We have used spin-echo small-angle neutron scattering (SESANS) to probe the hierarchy of structures present in polymer–carbon nanocomposites, with length scales spanning over three orders of magnitude, from 10 nm to 16 μm. The data processing and reduction show a unified approach across two SESANS instruments (TU Delft and Larmor at the ISIS neutron source) and yield consistent data that are able to be modelled using well-established hierarchical models in freely available software such as SasView. Using this approach, we are able to extend the measured length scales by over an order of magnitude compared to traditional scattering methods. This yields information about the structure in the bulk that is inaccessible with conventional scattering techniques (SANS/SAXS) and points to a way for interrogating and investigating polymer nanocomposites routinely across multiple length scales.@en

Plant-based meat alternatives are seeing considerable interest due to their potential to reduce environmental burden and enhance population health. The food industry, therefore, seeks routes to provide the consumer with whole-cut plant-based products that closely resemble meat products. High-moisture extrusion (HME) of plant proteins enables the industrial manufacturing of meat-like products with highly hierarchical structural organisation of fibres. The major bottleneck in serving the growing market for these products is a lack of insight into
how multiscale structures evolve during shear processing. Furthermore, it remains an open question of how two biopolymers, one being a plant protein and the other being a polysaccharide, contribute to the anisotropic structure formation during HME. This study shows how the complementary use of small-angle neutron scattering (SANS) and small-angle X-ray scattering (SAXS) can add clarity to these matters, benefiting from the different contrasts in scattering length density (SLD) encountered with each of these methods. It is demonstrated that two
biopolymers have differences in the development of structural anisotropy. The protein fibril alignment starts in the extruder section with its further development along the cooling die. On the other hand, for polysaccharide fibres, the strongest local alignment has been found in the transition zone.
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We conduct simulations of Spin Echo Small Angle Neutron Scattering (SESANS) by employing Monte Carlo methods to a setup using four magnetic Wollaston prisms. Our primary focus involves the validation of these models, encompassing monochromatic scenarios across various neutron wavelengths to ascertain the reliability of the simulations. Subsequently, we extend this validation to encompass simulations in time-of-flight mode. Our model consistently and precisely predicts the scattering patterns emanating from dilute spheres in both monochromatic and time-of-flight modes. Notably, it also accurately reproduces the intricate encoding associated with scattering occurring between the third and fourth magnetic Wollaston prism, which provides us with another approach to increase the solid angle coverage of a SESANS instrument. This validation process conclusively demonstrates the efficacy of our simulation methods. Importantly, it paves the way for simulating more intricate and realistic instrumental configurations, broadening the horizons for future research endeavours.@en

The organization of chromatin in the nuclei of rat lymphocyte was studied by time-of-flight spin-echo small-angle neutron scattering (ToF-SESANS). The procedures of the measurements in ToF and monochromatic SESANS modes were compared. It is shown that the sensitivity of the ToF method is significantly higher than that of the monochromatic mode. As a result, the SESANS correlation function can always be extracted from the ToF measurement of polarization, while this is not always the case with the monochromatic mode. The applicability of SESANS to fractal objects at the micrometre scale is demonstrated. The SESANS correlation function is well fitted by the exponential decay G(z) = exp(−z/ξ) with the correlation length ξ = 3.7 ± 0.1 µm. The exponential decay of the SESANS correlation function can be connected to the logarithmic correlation function γ(r) = ln(r/ξ) and the cubic law of the scattering intensity I(Q) = Q−3, which is in agreement with the concept of scattering from fractal objects. This finding is interpreted as evidence of a very specific logarithmic fractal structure of the large-scale organization of chromatin. The model of the logarithmic fractal is visualized as a hierarchical object obeying the volume-conservation principle at different scales.@en

A round-robin study has been carried out to estimate the impact of the human element in small-angle scattering data analysis. Four corrected datasets were provided to participants ready for analysis. All datasets were measured on samples containing spherical scatterers, with two datasets in dilute dispersions and two from powders. Most of the 46 participants correctly identified the number of populations in the dilute dispersions, with half of the population mean entries within 1.5% and half of the population width entries within 40%. Due to the added complexity of the structure factor, far fewer people submitted answers on the powder datasets. For those that did, half of the entries for the means and widths were within 44 and 86%, respectively. This round-robin experiment highlights several causes for the discrepancies, for which solutions are proposed.

