Development of Neutron Interferometer Using Multilayer Mirrors and Measurements of Neutron-Nuclear Scattering Length with Pulsed Neutron Source.

This study entailed the successful deployment of a novel neutron interferometer that utilizes multilayer mirrors. The apparatus facilitates a precise evaluation of the wavelength dependence of interference fringes utilizing a pulsed neutron source. Our interferometer achieved an impressive precision of 0.02 rad within a 20-min recording time. Compared to systems using silicon crystals, the measurement sensitivity was maintained even when using a simplified disturbance suppressor. By segregating beam paths entirely, we achieved successful measurements of neutron-nuclear scattering lengths across various samples. The values measured for Si, Al, and Ti were in agreement with those found in the literature, while V showed a disparity of 45%. This discrepancy may be attributable to impurities encountered in previous investigations. The accuracy of measurements can be enhanced further by mitigating systematic uncertainties that are associated with neutron wavelength, sample impurity, and thickness. This novel neutron interferometer enables us to measure fundamental parameters, such as the neutron-nuclear scattering length of materials, with a precision that surpasses that of conventional interferometers.

Neutron phase imaging by a Talbot-Lau interferometer at Kyoto University Reactor.

We have developed a new neutron phase imaging system with a Talbot-Lau interferometer for utilization at the CN-3 port of the Kyoto University Reactor. To achieve efficient differential-phase imaging and visibility (dark-field) imaging at this beamline, we adopted a relatively shorter design wavelength of 2.7 Å. By fabricating neutron absorption gratings with thick gadolinium absorbers, we were able to obtain clear moiré fringes with a high visibility of 55% for thermal neutrons. As a demonstration of its imaging capabilities for expanded actual utilization in the medium-sized sources, we observed additively manufactured rods of Inconel 718. Using visibility imaging, we successfully examined variations in the size of defects in the rods caused by hot isostatic pressing process. In addition, we conducted tomography measurements of the rods, which allowed us to reveal the spatial distribution of defects at sub-micrometer scales.

Neutron reflectometry under high shear in narrow gap for tribology study.

An operando analysis method has been established for evaluating the interfacial structure of an adsorbed layer formed by an additive on a metal surface under fluid lubricated conditions. A parallel-face narrow gap viscometer installed in an energy-resolved neutron reflectometer is used to evaluate the change in the interfacial structure under high shear. The viscometer was designed to operate at a high shear rate while maintaining a µm-order constant gap between two parallel surfaces. When an additive-free base oil was sandwiched in the gap, the neutron reflectivity profiles without and with upper surface rotation were the same. This demonstrates that the reflectivity profiles can be accurately measured regardless of whether the upper surface is rotated. When a base oil containing a polymethacrylate-based additive was sandwiched in the gap, both the thickness and density of the adsorbed additive layer in the rotation (shear field) condition were lower than those in the non-rotation (static) condition. This demonstrates that the proposed method can be used to analyse the structural changes in the adsorbed layer formed by an oil additive on a surface. This combination of a neutron reflectometer and narrow gap viscometer is a promising approach to near-future tribological studies.

Neutron flat-panel detector using In-Ga-Zn-O thin-film transistor.

Neutron imaging is a powerful tool for observing the internal structure of an object without destroying the object. Neutron imaging (neutron radiography) is a prominent application of neutrons but still requires significant improvements, for example, in sensitivity, resolution, radiation hardness, and handling of neutron imaging detectors. This paper presents the development and the first neutron imaging results of a neutron flat-panel detector (nFPD) based on an In-Ga-Zn-O (IGZO) thin-film transistor (TFT)/photodiode array coupled with a LiF/ZnS scintillator sheet. Direct photo-coupling to the scintillator increases the light collection efficiency. Moreover, unlike lens-coupled neutron cameras, the proposed detector is compact and easy to handle. Owing to the high off-state resistance of IGZO TFTs, their leakage current is lower than that of conventional TFTs, enabling the IGZO TFTs to hold an accumulated charge for a longer period of time and allowing longer exposure times for imaging. This would be a powerful feature for imaging at compact neutron sources with limited flux. This paper reports on the first neutron imaging results with an IGZO nFPD, its performance evaluation, and a demonstration of three-dimensional computed tomography with neutrons.

Neutron reflectometry-based in situ structural analysis of an aligning agent additive for the alignment of nematic liquid crystals on solid substrates.

