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At least 19 records

Data Reproducibility of Spin-Echo Small-Angle Neutron Scattering Instruments

Spin-echo small-angle neutron scattering (SESANS) is a unique method to measure structures of materials in real space with length scales from ∼ 30 μm to ∼20 µm. As shown in Figure 1, the accessible length scale of SESANS is given by its ability to encode the momentum transfer into the Larmor phase, namely Φ = $\vec{𝛿}$ ⋅ $\vec{𝑄}$, where $\vec{𝑄}$ is the momentum transfer and $\vec{𝛿}$ is the encoding vector of the setup and its projection along Q (δQ) is called spin-echo length (SEL). The spin echo length, which is synonymous with the spatial correlation distance probed, is defined as the following 𝛿𝑄 ∝ 𝜆 2 𝐵𝐿cot𝜃 where 𝜆 is neutron wavelength, B is magnetic field, L is length of the parallelogram magnetic field region, and 𝜃 is the angle between the inclined magnetic field boundary and the beam direction, as shown in Figure 1. The result of the SESANS experiment is a Hankel transformation of the SANS scattering function I(Q), which yields the correlation function of the sample in real space.

47 OTHER INSTRUMENTATION↗

Spin echo small-angle neutron scattering using superconducting magnetic Wollaston prisms

Here, we show the implementation of superconducting magnetic Wollaston prisms for spin echo small-angle neutron scattering. Two calibration methods for the spin echo length are presented: one utilizing spin echo modulated small-angle neutron scattering and the other based on the neutron refraction by quartz wedge crystals. Our experimental results with polystyrene nano-particle colloids showcase the system’s efficacy in measuring both dilute and concentrated colloidal systems. Additionally, investigations into the pore diameter and pitch of a nano-porous alumina membrane demonstrate its capability in analyzing nano-porous materials. Furthermore, we discuss potential optimizations to further extend the accessible spin echo length.

47 OTHER INSTRUMENTATION↗

Different agglomeration properties of PC 61 BM and PC 71 BM in photovoltaic inks – a spin-echo SANS study

Fullerene derivatives are used in a wide range of applications including as electron acceptors in solution-processable organic photovoltaics. We report agglomeration of fullerene derivatives in optically opaque solutions of PC 61 BM and PC 71 BM, with concentrations ranging from 30 mg mL -1 up to 90 mg mL -1 , in different solvents with relevance to organic photovoltaics, using a novel neutron scattering technique, Spin-Echo Small Angle Neutron Scattering (SESANS). From SESANS, agglomerates with correlation lengths larger than 1 μm are found in some PC 61 BM solutions, in contrast no agglomerates are seen in PC 71 BM solutions. These results clearly show that PC 71 BM is fundamentally more soluble than PC 61 BM in the solvents commonly used in photovoltaic inks and corroborating similar observations previously achieved using other experimental techniques. Computer models are presented to study the energetics of solution and agglomeration of both species, ascribing the difference to a kinetic effect probably related to the larger anisotropy of PC 71 BM. Also, this work showcases the power of SESANS to probe agglomerates of fullerene derivatives in completely opaque solutions for agglomerates of the order of one to several microns.

36 MATERIALS SCIENCE↗

Mesoporous Silica Formation Mechanisms Probed Using Combined Spin–Echo Modulated Small-Angle Neutron Scattering (SEMSANS) and Small-Angle Neutron Scattering (SANS)

In this work, the initial formation stages of surfactant-templated silica thin films which grow at the air–water interface were studied using combined spin–echo modulated small-angle neutron scattering (SEMSANS) and small-angle neutron scattering (SANS). The films are formed from either a cationic surfactant or nonionic surfactant (C 16 EO 8 ) in a dilute acidic solution by the addition of tetramethoxysilane. Previous work has suggested a two stage formation mechanism with mesostructured particle formation in the bulk solution driving film formation at the solution surface. From the SEMSANS data, it is possible to pinpoint accurately the time associated with the formation of large particles in solution that go on to form the film and to show their emergence is concomitant with the appearance of Bragg peaks in the SANS pattern, associated with the two-dimensional hexagonal order. The combination of SANS and SEMSANS allows a complete depiction of the steps of the synthesis that occur in the subphase.

