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At least 595 records · Page 33

Enhancing Adhesion: Relative Merits of Different Approaches

Adhesive performance is improved mainly by manipulation of the bimaterials interface zone, which is only a few molecules thick. There are three approaches to enhancement of interfacial adhesion at the molecular level. They are 1) changing the nonchemically bonded interactions across the interface from weak ones to strong ones, 2) making the true interfacial area much larger than the simple geometric area, and 3) inducing chemical bonding between the two materials forming the interface. Our goal this summer was to question some of the built-in assumptions contained within these approaches and to determine the most promising approach, both theoretically and practically, for enhancing adhesion in NASA structures. Our computations revealed that all three of these approaches have, in theory, the potential to enhance molecular adhesion approximately ten-fold. Experiments, however, revealed that this excellent level of enhancement is not likely to be reached in practice. Each approach was found to be severely limited by practical problems. In addition, some of the built-in assumptions associated with these approaches were found to be insufficient or inadequate. The first approach, changing the nonchemically bonded interactions from weak to strong, Is an example of one containing inadequate assumptions. The extensive literature on intermolecular interactions, based on solution studies, shows that certain functional group pairs interact much more strongly than others. It has always been assumed that these data can be reliably extended to systems where only one member of the pair is in solution and the other Is contained in a solid surface. Our experiments this summer demonstrated that solution data do not adequately predict the strength of functional group interaction at the solid-liquid interface. Furthermore, the strong solvents needed to dissolve the monomers or polymers to which the functional groups of interest are attached compete successfully with the solid surface for the functional group. As a result, functional groups in solution cannot pair with the complementary groups in the solid surface, and the expected enhancement of nonchemically bonded interactions is not realized. The second approach, increasing the true interfacial area, is an example of one containing inadequate assumptions and suffering from numerous practical problems. First, practitioners have assumed that material removal, such as bead blasting or etching, increases true surface area (and therefore interfacial area) in a meaningful way. Our geometric analysis demonstrated that removal methods increase area by a factor of two at most. To increase interfacial area by an order of magnitude or more. a thin layer of high porosity must be added to the substrate surface prior to application of the adhesive phase. Consistent with this finding, we attempted to create a thin layer of rigid, highly porous glass on the surface of our smooth glass substrate by means of sol-gel technology. We were unable to surmount a wide variety of practical problems and obtained only collapsed, nonporous layers. Thus this approach, appealing in principle, would require long term development and is not promising in the near term. The third approach, inducing chemical bonding at the interface, is an example of one having neither inadequate assumptions nor insurmountable practical problems. When silicate glass is the substrate, there are only a few chemical reactions that can be successfully conducted to create these chemical bonds, and these reactions usually involve silicon-containing reagents. We compared the silazane reagents to the silane reagents and found through experiment that the silazanes react with the glass surface much more readily, and under milder conditions, than the silanes. The functional groups attached to the glass surface by silazane reactions were not able to be removed by solvent extraction, elevated temperature exposure, or mechanical action. This clearly indicates that the formation of chemical bonds at the interface is the most effective approach for enhancing molecular adhesion.

Penn, L. S.↗

Catalytic Triad-Inspired Nanozyme Catalysts for Ester Hydrolysis in Organic Solvent Mixtures

We synthesized a series of molecular nanozyme catalysts containing functional groups (imidazole, carboxylic acid, and hydroxyl groups) inspired by the catalytic triad found in natural serine hydrolases. Different structural features were incorporated using two distinct synthesis routes to investigate the influence of interactions beyond the active site on catalytic activity in designing molecular nanozymes. Molecular dynamics simulations suggest that nanozyme activity is affected by structural features that influence nanozyme hydrophilicity and the organization of the local solvent environment. The most active nanozyme showed activity comparable to the enzyme α-chymotrypsin for the hydrolysis of a model ester (4-nitrophenyl 4- hydroxybenzoate) in a 95:5 (v/v%) water/acetonitrile mixture at ambient temperature. Increasing the temperature and organic solvent content decreases the activity of α-chymotrypsin while enhancing the activity of the nanozymes. The nanozymes can be immobilized on supported metal nanoparticles using a dithiol self-assembled monolayer, which facilitates their removal from the postreaction solution. These results demonstrate the potential in creating solvent-tolerant bioinspired catalysts, thereby combining the advantages of biocatalysts and chemical catalysts as next-generation industrial catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A coarse-grained model of clay colloidal aggregation and consolidation with explicit representation of the electrical double layer

