Who made the noise? Systematic approach for the assessment of neutron imaging scintillators.

We propose a method to analyze the characteristics of scintillator screens for neutron imaging applications. Using calculations based on the theory of cascaded linear steps as well as experimental measurements, we compared the characteristics of different lithium- and gadolinium-based scintillator screens. Our results show that, despite their much lower light output, gadolinium-based scintillators outperform lithium-based scintillators in terms of noise characteristics for a variety of imaging setups. However, the relative performance of scintillator screens is highly dependent on the other setup characteristics such as the beam spectrum, field of view, used optical lens and size of the camera sensor. Consequently, the selection of the best scintillator screen - as well as the scintillator characteristics assessment in new developments - requires a systematic consideration of all these elements, as enabled by the framework presented here.

Chloride-induced corrosion of steel in concrete-insights from bimodal neutron and X-ray microtomography combined with ex-situ microscopy.

The steel-concrete interface (SCI) is known to play a major role in corrosion of steel in concrete, but a fundamental understanding is still lacking. One reason is that concrete's opacity complicates the study of internal processes. Here, we report on the application of bimodal X-ray and neutron microtomography as in-situ imaging techniques to elucidate the mechanism of steel corrosion in concrete. The study demonstrates that the segmentation of the specimen components of relevance-steel, cementitious matrix, aggregates, voids, corrosion products-obtained through bimodal X-ray and neutron imaging is more reliable than that based on the results of each of the two techniques separately. Further, we suggest the combination of tomographic in-situ imaging with ex-situ SEM analysis of targeted sections, selected based on the segmented tomograms. These in-situ and ex-situ characterization techniques were applied to study localized corrosion in a very early stage under laboratory chloride-exposure conditions, using reinforced concrete cores retrieved from a concrete bridge. Several interesting observations were made. First, the acquired images revealed the formation of several corrosion sites close to each other. Second, the morphology of the corrosion pits was relatively shallow. Finally, only about half of the total 31 corrosion initiation spots were in close proximity to interfacial macroscopic air voids, and > 90% of the more than 160 interfacial macroscopic air voids were free from corrosion. The findings have implications for the mechanistic understanding of corrosion of steel in concrete and suggest that multimodal in-situ imaging is a valuable technique for further related studies. Supplementary Information: The online version contains supplementary material available at 10.1617/s11527-024-02337-7.

Hydrogen Transport and Evolution in Ni-MH Batteries by Neutron Imaging.

Efficiency losses due to side reactions are one of the main challenges in battery development. Despite providing valuable insights, the results of standard analysis on the individual components cannot be simply extrapolated to the full operating system. Therefore, non-destructive, and high resolution approaches that allow the investigation of the full system are desired. Herein, we combined neutron radiography and tomography with electrical monitoring of the state of charge of commercial Ni-mischmetal hydride batteries, to track the exchange and transport of hydrogen under operating conditions. This non-destructive approach allowed both the quantification of the hydrogen distribution in the electrodes in 4D, and the distinction between the electrochemically exchanged hydrogen and the hydrogen gas pressure generated by side reactions, as a function of the applied potential and current. One of the most counter-intuitive observation is that the generation of hydrogen gas during discharge depends on the charging state of the battery. The results presented provide critical new insights in the mechanisms governing the electrochemical processes during Nimischmetal hydride battery operation, and also pave the way for the extrapolation of this approach to the investigation of state-of-the-art Li-ions batteries.

Decomposing Magnetic Dark-Field Contrast in Spin Analyzed Talbot-Lau Interferometry: A Stern-Gerlach Experiment without Spatial Beam Splitting.

We have recently shown how a polarized beam in Talbot-Lau interferometric imaging can be used to analyze strong magnetic fields through the spin dependent differential phase effect at field gradients. While in that case an adiabatic spin coupling with the sample field is required, here we investigate a nonadiabatic coupling causing a spatial splitting of the neutron spin states with respect to the external magnetic field. This subsequently leads to no phase contrast signal but a loss of interferometer visibility referred to as dark-field contrast. We demonstrate how the implementation of spin analysis to the Talbot-Lau interferometer setup enables one to recover the differential phase induced to a single spin state. Thus, we show that the dark-field contrast is a measure of the quantum mechanical spin split analogous to the Stern-Gerlach experiment without, however, spatial beam separation. In addition, the spin analyzed dark-field contrast imaging introduced here bears the potential to probe polarization dependent small-angle scattering and thus magnetic microstructures.

Visibility simulation of realistic grating interferometers including grating geometries and energy spectra.