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Interactive Textbook. Het boek is een algemene introductie in het elektromagnetisme, zoals in de meeste Amerikaanse universiteiten in het eerste jaar wordt gegeven. Uiteindelijk worden de wetten van Maxwell in integraal-vorm gegeven. De begrippen elektrische lading, krachten en velden worden beschreven. Hieruit wordt het begrip potentiaal gedefinieerd, met als toepassing de condensator. Vervolgens wordt er een link gelegd tussen het macroscopische en microscopische beeld van elektrische stroom. De relatie tussen stroom en magnetisch veld wordt gelegd en geïllustreerd aan de hand van spoelen. Het gedrag van condensatoren en spoelen in wisselstroomschakelingen wordt afgeleid. Tot slot laten we zien dat elektromagnetische golven voldoen aan de wetten van Maxwell. De studenten leren de wetten van Maxwell toe te passen in eenvoudige problemen. Ze leren grootheden uit te rekenen en eenvoudige afleidingen te maken. Ze passen symmetrie toe om een probleem wiskundig sterk te vereenvoudigen. @en

The spin-echo small-angle neutron scattering (SESANS) technique utilises a series of inclined magnetic fields before and after the sample to encode the scattering angle into the polarisation to obtain a much higher resolution than in conventional SANS. The analogous technique (spin echo modulated SANS (SEMSANS)) implements spin manipulations before the sample only to encode the scattering into an intensity modulation. The technique can be combined with SANS to expand the length scale range probed from 1 nm to microns. Using McStas we show that using a series of four magnetic Wollaston prisms in two orthogonal pairs with a 90° rotation can be utilised to create SEMSANS modulations in 2-D. These modulations can also be of different periods in each encoding direction. This method can be applied to anisotropic scattering samples. Also this allows for the simultaneous measurement at two orthogonal independent spin-echo lengths. This technique yields directly information about the structure of oriented structures.

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A novel spin echo small-angle neutron scattering (SESANS) concept based on a rotationally symmetric magnetic field geometry is introduced. The proposed method is similar to the conventional linear SESANS technique but uses
longitudinal precession fields and field gradients in a radial direction, as typically found in neutron spin echo (NSE) spectrometers. Radial SESANS could thus be implemented as an add-on to NSE setups. The neutron trajectory through the
instrument is encoded with the help of radial gradients generated by radial shifters, which are coils placed in the beam area similar to Fresnel coils. The present work introduces the setup of the instrument and explores its performance and the relationship between the encoded momentum transfer and the precession angle. The results indicate that radial SESANS is only sensitive to scattering along the radial direction and thus measures the projected correlation function along this direction as a function of the spin echo length, defined similarly to linear SESANS. For an evaluation of the performance of the setup, the case of scattering from solid spheres is considered and the results calculated for the radial and linear SESANS cases are compared. Also discussed is the implementation of the radial magnetic field geometry in spin echo modulated small-angle neutron scattering.@en

For the further development of spin-echo techniques to label elastic scattering it is necessary to perform simulations of the Larmor precession of neutron spins in a magnetic field. The details of some of these techniques as implemented at the reactor in Delft are simulated. First, the workings of the magnetized foil flipper are simulated. A full virtual spin-echo small-angle neutron scattering instrument is built and tested without and with a realistic scattering sample. It is essential for these simulations to have a simulated sample that also describes the transmitted beam of unscattered neutrons, which usually is not implemented for the simulation of conventional small-angle neutron scattering (SANS) instruments. Finally, the workings of a spin-echo modulated small-angle neutron scattering (SEMSANS) instrument are simulated. The simulations are in good agreement with theory and experiments. This setup can be extended to include realistic magnetic field distributions to fully predict the features of future Larmor labelling elastic-scattering instruments. Configurations can now be simulated for more complicated combinations of SANS with SEMSANS.

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Spray-drying is a widely used industrial technique and has shown an immense potential in the fields of nanoscience and technology. This is due to its ability to synthesize microgranules consisting of correlated nanostructures using evaporation induced assembly through bottom-up approach. Although the nature of correlation among the constituent nanoparticles and their size distribution could earlier be obtained by conventional Small-angle Scattering (SAS) technique, a statistically averaged quantitative measure of the shell thickness and hollowness of the formed granules remained a challenge. In this work, we have used Spin-echo Small-angle Neutron Scattering (SESANS) technique to characterize spray-dried nanostructured microgranules having different hollowness. It is shown that this non-destructive technique provided precise quantification of the granular sizes and hollowness by utilizing polarization property of neutrons in real space directly.

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Small angle scattering is frequently applied to study the anisotropy in complex soft matter systems. One emerging application is to probe the multi-scale structure in food matrices; while few models are available to describe the anisotropic scattering pattern in a quantitative, yet simple manner. For this purpose, anisotropy is introduced to the Guinier–Porod model to study the scattering from non-spherical objects with a preferred orientation. This generalised anisotropic Guinier–Porod model can be adapted to approximate the sector scattering from both cylinders and ellipsoids (both prolate and oblate). In practice, it is applied to describe the anisotropic scattering from fibres in a meat analogue made of calcium caseinate. A good agreement is found between fitted dimensions of the fibres and those observed from the microscopy image. The effect of orientation distribution on the shape and intensity of the scattering pattern is further discussed and three means to obtain the orientation distribution of the symmetry axis are proposed. Given the model is straightforward and the fitting remains phenomenological, it provides a novel approach to extract information from complex food systems.

