since shear flow both affects nanoscale structures and flow stability as well as resulting in unreliable time-resolved data. Here, we demonstrate a flow-focusing mixing device for in situ nanostructural characterization using scanning-SAXS. Given the interfacial tension and viscosity ratio between core and sheath fluids, the core material confined by sheath flows is completely detached from the walls and forms a zero-shear plug flow at the channel center, allowing for a trivial conversion of spatial coordinates to mixing times. With this technique, the time-resolved gel formation of dispersed cellulose nanocrystals (CNCs) was studied by mixing with a sodium chloride solution. It is observed how locally ordered regions, so called tactoids, are disrupted when the added monovalent ions affect the electrostatic interactions, which in turn leads to a loss of CNC alignment through enhanced rotary diffusion. The demonstrated flow-focusing scanning-SAXS technique can be used to unveil important kinetics during structural formation of nanocellulosic materials. However, the same technique is also applicable in many soft matter systems to provide new insights into the nanoscale dynamics during mixing.
36 MATERIALS SCIENCE↗
Surface penetrators for planetary exploration: Science rationale and development program
Work on penetrators for planetary exploration is summarized. In particular, potential missions, including those to Mars, Mercury, the Galilean satellites, comets, and asteroids are described. A baseline penetrator design for the Mars mission is included, as well as potential instruments and their status in development. Penetration tests in soft soil and basalt to study material eroded from the penetrator; changes in the structure, composition, and physical properties of the impacted soil; seismic coupling; and penetrator deflection caused by impacting rocks, are described. Results of subsystem studies and tests are given for design of entry decelerators, high-g components, thermal control, data acquisition, and umbilical cable deployment.
Murphy, J. P.↗
Pressure-Coupled Acoustic-Transducer Assembly
Improved acoustic-transducer assembly easy to assemble, relocatable, and used at high temperatures. In assembly, piezoelectric acoustic transducer pressure-coupled to delay line or fixture through soft metal like aluminum, copper or gold. Transducer subassembly includes layered structure of coupling material, transducer, thin disk of coupling material acting as cushion for transducer, electrode disk with coaxial cable lead attached, insulation/damping material, and pressure plate. Pressure coupling precludes problem of matching coefficients of thermal expansion of transducer, coupling material, and delay line.
Parker, F. Raymond↗
Comparative study of x ray and microwave emissions during solar flares
The work supported by the grant consisted of two projects. The first project involved making detailed case studies of two flares using SMM data in conjunction with ground based observations. The first flare occurred at 1454 UT on June 20, 1989 and involved the eruption of a prominence near the limb. In the study we used data from many wavelength regimes including the radio, H-alpha, hard X-rays, and soft X-rays. We used a full gyrosynchrotron code to model the apparent presence of a 1.4 GHz source early in the flare that was in the form of a large coronal loop. The model results lead us to conclude that the initial acceleration occurs in small, dense loops which also produced the flare's hard X-ray emission. We also found evidence that a source at 1.4 GHz later in the event was due to second harmonic plasma emission. This source was adjacent to a leg of the prominence and comes from a dense column of material in the magnetic structure supporting the prominence. Finally, we investigated a source of microwaves and soft X-rays, occurring approximately 10 min after the hard X-ray peak, and calculate a lower limit for the density of the source. The second flare that was studied occurred at 2156 UT on June 20, 1989 and was observed with the VLA and the Owens Valley Radio Observatory (OVRO) Frequency Agile Array. We have developed a gyrosynchrotron model of the sources at flare peak using a new gyrosynchrotron approximation which is valid at very low harmonics of the gyrofrequency. We found that the accelerated particle densities of the sources decreased much more with radius from the source center than had been supposed in previous work, while the magnetic field varied less. We also used the available data to analyze a highly polarized source which appeared late in the flare. The second project involved compiling a statistical base for the relative timing of the hard X-ray peak, the turbulent and blue-shift velocities inferred from soft X-ray line emissions observed by SMM and the microwave peak as determined from ground-based observations. This timing was then used to aid the testing of newly developed global models for flares that incorporate the global magnetic topology as well as the electron dynamics that are responsible for the hard X-rays and microwaves.
Winglee, Robert M.↗
Giant uniaxial negative thermal expansion in FeZr 2 alloy over a wide temperature range
Negative thermal expansion (NTE) alloys possess great practical merit as thermal offsets for positive thermal expansion due to its metallic properties. However, achieving a large NTE with a wide temperature range remains a great challenge. Herein, a metallic framework-like material FeZr 2 is found to exhibit a giant uniaxial (1D) NTE with a wide temperature range (93-1078 K, $\overline{α}_{l}$=–34.01×10 –6 K –1 ). Such uniaxial NTE is the strongest in all metal-based NTE materials. The direct experimental evidence and DFT calculations reveal that the origin of giant NTE is the couple with phonons, flexible framework-like structure, and soft bonds. Interestingly, the present metallic FeZr 2 excites giant 1D NTE mainly driven by high-frequency optical branches. It is unlike the NTE in traditional framework materials, which are generally dominated by low energy acoustic branches. In the present study, a giant uniaxial NTE alloy is reported, and the complex mechanism has been revealed. It is of great significance for understanding the nature of thermal expansion and guiding the regulation of thermal expansion.