The performance of X-ray and neutron grating interferometers is characterised by their visibility, which is a measure for the maximum achievable contrast. In this study we show how the real grating geometry in a grating interferometer with three gratings impacts the interference and self projection that leads to visibility in the first place. We quantify the individual contributions of wavelength distributions and grating shapes in terms of visibility reduction by determining the absolute as well as relative effect of each contribution. The understanding of the impact of changed geometry and wavelength distributions on the interference of neutrons/X-rays allows us to present the first fully quantitative model of a grating interferometer setup. We demonstrate the capability of the simulation framework by building a model of the neutron grating interferometer at the ICON beamline and directly comparing simulated and measured visibility values. The general nature of the model makes it possible to extend it to any given grating interferometer for both X-rays and neutrons.

Neutron instrument concepts for a high intensity moderator at the European spallation source.

In the course of the Horizon 2020 project HighNESS, a second moderator concept has been developed for the European Spallation Source, which complements the currently built moderator and is optimized for high intensity with a large viewable surface area. In this work we introduce conceptual designs for neutron instruments for condensed matter research designed to make optimal use of the capabilities of this moderator. The focus is on two concepts for small-angle neutron scattering and one neutron imaging instrument, which are intended to complement corresponding instruments that are already under construction at the European Spallation Source. One small-angle neutron scattering instrument concept resembles a conventional pinhole collimator geometry and aims to profit from the proposed second moderator by enabling to illuminate larger samples and providing particularly high resolution, drawing on a 30 m collimation and corresponding detector distance. A second small-angle neutron scattering instrument concept adopts nested mirror optics that enable to efficiently exploit the large moderator size and provide high resolution by focusing on the detector. The neutron imaging instrument concept is a typical pinhole instrument that can be found at continuous sources and draws on the corresponding strengths of high flux and large homogeneous fields-of-view, while still providing moderate wavelength resolution for advanced imaging methods.

Multi-directional neutron dark-field imaging with single absorption grating.

Neutron dark-field imaging is a powerful technique for investigating the microstructural properties of materials through high-resolution full-field mapping of small-angle scattering. However, conventional neutron dark-field imaging utilizing Talbot-Lau interferometers is limited to probing only one scattering direction at a time. Here, we introduce a novel multi-directional neutron dark-field imaging approach that utilizes a single absorption grating with a two-dimensional pattern to simultaneously probe multiple scattering directions. The method is demonstrated to successfully resolve fiber orientations in a carbon compound material as well as the complex morphology of the transformed martensitic phase in additively manufactured stainless steel dogbone samples after mechanical deformation. The latter results reveal a preferential alignment of transformed domains parallel to the load direction, which is verified by EBSD. The measured real-space correlation functions are in good agreement with those extracted from the EBSD map. Our results demonstrate that multi-directional neutron dark-field imaging is overcoming significant limitations of conventional neutron dark-field imaging in assessing complex heterogeneous anisotropic microstructures and providing quantitative structural information on multiple length scales.

Revealing the impact of temperature in battery electrolytes via wavelength-resolved neutron imaging.

Understanding the limitations of electrolyte mixtures under extreme conditions is key to ensure reliable and safe battery performance. Among advanced characterization methods, time-of-flight neutron imaging (ToF-NI) is unique for its capability to map physicochemical changes of H-containing materials inside metallic casings and battery packs. The technique, however, requires long exposures in pulsed sources, which limits its applicability, particularly for analysis at low temperatures. To overcome these limitations, we use high-duty cycle ToF-NI at a continuous source, demonstrating its capability to expose physical and chemical changes of electrolytes due to variations in the overall molecular diffusion. The strategy described in this work reduces the exposure required and provides the baseline to study the thermal stability of electrolyte mixtures, from the proofing of state-of-the-art electrolyte mixtures up to their performance in batteries. This analysis and methodology apply to hydrogenous materials well beyond electrolytes for a wide range of applications.

Phase separation in a ternary DPPC/DOPC/POPC system with reducing hydration.

The maintenance of plasma membrane structure is vital for the viability of cells. Disruption of this structure can lead to cell death. One important example is the macroscopic phase separation observed during dehydration associated with desiccation and freezing, often leading to loss of permeability and cell death. It has previously been shown that the hybrid lipid 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC) can act as a line-active component in ternary lipid systems, inhibiting macroscopic phase separation and stabilising membrane microdomains in lipid vesicles [1]. The domain size is found to decrease with increasing POPC concentration until complete mixing is observed. However, no such studies have been carried out at reduced hydration. To examine if this phase separation is unique to vesicles in excess water, we have conducted studies on several binary and ternary model membrane systems at both reduced hydration ("powder" type samples and oriented membrane stacks) and in excess water (supported lipid bilayers) at 0.2 mol fraction POPC, in the range where microdomain stabilisation is reported. Differential scanning calorimetry (DSC) and Fourier transform infrared spectroscopy (FTIR) are used to map phase transition temperatures, with X-ray and neutron scattering providing details of the changes in lipid packing and phase information within these boundaries. Atomic force microscopy (AFM) is used to image bilayers on a substrate in excess water. In all cases, macroscopic phase separation was observed rather than microdomain formation at this molar ratio. Thus POPC does not stabilise microdomains under these conditions, regardless of the type of model membrane, hydration or temperature. Thus we conclude that the driving force for separation under these conditions overcomes any linactant effects of the hybrid lipid.

