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At least 1,117 records · Page 62

Unlocking hidden information in sparse small-angle neutron scattering measurements

Hypothesis Small-Angle Neutron Scattering (SANS) is a powerful technique for studying soft matter systems such as colloids, polymers, and lyotropic phases, providing nanoscale structural insights. However, its effectiveness is limited by low neutron flux, leading to long acquisition times and noisy data. Here, we hypothesize that Bayesian statistical inference using Gaussian Process Regression (GPR) can reconstruct high-fidelity scattering data from sparse measurements by leveraging intensity smoothness and continuity. Experiments and Simulations The method was benchmarked computationally and validated through SANS experiments on various soft matter systems, including wormlike micelles, colloidal suspensions, polymeric structures, and lyotropic phases. GPR-based inference was applied to both experimental and synthetic data to evaluate its effectiveness in noise reduction and intensity reconstruction. Findings GPR significantly enhances SANS data quality and therefore reducing measurement times by up to two orders of magnitude. This cost-effective approach maximizes experimental efficiency, enabling high-throughput studies and real-time monitoring of dynamic systems. It is particularly beneficial for weakly scattering and time-sensitive studies. Beyond SANS, this framework applies to other low-SNR techniques, including laboratory-based small-angle X-ray scattering and various dynamical scattering methods. Furthermore, it offers transformative potential for compact neutron sources, enhancing their viability for structural analysis in resource-limited settings.

Small angle neutron scattering↗

Decoupling the effects of texture and composition on magnetic properties of Fe-Si sheet processed by shear deformation

Soft magnetic Fe-Si alloys (electrical steels) possess exceptional functional properties such as high permeability, low coercivity, and low core loss, which generally improve with increasing Si content in the alloy. However, Fe-Si alloys containing > 3.5 wt% Si are also characterized by prohibitively low workability and poor ductility that have prevented their efficient commercial production in sheet form by rolling. This has limited their use for improving efficiency of motors and transformers. In this study, hybrid cutting-extrusion (HCE) is used as a single-step thermomechanical processing method to produce continuous Fe-Si alloy sheet with high Si compositions of 4 wt% to 6.5 wt%. HCE sheet is shown to have a homogeneous annealed grain structure and simple-shear crystallographic textures. By controlling the HCE deformation path, varied crystallographic shear textures are created in the sheet. Quasi-static magnetic properties of the HCE sheet are evaluated to decouple the effects of sheet texture and Si composition on resultant permeability and coercivity properties. The results suggest that HCE, with suitable process scaling, is a viable route for production of high-Si content electrical steel sheet for next-generation motors and transformers.

36 MATERIALS SCIENCE↗

Rheological dynamics and structural characteristics of supramolecular assemblies of β-cyclodextrin and sulfonic surfactants

Cyclodextrins are highly functional compounds with a hydrophobic cavity capable of forming supramolecular inclusion complexes with various classes of molecules including surfactants. The resultant rich nanostructures and their dynamics are an interesting research problem in the area of soft condensed matter and related applications. In this paper, we report novel dynamical supramolecular assemblies based on the complexation of β-cyclodextrin with 3 different sulfonic surfactants, which are sodium hexadecylsulfate, sodium dodecylbenzenesulfonate, and myristyl sulfobetaine. It was observed that a β-cyclodextrin : surfactant/2 : 1 molar ratio was ideal for inducing axial growth and imparting large viscosities in the suspensions. Such complexation processes were accompanied by intriguing nanostructural phase behaviors and rheological properties that were very sensitive to the molecular architecture of sulfonic surfactants. The presence of an amino group in the head group of the surfactant allowed for large viscosities that reached 2.4 × 10 4 Pa s which exhibited gel-like behavior. In contrast, smaller viscosity values with a lower consistency index were observed when a bulky aromatic ring was present instead. DIC microscopy was used to visually probe the microstructure of the systems with respect to sulfonate molecular architecture. Additionally, surface tension measurements, and FTIR and NMR spectroscopies were used to gain insights into the nature of interactions that lead to the complexation and nanostructural characteristics. Finally, mechanics correlating the supramolecular morphologies to the rheological properties were proposed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling Solution Drying by Moving a Liquid-Vapor Interface: Method and Applications