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By introducing hydrophilic polymers into silicone medical devices, highly beneficial biomedical properties can be realized. An established solution to introduce hydrophilic polymers is to form an interpenetrating polymer network (IPN) by performing the hydrogel synthesis in the presence of silicone swollen in supercritical carbon dioxide. The precise distribution of the two polymers is not known, and determining this is the goal of this study. Neutron scattering and microscopy were used to determine the distribution of the hydrophilic guest polymer. Atomic force microscopy revealed that the important length scale on the surface of these materials is 10–100 nm, and spin-echo small-angle neutron scattering (SESANS) on IPNs submerged in D₂O revealed structures of the same scale within the interior and enabled quantification of their size. SESANS with hydration by D₂O proved to be the only scattering technique that could determine the structure of the bulk of these types of materials, and it should be used as an important tool for characterizing polymer medical devices.

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Spin-echo small-angle neutron scattering (SESANS) yields structural information on length scales from 30 nanometres up till 20 micrometres. These length scales match nicely those of colloids, protein networks and fat droplets, which are present in many food materials. This makes SESANS an excellent probe to study food materials. An interesting feature of SESANS is the real space character of the raw data. Several examples of quantitative neutron scattering studies on food materials are shortly reviewed.@en

Functionalized biomass waste sources of cellulose have drawn attention due to their high availability and sustainability properties. In this work we characterize the structural and flow properties of high-pressure homogenized citrus fiber cellulose dispersions, employing SAXS, rheology and rheo-MRI techniques. The high-pressure treatment disrupts the microfibrillar network within the citrus fibers, but leaves the individual microfibrils intact. Under moderate shear (0.1-100 s^-1) in a confined (<1 mm) geometry, these functionalized citrus fiber cellulose dispersions exhibit thixotropic shear-banding behavior accompanied by cooperative flow of microfibril flocs with correlation lengths ξ ~ 100 μm. The presented findings form a basis towards understanding and manipulating the structural and rheological properties of non-wood biomass cellulose microfibrils under industrially-relevant conditions.

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Phospholipid gum mesostructures formed in crude soybean oil after water degumming (WD) and enzymatic degumming (ED) were studied at a range of phospholipid and water concentrations. For ED, phospholipase C (PLC), phospholipase A2 (PLA2) and a mixture of phospholipases Purifine 3G (3G) were used. Both WD and ED resulted in lamellar liquid-crystalline phases, however, of different topology. The dependence of the bilayer spacings (as observed by SANS and SAXS) on the ratio between amount of water and amphiphilic lipids differed for WD and PLA2 ED vs PLC and 3G ED. This difference was also observed for dynamics at molecular scale as observed by time-domain (TD) NMR and attributed to partial incorporation of diglycerides and free fatty acids into gum bilayers after PLC and 3G ED. Feasibility of using TD-NMR relaxometry for quantification of the gum phase and estimation of degumming efficiency was demonstrated.

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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 (C16EO8) 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.

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Pronounced fibres are formed through simple shearing of a dense calcium caseinate dispersion. Both mechanical tests and scanning electron microscopy images demonstrate that the material is anisotropic. It is hypothesised that calcium caseinate aggregates, under shear, align into micro-fibres and bundle further into a hierarchical structure. Yet no direct evidence at the sub-micron length scale can support the assumption. Small angle neutron scattering (SANS) experiments were conducted on calcium caseinate samples prepared at different conditions. Analysis of the SANS data revealed that the micro-fibres have a diameter of ∼100nm and a length of ∼300nm. The addition of enzyme and air contributed to longer and thinner micro-fibres. Furthermore, the extent of fibre alignment at the micro-scale and the macroscopic anisotropy index followed the same trends with varying processing conditions. It is concluded that the material does indeed possess a hierarchical structure and the micro-fibres are responsible for the anisotropy on the macro-scale.

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SESANS data analysis has been implemented in the SasView software package, allowing SESANS experiments to be analyzed using a numerical Hankel transformation of isotropic small-angle scattering (SAS) models. The error of the numerical approximation is three orders of magnitude below typical experimental errors. All advanced data fitting features of SasView (multi-model fitting, batch fitting, and simultaneous/constrained fitting) are now also available for SESANS and this is demonstrated by examples of fitting SAS models to SESANS measurements.

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