Correlative study of liquid in human bone by 3D neutron microscopy and lab-based X-ray µCT.

Liquid plays an important role in bone that has a complex 3D hierarchical pore structure. However, liquid (water) is difficult to discern from e.g. an organic matrix by X-ray imaging. Therefore, we use a correlative approach using both high resolution X-ray and neutron imaging. Human femoral bone with liquid adsorbed into some of the pores was imaged with both the Neutron Microscope at the ICON beamline, SINQ at PSI, and by lab-based µCT using 2.7 µm voxel size. Segmentation of the two datasets showed that, even though the liquid was clearly distinguishable in the neutron data and not in the X-ray data, it remained challenging to segment it from bone due to overlaps of peaks in the gray level histograms. In consequence, segmentations from X-ray and neutron data varied significantly. To address this issue, the segmented X-ray porosities was overlaid on the neutron data, making it possible to localize the liquid in the vascular porosities of the bone sample and use the neutron attenuation to identify it as H2O. The contrast in the neutron images was lowered slightly between the bone and the liquid compared to the bone and the air. This correlative study shows that the complementary use of X-rays and neutrons is very favorable, since H2O is very distinct in the neutron data, while D2O, H2O, and organic matter can barely be distinguished from air in the X-ray data.

Tem-per-ature dependence in Bragg edge neutron transmission measurements.

A systematic study has been carried out to investigate the neutron transmission signal as a function of sample tem-per-ature. In particular, the experimentally de-ter-mined wavelength-dependent neutron attenuation spectra for a martensitic steel at tem-per-atures ranging from 21 to 700°C are com-pared with simulated data. A theoretical description that includes the Debye-Waller factor in order to describe the tem-per-ature influence on the neutron cross sections was im-plemented in the nxsPlotter software and used for the simulations. The analysis of the attenuation coefficients at varying tem-per-atures shows that the missing contributions due to elastic and inelastic scattering can be clearly distinguished: while the elastically scattered intensities decrease with higher tem-per-atures, the inelastically scattered intensities increase, and the two can be separated from each other by analysing unique sharp features in the form of Bragg edges. This study presents the first systematic approach to qu-antify this effect and can serve as a basis , for example, to correct measurements taken during in situ heat treatments, in many cases being a prerequisite for obtaining qu-anti-fiable results.

NEURAP-A Dedicated Neutron-Imaging Facility for Highly Radioactive Samples.

NEURAP is a dedicated set-up at the Swiss neutron spallation source (SINQ) at the Paul Scherrer Institut (PSI), optionally implemented as a special configuration of the neutron-imaging station NEUTRA. It is one of very few instrumentations available worldwide enabling neutron-imaging of highly radioactive samples to be performed routinely, with special precautions and following a specific procedure. Since the relevant objects are strong γ-sources, dedicated techniques are needed to handle the samples and to perform neutron-imaging despite the radiation background. Dysprosium (Dy)-loaded imaging plates, effectively made sensitive to neutrons only, are employed. Neutrons are captured by Dy during neutron irradiation. Then the imaging plate is erased removing gamma detections. A subsequent relatively long self-exposure by the radiation from the intrinsic neutron-activated Dy within the imaging plate yields the neutron-only radiograph that is finally read out. During more than 20 years of NEURAP operation, images have been obtained for two major applications: (a) highly radioactive SINQ target components were investigated after long-term operation life; and (b) spent fuel rods and their cladding from Swiss nuclear power plants were characterized. Quantitative analysis of the image data demonstrated the accumulation of spallation products in the lead filled "Cannelloni" Zircaloy tubes of the SINQ target and the aggregation of hydrogen at specific sites in used fuel pins of power plants and their cladding, respectively. These results continue to help understanding material degradation and optimizing the operational regimes, which might lead to extending the safe lifetimes of these components.

Towards spatially resolved magnetic small-angle scattering studies by polarized and polarization-analyzed neutron dark-field contrast imaging.