36 MATERIALS SCIENCE↗

Vitamin E Acetate Causes Softening of Pulmonary Surfactant Membrane Models

The popularity of electronic cigarettes and vaping products has launched the outbreak of a condition affecting the respiratory system of users, known as electronic-cigarette/vaping-associated lung injury (EVALI). The build-up of vitamin E acetate (VEA), a diluent of some illicit vaping oils, in the bronchoalveolar lavage of patients with EVALI provided circumstantial evidence as a target for investigation. In this work, we provide a fundamental characterization of the interaction of VEA with lung cells and pulmonary surfactant (PS) models to explore the mechanisms by which vaping-related lung injuries may be present. We first confirm the localization and uptake of VEA in pulmonary epithelial cells. Further, as PS is vitally responsible for the biophysical functions of the lungs, we explore the effect of added VEA on three increasingly complex models of PS: dipalmitoylphosphatidylcholine (DPPC), a lipid-only synthetic PS, and the biologically derived extract Curosurf. Using high-resolution techniques of small-angle X-ray scattering, small-angle neutron scattering, neutron spin–echo spectroscopy, and neutron reflectometry, we compare the molecular-scale behaviors of these membranes to the bulk viscoelastic properties of surfactant monolayer films as studied by Langmuir monolayer techniques. While VEA does not obviously alter the structure or organization of PS membranes, a consistent softening of membrane systems—regardless of compositional complexity—provides a biophysical explanation for the respiratory distress associated with EVALI and yields a new perspective on the behavior of the PS system.

59 BASIC BIOLOGICAL SCIENCES↗

Intramolecular structure and dynamics in computationally designed peptide-based polymers displaying tunable chain stiffness

Here, polymers assembled using computationally designed coiled coil bundlemers display tunable stiffness via control of interbundlemer covalent connectivity as confirmed using small-angle neutron scattering. Neutron spin echo spectroscopy reveals that rigid rod polymers show a decay rate Γ~Q 2 (Q is the scattering vector) expected of straight cylinders. Semirigid polymers assembled using bundlemers linked via 4-armed organic linker show flexible segmental dynamics at mid-Q and Γ~Q 2 behavior at high Q. The results give insight into linker flexibility-dependent interbundlemer dynamics in the hybrid polymers.

36 MATERIALS SCIENCE↗

Neutron Radiography and Computed Tomography of Biological Systems at the Oak Ridge National Laboratory's High Flux Isotope Reactor

Neutrons have historically been used for a broad range of biological applications employing techniques such as small-angle neutron scattering, neutron spin echo, diffraction, and inelastic scattering. Unlike neutron scattering techniques that obtain information in reciprocal space, attenuation-based neutron imaging measures a signal in real space that is resolved on the order of tens of micrometers. The principle of neutron imaging follows the Beer-Lambert law and is based on the measurement of the bulk neutron attenuation through a sample. Greater attenuation is exhibited by some light elements (most notably, hydrogen), which are major components of biological samples. Contrast agents such as deuterium, gadolinium, or lithium compounds can be used to enhance contrast in a similar fashion as it is done in medical imaging, including techniques such as optical imaging, magnetic resonance imaging, X-ray, and positron emission tomography. For biological systems, neutron radiography and computed tomography have increasingly been used to investigate the complexity of the underground plant root network, its interaction with soils, and the dynamics of water flux in situ. Moreover, efforts to understand contrast details in animal samples, such as soft tissues and bones, have been explored. This manuscript focuses on the advances in neutron bioimaging such as sample preparation, instrumentation, data acquisition strategy, and data analysis using the High Flux Isotope Reactor CG-1D neutron imaging beamline. The aforementioned capabilities will be illustrated using a selection of examples in plant physiology (herbaceous plant/root/soil system) and biomedical applications (rat femur and mouse lung).

Bilheux, Hassina↗

Topological shaping of vortex neutron beams using forked phase gratings

Beams of light or matter that carry well-defined states of orbital angular momentum (OAM) are promising probes of topological and textured condensed matter systems such as magnetic skyrmions. Using spin-echo small-angle neutron scattering, a phase-sensitive technique that allows for a relatively low intensity beam, we demonstrate the production of vortex neutron beams from forked phase gratings of various topological charges. This type of interferometric verification of OAM we present here could be further extended to other platforms using probes that are similarly limited by the coherence and strength of the currently available sources.