A method of simulating the drying process of a soft matter solution with an implicit solvent model by moving the liquid-vapor interface is applied to various solution films and droplets. For a solution of a polymer and nanoparticles, we observe “polymer-on-top” stratification, similar to that found previously with an explicit solvent model. Furthermore, “polymer-on-top” is found even when the nanoparticle size is smaller than the radius of gyration of the polymer chains. For a suspension droplet of a bidisperse mixture of nanoparticles, we show that core-shell clusters of nanoparticles can be obtained via the “small-on-outside” stratification mechanism at fast evaporation rates. “Large-on-outside” stratification and uniform particle distribution are also observed when the evaporation rate is reduced. Polymeric particles with various morphologies, including Janus spheres, core-shell particles, and patchy particles, are produced from drying droplets of polymer solutions by combining fast evaporation with a controlled interaction between the polymers and the liquid-vapor interface. Our results validate the applicability of the moving interface method to a wide range of drying systems. The limitations of the method are pointed out and cautions are provided to potential practitioners on cases where the method might fail.

36 MATERIALS SCIENCE↗

SANS quantification of bound water in water-soluble polymers across multiple concentration regimes

Contrast-variation small-angle neutron scattering (CV-SANS) is a widely used technique for quantifying hydration water in soft matter systems, but it is predominantly applied in the dilute regime or for systems with a well-defined structure factor. Here, CV-SANS was used to quantify the number of hydration water molecules associating with three water-soluble polymers with different critical solution temperatures and types of water–solute interactions in dilute, semidilute, and concentrated solution through the exploration of novel methods of data fitting and analysis. Multiple SANS fitting workflows with varying levels of model assumptions were evaluated and compared to give insight into SANS model selection. These fitting pathways ranged from general, model-free algorithms to more standard form and structure factor fitting. In addition, Monte Carlo bootstrapping was evaluated as a method to estimate parameter uncertainty through simulation of technical replicates. The most robust fitting workflow for dilute solutions was found to be form factor fitting without CV-SANS ( i.e. polymer in 100% D 2 O). For semidilute and concentrated solutions, while the model-free approach can be mathematically defined for CV-SANS data, the addition of a structure factor imposes physical constraints on the optimization problem, suggesting that the optimal fitting pathway should include appropriate form and structure factor models. The measured hydration numbers were consistent with the number of tightly bound water molecules associated with each monomer unit, and the concentration dependence of the hydration number was largely governed by the chemistry-specific interactions between water and polymer. Polymers with weaker water–polymer interactions ( i.e. those with fewer hydration water molecules) were found to have more bound water at higher concentrations than those with stronger water–polymer interactions due to the increase in the number of forced water–polymer contacts in the concentrated system. This SANS-based method to count hydration water molecules can be applied to polymers in any concentration regime, which will lead to improved understanding of water–polymer interactions and their impact on materials design.

36 MATERIALS SCIENCE↗

Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers

Despite their adaptability and mechanical stability, Pickering emulsions based on the interfacial assembly of colloidal particles have not found use in iontronics, since the dense interfacial packing of micron-sized particles precludes functional connectivity between two droplets. In this work, we introduce a chemically reconfigurable droplet interface bilayer (DIB) platform based on the interfacial assembly of nanoparticle-surfactants (NPSs) that enables spontaneous or field-induced formation of ion-conducting nanochannels, eliminating the need of ionophores or nanochannel-forming proteins. These nanoscopic channels emerge from packing defects in the jammed interfacial assemblies of the charged NPSs and support size and charge selective, hysteretic ion transport governed by interfacial electrostatics and dimensional constraints. The NPS-DIBs show short-term and long-term plasticity, hallmarks of neuromorphic behavior, that are mediated by the structural and chemical design of the bilayer. These assemblies establish a versatile, chemically tunable platform that couples soft-matter mechanics with interfacial ionic functionality, offering a robust foundation for soft iontronic systems.