In the past decade neutron dark-field contrast imaging has developed from a qualitative tool depicting microstructural inhomogeneities in bulk samples on a macroscopic scale of tens to hundreds of micrometers to a quantitative spatial resolved small-angle scattering instrument. While the direct macroscopic image resolution around tens of micrometers remains untouched microscopic structures have become assessable quantitatively from the nanometer to the micrometer range. Although it was found that magnetic structures provide remarkable contrast we could only recently introduce polarized neutron grating interferometric imaging. Here we present a polarized and polarization analyzed dark-field contrast method for spatially resolved small-angle scattering studies of magnetic microstructures. It is demonstrated how a polarization analyzer added to a polarized neutron grating interferometer does not disturb the interferometric measurements but allows to separate and measure spin-flip and non-spin-flip small-angle scattering and thus also the potential for a distinction of nuclear and different magnetic contributions in the analyzed small-angle scattering.

The Neutron Imaging Instrument CONRAD-Post-Operational Review.

The neutron imaging instrument CONRAD was operated as a part of the user program of the research reactor BER-II at Helmholtz-Zentrum Berlin (HZB) from 2005 to 2020. The instrument was designed to use the neutron flux from the cold source of the reactor, transported by a curved neutron guide. The pure cold neutron spectrum provided a great advantage in the use of different neutron optical components such as focusing lenses and guides, solid-state polarizers, monochromators and phase gratings. The flexible setup of the instrument allowed for implementation of new methods including wavelength-selective, dark-field, phase-contrast and imaging with polarized neutrons. In summary, these developments helped to attract a large number of scientists and industrial customers, who were introduced to neutron imaging and subsequently contributed to the expansion of the neutron imaging community.

A parametric neutron Bragg edge imaging study of additively manufactured samples treated by laser shock peening.

Laser powder bed fusion is an additive manufacturing technique extensively used for the production of metallic components. Despite this process has reached a status at which parts are produced with mechanical properties comparable to those from conventional production, it is still prone to introduce detrimental tensile residual stresses towards the surfaces along the building direction, implying negative consequences on fatigue life and resistance to crack formations. Laser shock peening (LSP) is a promising method adopted to compensate tensile residual stresses and to introduce beneficial compressive residual stress on the treated surfaces. Using neutron Bragg edge imaging, we perform a parametric study of LSP applied to 316L steel samples produced by laser powder bed fusion additive manufacturing. We include in the study the novel 3D-LSP technique, where samples are LSP treated also during the building process, at intermediate build layers. The LSP energy and spot overlap were set to either 1.0 or 1.5 J and 40[Formula: see text] or 80[Formula: see text] respectively. The results support the use of 3D-LSP treatment with the higher LSP laser energy and overlap applied, which showed a relative increase of surface compressive residual stress (CRS) and CRS depth by 54[Formula: see text] and 104[Formula: see text] respectively, compared to the conventional LSP treatment.

Highly Concentrated, Zwitterionic Ligand-Capped Mn2+:CsPb(Br x Cl1-x )3 Nanocrystals as Bright Scintillators for Fast Neutron Imaging.

Fast neutron imaging is a nondestructive technique for large-scale objects such as nuclear fuel rods. However, present detectors are based on conventional phosphors (typically microcrystalline ZnS:Cu) that have intrinsic drawbacks, including light scattering, γ-ray sensitivity, and afterglow. Fast neutron imaging with colloidal nanocrystals (NCs) was demonstrated to eliminate light scattering. While lead halide perovskite (LHP) FAPbBr3 NCs emitting brightly showed poor spatial resolution due to reabsorption, the Mn2+-doped CsPb(BrCl)3 NCs with oleyl ligands had higher resolution because of large apparent Stokes shift but insufficient concentration for high light yield. In this work, we demonstrate a NC scintillator that features simultaneously high quantum yields, high concentrations, and a large apparent Stokes shift. In particular, we use long-chain zwitterionic ligand capping in the synthesis of Mn2+-doped CsPb(BrCl)3 NCs that allows for attaining very high concentrations (>100 mg/mL) of colloids. The emissive behavior of these ASC18-capped NCs was carefully controlled by compositional tuning that permitted us to select for high quantum yields (>50%) coinciding with Mn-dominated emission for minimal self-absorption. These tailored Mn2+:CsPb(BrCl)3 NCs demonstrated over 8 times brighter light yield than their oleyl-capped variants under fast neutron irradiation, which is competitive with that of near-unity FAPbBr3 NCs, while essentially eliminating self-absorption. Because of their rare combination of concentrations above 100 mg/mL and high quantum yields, along with minimal self-absorption for good spatial resolution, Mn2+:CsPb(BrCl)3 NCs have the potential to displace ZnS:Cu as the leading scintillator for fast neutron imaging.