The aggregation of clay minerals in liquid water exemplifies colloidal self-assembly in nature. These negatively charged aluminosilicate platelets interact through multiple mechanisms with different sensitivities to particle shape, surface charge, aqueous chemistry, and interparticle distance and exhibit complex aggregation structures. Experiments have difficulty resolving the associated colloidal assemblages at the scale of individual particles. Conversely, all-atom molecular dynamics (MD) simulations provide detailed insight on clay colloidal interaction mechanisms, but they are limited to systems containing a few particles. We develop a new coarse-grained (CG) model capable of representing assemblages of hundreds of clay particles with accuracy approaching that of MD simulations, at a fraction of the computational cost. Our CG model is parameterized based on MD simulations of a pair of smectite clay particles in liquid water. A distinctive feature of our model is that it explicitly represents the electrical double layer (EDL), i.e., the cloud of charge-compensating cations that surrounds the clay particles. Our model captures the simultaneous importance of long-range colloidal interactions (i.e., interactions consistent with simplified analytical models, already included in extant clay CG models) and short-range interactions such as ion correlation and surface and ion hydration effects. The resulting simulations correctly predict, at low solid-water ratios, the existence of ordered arrangements of parallel particles separated by water films with a thickness up to ~10 nm and, at high solid-water ratios, the coexistence of crystalline and osmotic swelling states, in agreement with experimental observations.

54 ENVIRONMENTAL SCIENCES↗

Atomistic understanding of interdependence of crystal growth of two seeds embedded in glass

Recent results showed that during growth, a crystal seed embedded in glass experiences nonuniform forces from the host matrix. This result raised the possibility that during devitrification of glass, the growth of a crystal can be affected by the presence of neighboring crystals. To investigate the nature of any such interdependence of growth of neighboring crystals, atomic scale morphology of two seeds growing in a glass matrix was simulated as a function of their separation and relative misorientation. The results show a coupled rotation of seeds driven by (1) non-uniform forces from the surrounding glass, and (2) mutual interactions between the seeds. At small separations and low misorientation, each seed rotates toward perfect alignment, ultimately forming a single crystal. The onset and rate of alignment, as well as subsequent crystal growth, are strongly dependent on the growth temperature. In contrast, at larger separations and higher misorientation, the seeds cannot achieve full alignment before coalescing, resulting in polycrystalline structures.

36 MATERIALS SCIENCE↗

How Silica Surface Chemistry Modulates Interfacial Water: Insights from Machine Learning Molecular Dynamics

Controlling water structure and dynamics at silica interfaces are central to a wide range of technologies, including protective oxide layers for solar water splitting and nanoporous membranes. In this work, we develop a machine learning interatomic potential, trained via active learning, to achieve ab initio accuracy for water confined between hydroxylated silica surfaces over a range of silanol coverages and slit widths. We find that partially hydroxylated surfaces (50 and 75% OH) support stronger water−surface hydrogen bonding and more extended interfacial density profiles than fully hydroxylated (100% OH) surfaces, indicating that increasing OH coverage does not necessarily strengthen interfacial hydrogenbond networks. Translational diffusion decreases approximately linearly with slit width and OH coverage, whereas rotational dynamics respond nonlinearly. In particular, at the smallest slit width of 5 Å, 75% OH coverage produces an enhanced local tetrahedral ordered interfacial network that strongly suppresses reorientation, while 100% coverage yields a crowded, disordered interfacial layer that also hinders rotation. In contrast, the 50% OH coverage is sufficiently sparse that it does not markedly alter water structure or dynamics under confinement. These results show that coupled control of pore size and surface chemistry enables nonlinear tuning of interfacial water structure and transport, providing a design strategy for optimizing porous silica for either enhanced interfacial stability and controlled reactivity or rapid and selective transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring Microphase Separation in Semi-Fluorinated Diblock Copolymers: A Combined Experimental and Modeling Investigation