36 MATERIALS SCIENCE↗
Superconducting Quantum Metamaterials from Convergence of Soft and Hard Condensed Matter Science
Superconducting quantum metamaterials are expected to exhibit a variety of novel properties, but have been a major challenge to prepare as a result of the lack of appropriate synthetic routes to high-quality materials. Here, the discovery of synthesis routes to block copolymer (BCP) self-assembly-directed niobium nitrides and carbonitrides is described. The resulting materials exhibit unusual structure retention even at temperatures as high as 1000 °C and resulting critical temperature, T c , values comparable to their bulk analogues. Applying the concepts of soft matter self-assembly, it is demonstrated that a series of four different BCP-directed mesostructured superconductors are accessible from a single triblock terpolymer. Resulting materials display a mesostructure-dependent T c without substantial variation of the XRDmeasured lattice parameters. Lastly, field-dependent magnetization measurements of a sample with double-gyroid morphology show abrupt jumps comparable in overall behavior to flux avalanches. Results suggest a fruitful convergence of soft and hard condensed matter science.
36 MATERIALS SCIENCE↗
Colloquium : Physical properties of group-IV monochalcogenide monolayers
The state-of-the-art knowledge of ferroelectric and ferroelastic group-IV monochalcogenide monolayers is surveyed. These semiconductors feature remarkable structural and mechanical properties, such as a switchable in-plane spontaneous polarization, soft elastic constants, structural degeneracies, and thermally driven two-dimensional structural transformations. Additionally, these 2D materials display selective valley excitations, valley Hall effects, and persistent spin helix behavior. After a description of their Raman spectra, a discussion of optical properties arising from their lack of centrosymmetry (such as an unusually strong second-harmonic intensity, large bulk photovoltaic effects, photostriction, and tunable exciton binding energies) is provided as well. Here, the physical properties observed in these materials originate from (correlate with) their intrinsic and switchable electric polarization, and the physical behavior hereby reviewed could be of use in nonvolatile memory, valleytronic, spintronic, and optoelectronic devices: these 2D multiferroics enrich and diversify the 2D material toolbox.
2D ferroelectrics↗
Supramolecular-covalent hybrid polymers for light-activated mechanical actuation
Abstract not provided
Li, Chuang↗
Characterizing electronic and atomic structures for amorphous and molecular metal oxide catalysts at functional interfaces by combining soft X-ray spectroscopy and high-energy X-ray scattering
Amorphous thin film materials and heterogenized molecular catalysts supported on electrode and other functional interfaces are widely investigated as promising catalyst formats for applications in solar and electrochemical fuels catalysis. However the amorphous character of these catalysts and the complexity of the interfacial architectures that merge charge transport properties of electrode and semiconductor supports with discrete sites for multi-step catalysis poses challenges for probing mechanisms that activate and tune sites for catalysis. This minireview discusses advances in soft X-ray spectroscopy and high-energy X-ray scattering that provide opportunities to resolve interfacial electronic and atomic structures, respectively, that are linked to catalysis. This review discusses how these techniques can be partnered with advances in nanostructured interface synthesis for combined soft X-ray spectroscopy and high-energy X-ray scattering analyses of thin film and heterogenized molecular catalysts. Further, these combined approaches enable opportunities for the characterization of both electronic and atomic structures underlying fundamental catalytic function, and that can be applied under conditions relevant to device applications.
14 SOLAR ENERGY↗
What dictates soft clay-like lithium superionic conductor formation from rigid salts mixture
Abstract Soft clay-like Li-superionic conductors, integral to realizing all-solid-state batteries, have been recently synthesized by mixing rigid-salts. Here, through computational and experimental analysis, we clarify how a soft clay-like material can be created from a mixture of rigid-salts. Using molecular dynamics simulations with a deep learning-based interatomic potential energy model, we uncover the microscopic features responsible for soft clay-formation from ionic solid mixtures. We find that salt mixtures capable of forming molecular solid units on anion exchange, along with the slow kinetics of such reactions, are key to soft-clay formation. Molecular solid units serve as sites for shear transformation zones, and their inherent softness enables plasticity at low stress. Extended X-ray absorption fine structure spectroscopy confirms the formation of molecular solid units. A general strategy for creating soft clay-like materials from ionic solid mixtures is formulated.
25 ENERGY STORAGE↗
A model for the distribution of material generating the soft X-ray background
The observational evidence relating to the soft X-ray diffuse background is discussed, and a simple model for its source and spatial structure is presented. In this simple model with one free parameter, the observed 1/4 keV X-ray intensity originates as thermal emission from a uniform hot plasma filling a cavity in the neutral material of the Galactic disk which contains the sun. Variations in the observed X-ray intensity are due to variations in the extent of the emission volume and therefore the emission measure of the plasma. The model reproduces the observed negative correlation between X-ray intensity and H I column density and predicts reasonable values for interstellar medium parameters.