36 MATERIALS SCIENCE↗

New Laboratory and Astrophysical Probes of Physics Beyond the Standard Model (Final Technical Report)

The first of these directions centers on new ideas in dark matter detection. As experimental scrutiny narrows the window for new physics at the weak scale, it has become apparent that the solution to the dark matter mystery may not reside there. Theoretical developments such as the hidden sector/valley paradigm have, at the same time, shown that compelling theories of dark matter reside below the weak scale. Searching for dark matter at lower mass scales requires looking beyond the current paradigm of dark matter direct detection based on nuclear recoils. It is the goal of this project to provide new ideas to guide the experimental program looking for light dark matter. I am actively proposing ideas for detecting dark matter as light as a meV, well beyond the current focus of GeV-TeV scale dark matter. Some of the ideas I have proposed, such as superconducting, superfluid, and polar material targets, are actively being developed into experiments. My group will provide the relevant calculations to determine dark matter reach, providing crucial input to experiment on which targets should be developed. We will also provide an effective field theory framework to understand which types of experiments are most sensitive to each interaction type. The second of these directions is on probes of dark matter substructure as a mean to constrain, or observe, models of dark matter. The standard ΛCDM paradigm assumes that the dark matter density perturbations are adiabatic, scale invariant, and produced during inflation. However, many standard models of dark matter will produce modifications of this prediction, such as axion models with symmetry broken below the inflationary scale. Remarkably, we have limited direct measurements of the dark matter clumpiness at mass scales below dwarf galaxies. This allows for the possibility of observing modifications from vanilla ΛCDM due to particle dynamics. In many cases, simulations of dark matter structure in the presence of non-scale invariant fluctu- ations are understudied or completely lacking. I plan to develop both theoretical predictions for small scale structure in models with additional matter power on small scales, as well as observa- tional probes of small scale halos or clumps. One idea I have been recently focused on is pulsar timing, though my group will pursue a variety of lensing and astrometric probes. Lastly, the most risky direction involves spacetime fluctuations from quantum gravity. I showed that if one assumes that metric fluctuations in the Minkowski vacuum, at a surface separating a region in and out of causal contact (which we call a “horizon”), are determined by standard thermodynamic considerations at horizon, these metric fluctuations are large enough to observe in an interferometer with similar sensitivity to LIGO. In a follow-up paper we showed that these assumption holds for the vacuum in AdS/CFT. In future work, I plan to connect this work to recent soft graviton results, to frame this work in a concrete Randall-Sundrum model, and to work out concrete phenomenological predictions from the model. This work unquestionably takes a less trodden path, and works well as part of a well-rounded portfolio of less and more risky ideas. Particle physics is currently at a juncture which requires bold exploration of qualitatively new directions. This proposal outlines some of my plans over the coming years in these directions, leaving room also for surprises.

79 ASTRONOMY AND ASTROPHYSICS↗

Antichiral spin order, its soft modes, and their hybridization with phonons in the topological semimetal Mn 3 Ge

Here we report the magnetic structure and spin excitations of Mn 3 Ge , a breathing kagome antiferromagnet with transport anomalies attributed to Weyl nodes. Using polarized neutron diffraction, we show the magnetic order is a k = 0 coplanar state belonging to a Γ 9 irreducible representation, which can be described as a perfect 120 ° antichiral structure with a moment of 2.2(1) μ B /Mn, superimposed with weak collinear ferromagnetism. Inelastic neutron scattering shows three collective Q = 0 excitations at Δ 1 = 2.9 ( 6 ) meV, Δ 2 = 14.6 ( 3 ) meV, and Δ 3 = 17.5 ( 3 ) meV. A field theory of Q ≈ 0 spin waves in triangular antiferromagnets with a 120 ° spin structure was used to classify these modes. The in-plane mode ( α ) is gapless, Δ 1 is the gap to a doublet of out-of-plane spin excitations ( β x , β y ), and Δ 2 , Δ 3 result from hybridization of optical phonons with magnetic excitations. While a phenomenological spin Hamiltonian including exchange interactions, Dzyaloshinskii-Moriya interactions, and single-ion crystal field terms can describe aspects of the Mn-based magnetism, spin-wave damping [ Γ = 25 ( 8 ) meV] and the extended range of magnetic interactions indicate itinerant magnetism consistent with the transport anomalies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Soft interface instability and gas flow channeling in low-permeability deformable media