We report the combined experimental and theoretical study of the bulk self-assembly behavior of polystyrene-blockpoly( 2,3,4,5,6-pentafluorostyrene) diblock copolymers. These block copolymers were designed to create highly antagonistic blocks (with a high Flory−Huggins interaction parameter, χ) with minimum disruption to the molecular construct (i.e., only replacing five hydrogen atoms with five fluorine atoms). A large library of diblock copolymers (41 samples) was synthesized by reversible addition− fragmentation chain transfer (RAFT) polymerization to map out a major portion of the phase space. All block copolymers exhibited narrow molecular weight distributions with dispersity (D) values between 1.07 and 1.32, and subsequent thermal annealing revealed phase separation into well-defined nanoscale morphologies depending on their molecular composition, as determined from small-angle X-ray scattering and transmission electron microscopy analyses, with an experimental phase diagram being constructed. The χ value at 25 °C for this block copolymer was estimated to be 0.2 using strong segregation theory, based on trends in phase-separated domain spacing and interfacial width. When applying theoretical approaches, the majority of the domain spacing data trends were captured by a coil−coil diblock copolymer model; however, a better fit to the data for samples with shorter fluorinated blocks was obtained with a rod−coil model, indicating that the chains in these fluorinated blocks likely have a higher inherent stiffness and were thus rod-like. This observation demonstrates that, due to the very high value of χ, a transition from coil−coil to rod−coil behavior can be obtained purely by reducing the length of the stiffer of the two blocks and without varying temperature or the chemical composition of the polymers. Here, this work showcases the presence of strong microphase separation within AB diblock copolymers despite the relatively similar chemical composition of the constituent “A” and “B” units, with a clear transition from rod−coil to coil−coil segregation behavior.

RAFT polymerization↗

Influence of Carbon-Nitride Dot-Emitting Species and Evolution on Fluorescence-Based Sensing and Differentiation

Carbon dots have attracted widespread interest for sensing applications based on their low cost, ease of synthesis, and robust optical properties. We investigate structure–function evolution on multiemitter fluorescence patterns for model carbon-nitride dots (CNDs) and their implications on trace-level sensing. Hydrothermally synthesized CNDs with different reaction times were used to determine how specific functionalities and their corresponding fluorescence signatures respond upon the addition of trace-level analytes. Archetype explosives molecules were chosen as a testbed due to similarities in substituent groups or inductive properties (i.e., electron withdrawing), and solution-based assays were performed using ratiometric fluorescence excitation–emission mapping (EEM). Analyte-specific quenching and enhancement responses were observed in EEM landscapes that varied with the CND reaction time. We then used self-organizing map models to examine EEM feature clustering with specific analytes. Finally, the results reveal that interactions between carbon-nitride frameworks and molecular-like species dictate response characteristics that may be harnessed to tailor sensor development for specific applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Substrate binding plasticity revealed by Cryo-EM structures of SLC26A2

SLC26A2 is a vital solute carrier responsible for transporting essential nutritional ions, including sulfate, within the human body. Pathogenic mutations within SLC26A2 give rise to a spectrum of human diseases, ranging from lethal to mild symptoms. The molecular details regarding the versatile substrate-transporter interactions and the impact of pathogenic mutations on SLC26A2 transporter function remain unclear. Here, using cryo-electron microscopy, we determine three high-resolution structures of SLC26A2 in complexes with different substrates. These structures unveil valuable insights, including the distinct features of the homodimer assembly, the dynamic nature of substrate binding, and the potential ramifications of pathogenic mutations. This structural-functional information regarding SLC26A2 will advance our understanding of cellular sulfate transport mechanisms and provide foundations for future therapeutic development against various human diseases.

59 BASIC BIOLOGICAL SCIENCES↗

Trapping of spermine, Kukoamine A, and polyamine toxin blockers in GluK2 kainate receptor channels

Abstract Kainate receptors (KARs) are a subtype of ionotropic glutamate receptor (iGluR) channels, a superfamily of ligand-gated ion channels which mediate the majority of excitatory neurotransmission in the central nervous system. KARs modulate neuronal circuits and plasticity during development and are implicated in neurological disorders, including epilepsy, depression, schizophrenia, anxiety, and autism. Calcium-permeable KARs undergo ion channel block, but the therapeutic potential of channel blockers remains underdeveloped, mainly due to limited structural knowledge. Here, we present closed-state structures of GluK2 KAR homotetramers in complex with ion channel blockers NpTx-8, PhTx-74, Kukoamine A, and spermine. We find that blockers reside inside the GluK2 ion channel pore, intracellular to the closed M3 helix bundle-crossing gate, with their hydrophobic heads filling the central cavity and positively charged polyamine tails spanning the selectivity filter. Molecular dynamics (MD) simulations of our structures illuminate interactions responsible for different affinity and binding poses of the blockers. Our structures elucidate the trapping mechanism of KAR channel block and provide a template for designing new blockers that can selectively target calcium-permeable KARs in neuropathologies.