Snowden, S. L.↗
Swelling characteristics of DNA polymerization gels
The development of biomolecular stimuli-responsive hydrogels is important for biomimetic structures, soft robots, tissue engineering, and drug delivery. DNA polymerization gels are a new class of soft materials composed of polymer gel backbones with DNA duplex crosslinks that can be swollen by sequential strand displacement using hairpin-shaped DNA strands. The extensive swelling can be tuned using physical parameters such as salt concentration and biomolecule design. Previously, DNA polymerization gels have been used to create shape-changing gel automata with a large design space and high programmability. Here we systematically investigate how the swelling response of DNA polymerization gels can be tuned by adjusting the design and concentration of DNA crosslinks in the hydrogels or DNA hairpin triggers, and the ionic strength of the solution in which swelling takes place. Finally, we also explore the effect hydrogel size and shape have on the swelling response. Tuning these variables can alter the swelling rate and extent across a broad range and provide a quantitative connection between biochemical reactions and macroscopic material behaviour.
59 BASIC BIOLOGICAL SCIENCES↗
New Acoustic Treatment For Aircraft Sidewalls
New aircraft-sidewall acoustic treatment reduces interior noise to acceptable levels and minimizes addition of weight to aircraft. Transmission of noise through aircraft sidewall reduced by stiffening device attached to interior side of aircraft skin, constrained-layer damping tape attached to stiffening device, porous acoustic materials of high resistivity, and relatively-soft trim panel isolated from vibrations of main fuselage structure.
Vaicaitis, Rimas↗
Damage Detection and Self-Repair in Inflatable/Deployable Structures
Inflatable/deployable structures are under consideration for applications as varied as expansion modules for the International Space Station to destinations for space tourism to habitats for the lunar surface. Monitoring and maintaining the integrity of the physical structure is critical, particularly since these structures rely on non-traditional engineering materials such as fabrics, foams, and elastomeric polymers to provide the primary protection for the human crew. The closely related prior concept of monitoring structural integrity by use of built-in or permanently attached sensors has been applied to structures made of such standard engineering materials as metals, alloys, and rigid composites. To effect monitoring of flexible structures comprised mainly of soft goods, however, it will be necessary to solve a different set of problems - especially those of integrating power and data-transfer cabling that can withstand, and not unduly interfere with, stowage and subsequent deployment of the structures. By incorporating capabilities for self-repair along with capabilities for structural health monitoring, successful implementation of these technologies would be a significant step toward semi-autonomous structures, which need little human intervention to maintain. This would not only increase the safety of these structures, but also reduce the inspection and maintenance costs associated with more conventional structures.
Brandon, Erik↗
Hybrid Additive and Subtractive Manufacturing of Dual‐Wavelength Photopolymer Thermosets
Additive manufacturing (AM) techniques such as digital light processing (DLP) AM and stereolithography enable the production of highly complex structures with speed and ease as not previously possible. However, many traditional thermosetting photopolymers used in these processes result in a permanently crosslinked structure incapable of being broken down or modified without the use of energy-intensive processes such as mechanical machining or ablation. To overcome this limitation, this production is described of thiol-ene photopolymer thermosets with dual-wavelength photopolymerization and photodegradation reaction pathways. The dual wavelength selectivity of the polymerization (405 nm) and degradation (365 nm) processes, combined with dual-wavelength DLP AM technology, enables hybrid manufacturing with the ability to add and sequentially subtract material with excellent spatiotemporal control. 2D lithographs and complex 3D architectures with soft elastomeric properties are produced with resolutions as small as 50 µm. Furthermore, the ability to selectively subtract supports from 3D printed structures with deliberate and accurate control is demonstrated. In conclusion, the ability to correct or modify existing structures enables a new paradigm of adaptable materials for corrective manufacturing techniques and temporary structures.
3D Printing↗
Pressure-induced spin crossover in a Fe 78 Si 9 B 13 metallic glass
The pressure effect on structures and properties of a Fe 78 Si 9 B 13 metallic glass was investigated by in situ high-pressure synchrotron Fe Kβ x-ray emission spectroscopy and x-ray diffraction, and electrical resistivity measurements up to ~51 GPa. The study reveals a reversible and continuous pressure-induced high- to low-spin crossover of Fe atoms in an amorphous structure. The changes of the local spin moment can be scaled to match its average atomic distance shrinkage very well during compression. The crossover of electronic spin states in the Fe 78 Si 9 B 13 metallic glass resembles that of typical crystalline Fe-bearing materials but without a sharp atomic volume collapse and an abrupt electrical resistivity jump. Furthermore, these findings could help guide applications of Fe-based metallic glasses as a soft ferromagnetic material at extreme conditions and also improve our understanding of magnetism and coupling of its changes with disordered atomic structures and other properties in metallic glasses.
36 MATERIALS SCIENCE↗