Understanding gas percolation through a clay layer or a shale formation is of great importance for the development of a geologic repository for nuclear waste disposal, a subsurface system for gas storage, and an engineering approach for hydrocarbon extraction from unconventional reservoirs. Gas injection experiments have revealed complex dynamic behaviours of gas percolation through water saturated compacted bentonite, characterized by a high breakthrough pressure, rapid breakthrough, a pressure/stress decay after the breakthrough, a relatively high migration rate, high-frequency periodic/nonperiodic variations in flow rate, stepwise rate reductions during relaxation, and low gas saturation over the whole process, all indicating channelling nature of the processes. Using linear stability analyses, we show that this channelling can autonomously emerge from the instability of the deformable interface between the injected gas and the compacted bentonite matrix driven by local stress concentration, pore dilation, and hydrologic gradient. Channel patterns formed would possess a fractal geometry. We further show that, once a percolating channel is established, the gas injected would percolate through the channel in a chain of gas bubbles, also due to the interface instability, resulting in periodic/chaotic variations in gas flow rate. Our work provides a unified explanation for key features observed for gas percolation in low-permeability deformable media. The work also suggests a possibility of designing an engineered barrier system for a nuclear waste repository that can have controllable gas release while limit water transport.

Bentonite↗

Circumventing thermodynamics to synthesize highly metastable perovskites: nano eggshells of SnHfO 3

Sn(II)-based perovskite oxides, being the subject of longstanding theoretical interest for the past two decades, have been synthesized for the first time in the form of nano eggshell particle morphologies. All past reported synthetic attempts have been unsuccessful owing to their metastable nature, i.e., by their thermodynamic instability towards decomposition to their constituent oxides. A new approach was discovered that finally provides an effective solution to surmounting this intractable synthetic barrier and which can be the key to unlocking the door to many other predicted metastable oxides. A low-melting KSn 2 Cl 5 salt was utilized to achieve a soft topotactic exchange of Sn(II) cations into a Ba-containing perovskite, i.e., BaHfO 3 with particle sizes of ~350 nm, at a low reaction temperature of 200 °C. The resulting particles exhibit nanoshell-over-nanoshell morphologies, i.e., with SnHfO 3 forming as ~20 nm thick shells over the surfaces of the BaHfO 3 eggshell particles. Formation of the metastable SnHfO 3 is found to be thermodynamically driven by the co-production of the highly stable BaCl 2 and KCl side products. Despite this, total energy calculations show that Sn(II) distorts from the A-site asymmetrically and randomly and the interdiffusion has a negligible impact on the energy of the system (i.e., layered vs. solid solution). Additionally, nano eggshell particle morphologies of BaHfO 3 were found to yield highly pure SnHfO 3 for the first time, thus circumventing the intrinsic ion-diffusion limits occurring at this low reaction temperature. In summary, these results demonstrate that the metastability of many theoretically predicted Sn(II)-perovskites can be overcome by leveraging the high cohesive energies of the reactants, the exothermic formation of a stable salt side product, and a shortened diffusion pathway for the Sn(II) cations.

36 MATERIALS SCIENCE↗

Simulation-guided analysis of resonant soft X-ray scattering for determining the microstructure of triblock copolymers

Resonant soft X-ray scattering (RSoXS) probes structure with chemical sensitivity that is useful for determining the morphology of multiblock copolymers. However, the hyperspectral scattering data produced by this technique can be challenging to interpret. Here, in this study, we use computational scattering simulations to extract the microstructure of a model triblock copolymer from the energy-dependent scattering from RSoXS. An ABC triblock terpolymer formed from poly(4-methylcaprolactone) (P4MCL), poly(2,2,2-trifluoroethylacrylate) (PTFEA), and poly (dodecylacrylate) (PDDA), P4MCL-block-PTFEA-block-PDDA, was synthesized as the model triblock system. Through quantitative evaluation of simulated scattering data from a physics-informed set of candidate structure models against experimental RSoXS data, we find the best agreement with hexagonally packed core–shell cylinders. This result is also consistent with electron-density reconstruction from hard X-ray scattering data evaluated against electron-density maps generated with the same model set. These results demonstrate the utility of simulation-guided scattering analysis to study complex microstructures that are challenging to image by microscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the solidification of quasicrystals via joint experiment and simulation (Final Report)