Science & Technology - Other Topics↗

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

Physics↗

A butterfly-shaped acceptor with rigid skeleton and unique assembly enables both efficient organic photovoltaics and high-speed organic photodetectors

ABSTRACT It remains challenging to design efficient bifunctional semiconductor materials in organic photovoltaic and photodetector devices. Here, we report a butterfly-shaped molecule, named WD-6, which exhibits low energy disorder and small reorganization energy due to its enhanced molecular rigidity and unique assembly with strong intermolecular interaction. The binary photovoltaic device based on PM6:WD-6 achieved an efficiency of 18.41%. Notably, an efficiency of 19.42% was achieved for the ternary device based on PM6:BTP-eC9:WD-6. Moreover, the photodetection device based on WD-6 demonstrated an ultrafast response speed (205 ns response time at λ of 820 nm) and a high cutoff frequency of −3 dB (2.45 MHz), surpassing the values of most commercial Si photodiodes. Based on these findings, we showcased an application of the WD-6-based photodetection device in high-speed optical communication. These results offer valuable insights into the design of organic semiconductor materials capable of simultaneously exhibiting high photovoltaic and photodetective performance.

Science & Technology - Other Topics↗

Degradation studies of SMRM Teflon

A working group was organized to study materials and components of the Solar Max Satellite (SMS) that was returned by the STS 41C. These materials were exposed in space for 50 months and represent the only real time long term exposure data available to date. In the molecular modeling of material and energetic oxygen atom interaction, it is pointed out that the importance of developing correlation between accelerated exposure data from STS and some real time data. In particular, it was predicted that Teflon which showed no detectable degradation on various STS flights may be susceptible to atomic oxygen degradation under real time conditions. Initial inspection of returned SMS samples showed that Teflon suffered visual damage such as cracking and yellowing. The results of examination of these samples are given.

Liang, R. H.↗

Degradation studies of SMRM teflon

Teflon samples returned from the Solar Max Satellite (SMS) suffered noticeable damage such as cracking and yellowing. This is in contrast to teflon exposed aboard STS-5 and STS-8 which showed no detectable changes. Selected teflon tape samples from SMS were studied to evaluate the extent and mechanism of degradation. ESCA studies revealed that these teflon samples contain hydrocarbon segments which were susceptible to oxygen atom degradation. Mechanical measurements also showed bulk property changes as a result of LEO exposure. A molecular model of material and energetic oxygen atom interaction was proposed. SMS data and the importance of developing correlation between accelerated exposure data from STS and ground-based testing and real time data will be presented.

Liang, Ranty H.↗

Indirect measurement of N-14 quadrupolar coupling for NH3 intercalated in potassium graphite

A method for indirect measurement of the nuclear quadrupolar coupling was developed and applied to NH3 molecules in the graphite intercalation compound K(NH3)4.3C24, which has a layered structure with alternating carbon and intercalant layers. Three triplets were observed in the H-1 NMR spectra of the compound. The value of the N-14 quadrupolar coupling constant of NH3 (3.7 MHz), determined indirectly from the H-1 NMR spectra, was intermediate between the gas value of 4.1 MHz and the solid-state value of 3.2 MHz. The method was also used to deduce the (H-1)-(H-1) and (N-14)-(H-1) dipolar interactions, the H-1 chemical shifts, and the molecular orientations and motions of NH3.

Tsang, T.↗

Qualitative models for space system engineering

The objectives of this project were: (1) to investigate the implications of qualitative modeling techniques for problems arising in the monitoring, diagnosis, and design of Space Station subsystems and procedures; (2) to identify the issues involved in using qualitative models to enhance and automate engineering functions. These issues include representing operational criteria, fault models, alternate ontologies, and modeling continuous signals at a functional level of description; and (3) to develop a prototype collection of qualitative models for fluid and thermal systems commonly found in Space Station subsystems. Potential applications of qualitative modeling to space-systems engineering, including the notion of intelligent computer-aided engineering are summarized. Emphasis is given to determining which systems of the proposed Space Station provide the most leverage for study, given the current state of the art. Progress on using qualitative models, including development of the molecular collection ontology for reasoning about fluids, the interaction of qualitative and quantitative knowledge in analyzing thermodynamic cycles, and an experiment on building a natural language interface to qualitative reasoning is reported. Finally, some recommendations are made for future research.