Cold atoms & matter waves↗

Time-of-flight modulated intensity small-angle neutron scattering measurement of the self-diffusion constant of water

We report that the modulated intensity by zero effort small-angle neutron scattering (MI-SANS) technique is used to measure scattering with a high energy resolution on samples normally ill-suited for neutron resonance spin echo. The self-diffusion constant of water is measured over a q–t range of 0.01–0.2 Å -1 and 70–500 ps. In addition to demonstrating the methodology of using time-of-flight MI-SANS instruments to observe diffusion in liquids, the results support previous measurements on water performed with different methods. This polarized neutron technique simultaneously measures the intermediate scattering function for a wide range of time and length scales. Two radio frequency flippers were used in a spin-echo setup with a 100 kHz frequency difference in order to create a high-resolution time measurement. The results are compared with self-diffusion measurements made by other techniques and the general applicability of MI-SANS at a pulsed source is assessed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Extended flexibility of neutron Larmor diffraction for increased diffraction range in mosaicity measurements

Larmor diffraction (LD) is a neutron scattering technique that offers enhanced resolution by harnessing the Larmor precession of neutron spins in a magnetic field. By encoding subtle changes in neutron momentum transfer into significant alterations in the Larmor phase of neutron spins, LD can be employed to measure lattice expansion, lattice distortion, and mosaicity with exceptional resolution. As originally proposed by Rekveldt et al., LD necessitates the magnetic field boundaries to be tilted to be parallel to the crystal plane of interest. Here, this report explores the fundamental principles shared between LD and spin-echo small-angle neutron scattering (SESANS). Drawing inspiration from the flexibility of SESANS to adjust magnetic field boundaries to optimize the resolution in the measurement of the neutron momentum transfers q, we will demonstrate that the strict requirement of parallel alignment between the magnetic field boundaries and the crystal plane can be relaxed for the measurements of mosaicity. Such relaxation will expand the accessible diffraction angles for these situations that are highly constrained.

Larmor diffraction↗

Understanding Interfacial Block Copolymer Structure and Dynamics

Here, block copolymer (BCP) structure and dynamics were studied using small-angle neutron scattering (SANS), neutron spin echo (NSE) spectroscopy, and molecular dynamics (MD) simulations to obtain a fundamental understanding of the impact of an interfacial block on chain dynamics. A glassy block acted as the interface, and the dynamics of a rubbery block was studied. The rubbery block was protonated near the interface in one sample and near the chain end in another sample to observe the interfacial effect on the rubbery polymer. Analysis of the structure and dynamics revealed that the interfacial rubbery block was confined in layered morphologies and exhibited much slower dynamics than the chain-end rubbery block that was dispersed in the rubbery matrix. The interfacial rubbery block showed weaker dynamical relaxation than that at the chain end, and it also had critically important length scale dependence. Dynamical slowing was only observed at length scales significantly larger than the characteristic segmental length, and the disparity between interfacial and chain-end dynamics increased with increasing length.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamical Signatures of Thermotoga maritima Maltose-Binding Proteins Affected by Ligand Binding

Functional segregation among protein isoforms depends on the interplay of their overall structures and the molecular dynamics of these structures. Thermotoga maritima maltose-binding protein (tmMBP) isoforms show size-dependent differential binding of maltose and malto-oligomers while maintaining remarkable fold conservation. This differential behavior needs detailed characterization in native-like aqueous conditions to understand the effects of protein dynamics on ligand binding and recognition. Small-angle neutron scattering (SANS), neutron spin echo (NSE) spectroscopy, and dynamic light scattering (DLS) were used in conjunction with previously published computational molecular dynamics (MD) simulations to understand the dynamic behavior of tmMBPs experimentally. SANS provided information on the overall structure of the molecules, while NSE was used to determine the dynamics in the nanosecond time scale. Both tmMBP2 and tmMBP3 have a bidomain architecture linked with a flexible hinge, with the binding pocket sitting in the cleft between the two domains. tmMBP2 and tmMBP3 showed different solution dynamics, with the translational and rotational components dominating the dynamics of both systems, resulting in a clear differentiation of their diffusion pattern. A faster dynamics component was also observed and was attributed to segmental dynamics. Differences observed between the ligand-free (apo) and ligand-bound (holo) states of the two proteins are attributed to conformational entropy. Our results highlight the intricacies of how structure and dynamics can together shape binding to a repertoire of substrates in structurally similar proteins.