Quasicrystals (QCs) possess long-range positional order but non-crystallographic orientational order. Their classically ‘forbidden’ symmetry has long attracted the interest of scientists worldwide. Despite their frequent observation in both metal alloys and soft matter structures in the 35 years since their discovery, little is known about how QCs evolve from a liquid, amorphous, or crystalline precursor. In this project, we sought to resolve the enigma of QC self-assembly through a combined experimental and computational program. The Shahani group employed in situ electron and synchrotron X ray imaging to peer into the growth dynamics of QCs in a liquid, covering a broad range of length scales and solidification pathways. Glotzer's team developed new simulation models incorporating phasonic defects — which are unique to quasicrystals — and used this model to investigate two grains growing together, closely mimicking the experimental conditions. While QCs remain exceptional structures, most compounds in the realm of intermetallics adopt non-trivial geometries. In fact, only around 6% of phases are comprised of the simplest sphere packings that researchers so readily associate with metals. State-of-the-art knowledge of phase transformations at the outset of this collaborative project did not encompass the remaining 94% of intermetallic compounds that possess complex and aperiodic structure types. Therefore, we expect that outcomes from this project will have immediate and profound impact on synthesis and processing science: our efforts will be used to not only explain the growth dynamics of QCs but also complex intermetallics more broadly.

36 MATERIALS SCIENCE↗

Novel Fast Cure Silicone Inks for Single-Step, Support-Free 3D Printing of Tall, Overhanging, and High Aspect Ratio Structures

Silicone elastomers have a broad variety of applications, such as soft robotics, biomedical devices, and structural metamaterials. The extrusion-based method known as direct ink write (DIW) has enabled the production of additively manufactured silicone structures. However, this method is limited to manufacturing mostly planar or pseudo-3D structures. Due to the low self-supporting capabilities of extruded strands for traditional silicone-based “inks,” obtaining tall or overhanging structures, or structures comprised by thin walls is not feasible. Here, in this study, a novel Fast Cure silicone-based ink is demonstrated that enables manufacturing of complex 3D structures. The Fast Cure ink is a two-part mixture and silicone structures are produced by inline mixing and coextrusion of a part containing a catalyst (part A) and a part containing a crosslinker (part B). By the virtue of crosslinking, the extruded strands rapidly rigidize, increasing their self-supportive capacity. Hence, structures can be obtained with superior shape retention and previously unobtainable parts are realized that are tall, with aspect ratios higher than 3, and have overhanging features, achieving inclination angles smaller than 35° with respect to the printing plane. These minimal sag parts are achieved without requiring extra curing or mechanisms, support structures, or suspension baths.

36 MATERIALS SCIENCE↗

A soft departure from jamming: the compaction of deformable granular matter under high pressures

Here, the high-pressure compaction of three-dimensional granular packings is simulated using a bonded particle model (BPM) to capture linear elastic deformation. In the model, grains are represented by a collection of point particles connected by bonds. A simple multibody interaction is introduced to control Poisson's ratio and the arrangement of particles on the surface of a grain is varied to model both high- and low-frictional grains. At low pressures, the growth in packing fraction and coordination number follows the expected behavior near jamming and exhibit friction dependence. As the pressure increases, deviations from the low-pressure power-law scaling emerge after the packing fraction grows by approximately 0.1 and results from simulations with different friction coefficients converge. These results are compared to predictions from traditional discrete element method simulations which, depending on the definition of packing fraction and coordination number, may only differ by a factor of two. As grains deform under compaction, the average volumetric strain and asphericity, a measure of the change in the shape of grains, are found to grow as power laws and depend heavily on the Poisson's ratio of the constituent solid. Larger Poisson's ratios are associated with less volumetric strain and more asphericity and the apparent power-law exponent of the asphericity may vary. The elastic properties of the packed grains are also calculated as a function of packing fraction. In particular, we find the Poisson's ratio near jamming is 1/2 but decreases to around 1/4 before rising again as systems densify.