Luminescent Lead Halide Ionic Liquids for High-Spatial-Resolution Fast Neutron Imaging.

The fast neutron imaging technique with recoil proton detection harbors significant potential for imaging of thick, large-scale objects containing high-Z elements. However, the challenge to find efficient fast neutron scintillators with high spatial resolution is ongoing. The list of requirements for such scintillators is long and demanding: a proton-rich, scattering-free material combining high light yield with the absence of light reabsorption. To meet these challenges, we look for a suitable material among a rising class of 0D organic-inorganic Pb(II) halide hybrids. The use of large organic cations, e.g., trihexyltetradecylphosphonium, results in room-temperature ionic liquids that combine highly Stokes-shifted (up to 1.7 eV), reabsorption-free, and efficient emission (photoluminescence quantum yield up to 60%) from molecularly small and dense (PbX2 molar fraction up to 0.33) emitting centers. We investigate the optical properties of the resulting ionic liquids and showcase their utility as fast neutron imaging scintillators. Concomitantly with good light yield, such fast-neutron scintillators exhibit both higher spatial resolution and lower γ-ray sensitivity compared with commercial ZnS:Cu-based screens.

Milk gelation studied with small angle neutron scattering techniques and Monte Carlo simulations.

The sol-gel transition of fat-free milk by acidification was studied with neutron scattering experiments and Monte Carlo simulations. Spin-echo small angle neutron scattering (SESANS) and ultrasmall angle neutron scattering (USANS) experiments were performed to measure the static structure of milk and yogurt, as well as the aggregation kinetics. Colloidal gelation was simulated from a reaction limited domain (RLCA) to the diffusion limited regime (DLCA) as cluster-cluster aggregation of adhesive, hard spheres on a three-dimensional lattice. Comparisons were drawn between experimental and numerical correlation functions. Milk was modeled as a suspension of casein micelles in water, and its structure was described with a dilute system of solid spheres with a log-normal distribution of sizes. The structure and formation of yogurt were described with a self-affine model, used for systems containing heterogeneities with a wide range of sizes. Simulation speed was increased by 1 order-of-magnitude using a new algorithm to eliminate dead time. Observations by SESANS and USANS of milk particle sizes and yogurt length scales were consistent and agreed well with literature. Kinetic USANS data yielded reliable information about the growth of typical length scale during aggregation. The simulation model predicted the measurement data qualitatively best staying close to the RLCA regime until large structures had formed. Correlation lengths were in good quantitative agreement, but longest simulated length scales were a of factor 2(1)/(2) below experimental findings. We conclude that small, mobile aggregates are formed during the first 3 h, mostly influencing the dimensionality of the system and that large, inert structures are formed from 2 up to 8 h, which determine the typical length scale.

Frame overlap Bragg edge imaging.

Neutron Bragg edge imaging enables spatially resolved studies of crystalline features through the exploitation and analysis of Bragg edges in the transmission spectra recorded in each pixel of an imaging detector. Studies with high spectral resolutions, as is required e.g. for high-resolution strain mapping, and with large wavelength ranges have been largely reserved to pulsed neutron sources. This is due to the fact, that the efficiency for high wavelength resolution measurements is significantly higher at short pulse sources. At continuous sources a large fraction of the available neutrons must be sacrificed in order to achieve high wavelength resolution for a relevant bandwidth e.g. through a chopper system. Here we introduce a pulse overlap transmission imaging technique, which is suited to increase the available flux of high wavelength resolution time-of-flight neutron Bragg edge imaging at continuous neutron sources about an order of magnitude. Proof-of-principle measurements utilizing a chopper with a fourfold repeated random slit distribution of eight slits were performed at a thermal neutron beamline. It is demonstrated, that disentanglement of the overlapping pulses is achieved with the correlation theorem for signal processing. Thus, the Bragg edge pattern can be reconstructed from the strongly overlapping Bragg edge spectra recorded and the results demonstrate the feasibility of the technique.

Neutron Diffraction and Diffraction Contrast Imaging for Mapping the TRIP Effect under Load Path Change.

The transformation induced plasticity (TRIP) effect is investigated during a load path change using a cruciform sample. The transformation properties are followed by in-situ neutron diffraction derived from the central area of the cruciform sample. Additionally, the spatial distribution of the TRIP effect triggered by stress concentrations is visualized using neutron Bragg edge imaging including, e.g., weak positions of the cruciform geometry. The results demonstrate that neutron diffraction contrast imaging offers the possibility to capture the TRIP effect in objects with complex geometries under complex stress states.