Forbus, Kenneth D.↗

High-Temperature Shape Memory Polymers

physical conformation changes when exposed to an external stimulus, such as a change in temperature. Such materials have a permanent shape, but can be reshaped above a critical temperature and fixed into a temporary shape when cooled under stress to below the critical temperature. When reheated above the critical temperature (Tc, also sometimes called the triggering or switching temperature), the materials revert to the permanent shape. The current innovation involves a chemically treated (sulfonated, carboxylated, phosphonated, or other polar function group), high-temperature, semicrystalline thermoplastic poly(ether ether ketone) (Tg .140 C, Tm = 340 C) mix containing organometallic complexes (Zn++, Li+, or other metal, ammonium, or phosphonium salts), or high-temperature ionic liquids (e.g. hexafluorosilicate salt with 1-propyl-3- methyl imidazolium, Tm = 210 C) to form a network where dipolar or ionic interactions between the polymer and the low-molecular-weight or inorganic compound forms a complex that provides a physical crosslink. Hereafter, these compounds will be referred to as "additives". The polymer is semicrystalline, and the high-melt-point crystals provide a temporary crosslink that acts as a permanent crosslink just so long as the melting temperature is not exceeded. In this example case, the melting point is .340 C, and the shape memory critical temperature is between 150 and 250 C. PEEK is an engineering thermoplastic with a high Young fs modulus, nominally 3.6 GPa. An important aspect of the invention is the control of the PEEK functionalization (in this example, the sulfonation degree), and the thermal properties (i.e. melting point) of the additive, which determines the switching temperature. Because the compound is thermoplastic, it can be formed into the "permanent" shape by conventional plastics processing operations. In addition, the compound may be covalently cross - linked after forming the permanent shape by S-PEEK by applying ionizing radiation ( radiation, neutrons), or by chemical crosslinking to form a covalent permanent network. With respect to other shape memory polymers, this invention is novel in that it describes the use of a thermoplastic composition that can be thermally molded or solution-cast into complex "permanent" shapes, and then reheated or redissolved and recast from solution to prepare another shape. It is also unique in that the shape memory behavior is provided by a non-polymer additive.

Yoonessi, Mitra↗

The Cosmic-Ray and Gas Content of the Cygnus Region as Measured in Gamma Rays by the Fermi Large Area Telescope

Context. The Cygnus region hosts a giant molecular-cloud complex which actively forms massive stars. Interactions of cosmic rays with interstellar gas and radiation fields make it shine at y-ray energies. Several gamma-ray pulsars and other energetic sources are seen in this direction. Aims. In this paper we analyse the gamma-ray emission measured by the Fermi Large Area Telescope in the energy range from 100 Me V to 100 Ge V in order to probe the gas and cosmic-ray content over the scale of the whole Cygnus complex. The gamma-ray emission on the scale of the central massive stellar clusters and from individual sources is addressed elsewhere. Methods. The signal from bright pulsars is largely reduced by selecting photons in their off-pulse phase intervals. We compare the diffuse gamma-ray emission with interstellar gas maps derived from radio/mm-wave lines and visual extinction data. and a global model of the region, including other pulsars and gamma-ray sources, is sought. Results. The integral H I emissivity above 100 MeV averaged over the whole Cygnus complex amounts to 12.06 +/- 0.11 (stat.) (+0.15 -0.84) (syst.J] x 10(exp -26) photons /s / sr / H-atom, where the systematic error is dominated by the uncertainty on the H I opacity to calculate its column densities. The integral emissivity and its spectral energy distribution are both consistent within the systematics with LAT measurements in the interstellar space near the solar system. The average X(sub co) N(H2)/W(sub co) ratio is found to be [1.68 +/- 0.05 (stat.) (H I opacity)] x 1020 molecules cm-2 (K km/s /r, consistent with other LAT measurements in the Local Arm. We detect significant gamma-ray emission from dark neutral gas for a mass corresponding to approx 40% of that traced by CO. The total interstellar mass in the Cygnus complex inferred from its gamma-ray emission amounts to 8(+5 -1) x 10(exp 6) Solar M at a distance of 1.4 kpc. Conclusions. Despite the conspicuous star formation activity and large masses of the interstellar clouds, the cosmic-ray population in the Cygnus complex averaged over a few hundred parsecs is similar to that of the local interstellar space.

Ackermann, M.↗