36 MATERIALS SCIENCE↗

Silicon wafer fracture stress for tracking sensors in particle physics experiments

For the construction of the ATLAS Inner Tracker strip detector, silicon strip sensor modules are glued directly onto carbon fibre support structures using a soft silicone gel. During tests at temperatures below -35°C, several of the sensors were found to crack due to a mismatch in coefficients of thermal expansion between polyimide circuit boards with copper metal layers (glued onto the sensor) and the silicon sensor itself. While module assembly procedures were developed to minimise variations between modules, cold tests showed a wide range of temperatures at which supposedly comparable modules failed. The observed variance (fracture temperatures between -35°C and -70°C) for supposedly comparable modules suggests an undetected variation between modules suspected to be intrinsic to the silicon wafer itself. Therefore, a test programme was developed to investigate the fracture stress of representative sensor wafer cutoffs. This paper presents results for the fracture stress of silicon sensors used in detector modules.

Detector design and construction technologies and ↗

Probing the Behavior of Composition‐Tunable Ultrathin PtNi Nanowires for CO Oxidation and Small‐Molecule Electrocatalytic Reactions

We have successfully synthesized ultrathin nanowires of pure Pt, Pt 99 Ni 1 , Pt 9 Ni 1 , and Pt 7 Ni 3 using a modified room-temperature soft-template method. Analysis of both methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR) results found that the Pt 7 Ni 3 samples yielded the best performance with specific activities of 0.36 and 0.34 mA/cm 2 respectively. Additionally, formic acid oxidation reaction (FAOR) tests noted that both Pt and PtNi nanowires oxidize small organic molecules (SOMs) via an indirect pathway. CO oxidation data suggests little measurable performance without any pre-reduction treatment; however, after annealing in H 2 , we detected significantly improved CO 2 formation for both Pt 9 Ni 1 and Pt 7 Ni 3 motifs. These observations highlight the importance of pre-treating these nanowires under a reducing atmosphere to enhance their performance for CO oxidation. To explain these findings, we collected extended x-ray adsorption fine structure (EXAFS) spectroscopy data, consistent with the presence of partial alloying with a tendency for Pt and Ni to segregate, thereby implying the formation of a Pt-rich shell coupled with a Ni-rich core. Here, we also observed that the degree of alloying within the nanowires increased after annealing in a reducing atmosphere, a finding deduced through analysis of the coordination numbers and calculations of Cowley's short range order parameters.

36 MATERIALS SCIENCE↗

A compact approach to higher-resolution resonant inelastic x-ray scattering detection using photoelectrons

The detection of inelastically scattered soft x-rays with high energy resolution usually requires large grating spectrometers. Recently, photoelectron spectrometry for analysis of x-rays (PAX) has been rediscovered for modern spectroscopy experiments at synchrotron light sources. By converting scattered photons to electrons and using an electron energy analyser, the energy resolution for resonant inelastic x-ray scattering (RIXS) becomes decoupled from the x-ray spot size and instrument length. In this work, we develop PAX towards high energy resolution using a modern photoemission spectroscopy setup studying Ba 2 Cu 3 O 4 Cl 2 at the Cu L 3 -edge. We measure a momentum transfer range of 24% of the first Brillouin zone simultaneously. Our results hint at the observation of a magnon excitation below 100 meV energy transfer and show intensity variations related to the dispersion of dd-excitations. With dedicated setups, PAX can complement the best and largest RIXS instruments, while at the same time opening new opportunities to acquire RIXS at a range of momentum transfers simultaneously and combine it with angle-resolved photoemission spectroscopy in a single instrument.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Manipulation of the orbital angular momentum of soft X-ray beams by consecutive diffractive optics

Production and manipulation of orbital angular momentum (OAM) of coherent soft X-ray beams is demonstrated utilizing consecutive diffractive optics. OAM addition is observed upon passing the beam through consecutive fork gratings. Here, the OAM of the beam was found to be decoupled from its spin angular momentum (SAM). Practical implementation of angular momentum control by consecutive devices in the X-ray regime opens new experimental opportunities, such as direct measurement of the beam’s OAM without resorting to phase-sensitive techniques, including holography. OAM analyzers utilizing fork gratings can be used to characterize the beams produced by synchrotron and free electron lasers sources; they can also be used in scattering experiments.

36 MATERIALS SCIENCE↗