Diffusion↗

Perturbation of nanoplastics on biomembranes: molecular insights from neutron scattering

Plastic waste is now pervasive in the environment, breaking down into microplastics and nanoplastics under many environmental conditions. These particles have been found in various ecosystems and even in human tissues, raising significant environmental and health concerns. In this study, we investigated the interaction of polystyrene nanoplastics, with and without surface modifications, on biomembrane structures using contrast-matching small-angle neutron scattering and neutron spin echo spectroscopy. The neutron contrast matching enabled the selective study of biomembranes in the presence of nanoplastics. Two model membranes were employed: a simple zwitterionic bilayer (i.e., dimyristoylphosphatidylcholine [DMPC]) and an Escherichia coli lipid extract as a bacterial membrane model. The results show profound membrane disruptions, including possible thinning, vesicle fragmentation, lipid monolayer formation, and inter-vesicle aggregation, with the more severe effects observed in DMPC membranes. Notably, E. coli membranes exhibited greater resilience, suggesting that natural membranes with diverse lipid compositions may reduce susceptibility to perturbation by extracellular nanoplastics. Here, these findings highlight potential risks posed by environmental nanoplastic particles to biological membranes, with insights into molecular-level interactions and the environmental toxicity of nanoplastics. This work provides a foundation for future studies into nanoplastic–biomembrane interactions and their broader implications for health and environment using neutrons.

Qian, Shuo [Oak Ridge National Laboratory (ORNL), ↗

Experimental evidence for the two-path description of neutron spin echo

Here, we describe an experiment that strongly supports a two-path interferometric model in which the spin-up and spin-down components of each neutron propagate coherently along spatially separated parallel paths in a typical neutron spin-echo small-angle scattering (SESANS) experiment. Specifically, we show that the usual semi-classical, single-path treatment of Larmor precession of a polarized neutron in an external magnetic field predicts a damping as a function of the spin-echo length of the SESANS signal obtained with a periodic phase grating when the transverse width of the neutron wave packet is finite. However, no such damping is observed experimentally, implying either that the Larmor model is incorrect or that the transverse extent of the wave packet is very large. In contrast, we demonstrate theoretically that a quantum-mechanical interferometric model in which the two mode-entangled (i.e., intraparticle entangled) spin states of a single neutron are separated in space when they interact with the grating accurately predicts the measured SESANS signal, which is independent of the wave packet width.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Spin-textured neutron beams with orbital angular momentum

In this work, we present a rigorous theoretical framework underpinning the technique of spin-echo modulated small-angle neutron scattering (SEMSANS), and show how the technique can be extended in order to generate spin-textured neutron beams with orbital angular momentum (OAM) via birefringent neutron spin-polarization devices known as magnetic Wollaston prisms. Neutron OAM beams are mathematically characterized by a “cork-screw” phase singularity e iℓΦ about the propagation axis where ℓ is the OAM quantum number. To understand the precise relationship between the emergent OAM state and the variety of spin textures realized by various setups, we have developed a path-integral approach that in the interferometric limit makes a judicious use of magnetic Snell's law. We show that our proposed technique produces a complex two-dimensional pattern of spin-OAM entangled states which may be useful as a probe of quantum magnetic materials. We compare our path-integral approach to the well-known single-path Larmor precession model and present a pedagogical derivation of magnetic Snell's law of refraction for both massive and massless particles based on Maupertuis's action principle.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Conceptual Polarization Setup at CENTAUR, the SANS/WANS Instrument at the Second Target Station of SNS

CENTAUR is a multifunctional general purpose small-angle and wide-angle neutron scattering instrument with diffraction and spectroscopic capability in the future Second Target Station at the Spallation Neutron Source of the Oak Ridge National Laboratory. To fill a gap in neutron polarization capability, the instrument will be designed to provide polarization analysis. Here we present the conceptual polarization setup at CENTAUR, as well as the Spin Echo Modulated Small-Angle Neutron Scattering setup which will further expand the length scale covered by the instrument.

Qian, Shuo↗