Surface aligning agents, such as amphiphilic surfactants, are widely used to control the initial alignment of nematic liquid crystals (NLCs) in liquid crystal displays (LCDs). Generally, these agents are first coated on a substrate prior to NLC introduction. When mixed with NLCs, long alkyl chain amphiphilic agent additives may control the NLC alignment without requiring pretreatment because they may spontaneously form an adsorbed layer at the solid-NLC interface. These self-assembled layers (SALs) appear promising in the effective control of the initial alignment of LCDs. However, direct observation of the adsorbed layer structure in contact with the NLCs is challenging due to probe limitations. Furthermore, the areal densities and alignments of the amphiphiles adsorbed from NLCs at the solid-NLC interface are not previously reported. Herein, the structure of the surface aligning agent n-hexadecyltrimethylammonium-d42 bromide (d-CTAB) was investigated at the silicon-NLC interface using in situ neutron reflectometry (NR), which indicated that the CTAB self-assembled as a monolayer, with its alignment dependent on the amphiphile concentration. At low amphiphile concentrations, the alignment of the SAL and NLCs was parallel to the substrate. With increasing amphiphile concentration, the number of amphiphiles attached to the substrate increased within the framework of the Gibbs monolayer, with the alignment of the amphiphiles and NLCs becoming perpendicular to the substrate. The experimental setup used here is comparable to those of more natural systems, such as those found in the alignment of NLCs in LCDs.

Neutron Imaging Using a Fine-Grained Nuclear Emulsion.

A neutron detector using a fine-grained nuclear emulsion has a sub-micron spatial resolution and thus has potential to be applied as high-resolution neutron imaging. In this paper, we present two approaches to applying the emulsion detectors for neutron imaging. One is using a track analysis to derive the reaction points for high resolution. From an image obtained with a 9 µm pitch Gd grating with cold neutrons, periodic peak with a standard deviation of 1.3 µm was observed. The other is an approach without a track analysis for high-density irradiation. An internal structure of a crystal oscillator chip, with a scale of approximately 30 µm, was able to be observed after an image analysis.

Application of precise neutron focusing mirrors for neutron reflectometry: latest results and future prospects.

Neutron reflectometry (NR) is a powerful tool for providing insight into the evolution of interfacial structures, for example via operando measurements for electrode-electrolyte interfaces, with a spatial resolution of nanometres. The time resolution of NR, which ranges from seconds to minutes depending on the reflection intensity, unfortunately remains low, particularly for small samples made of state-of-the-art materials even with the latest neutron reflectometers. To overcome this problem, a large-area focusing supermirror manufactured with ultra-precision machining has been employed to enhance the neutron flux at the sample, and a gain of approximately 100% in the neutron flux was achieved. Using this mirror, a reflectivity measurement was performed on a thin cathode film on an SrTiO3 substrate in contact with an electrolyte with a small area of 15 × 15 mm. The reflectivity data obtained with the focusing mirror were consistent with those without the mirror, but the acquisition time was shortened to half that of the original, which is an important milestone for rapid measurements with a limited reciprocal space. Furthermore, a method for further upgrades that will reveal the structural evolution with a wide reciprocal space is proposed, by applying this mirror for multi-incident-angle neutron reflectometry.

MONOPOL - A traveling-wave magnetic neutron spin resonator for tailoring polarized neutron beams.

We report on first experimental tests of a neutron magnetic spin resonator at a very cold neutron beam port of the high flux reactor at the ILL Grenoble. When placed between two supermirror neutron polarizers and operated in a pulsed traveling-wave mode it allows to decouple its time- and wavelength-resolution and can therefore be used simultaneously as electronically tunable monochromator and fast beam chopper. As a first 'real' scientific application we intend its implementation in the PERC (p roton and e lectron r adiation c hannel) project related to high-precision experiments in neutron beta decay.

Elliptic neutron-focusing supermirror for illuminating small samples in neutron reflectometry.

This paper details the development of a precise assembly of two supermirrors for neutron-focusing, designed for installation in neutron reflectometer SOFIA at BL16 in J-PARC MLF to intensify the illumination for small samples. The supermirrors are sputtered on two metal substrates, whose surfaces are coated with amorphous Ni-P plating, and are figured by diamond cutting and polished to subnanometer roughness. Special care is taken while polishing the substrates to reduce waviness and surface roughness for achieving a sharp focusing spot and uniform neutron reflectivity. The supermirror could converge the neutrons into a focal spot with a width of 0.13 mm in the full width at half maximum.

Development of precision elliptic neutron-focusing supermirror.

This paper details methods for the precision design and fabrication of neutron-focusing supermirrors, based on electroless nickel plating. We fabricated an elliptic mirror for neutron reflectometry, which is our second mirror improved from the first. The mirror is a 550-millimeter-long segmented mirror assembled using kinematic couplings, with each segment figured by diamond cutting, polished using colloidal silica, and supermirror coated through ion-beam sputtering. The mirror was evaluated with neutron beams, and the reflectivity was found to be 68-90% at a critical angle. The focusing width was 0.17 mm at the full width at half maximum.

Development of a large plano-elliptical neutron-focusing supermirror with metallic substrates.

Results of this study demonstrated that electroless nickel-phosphorus (NiP) plated metal substrate is an excellent material for producing large aspherical neutron-focusing supermirrors. A large plano-elliptical neutron-focusing supermirror comprising two metallic segments was fabricated using single-point diamond cutting, precision polishing and supermirror coating. The average surface roughness of the metallic substrates was approximately 0.3 nm rms. For evaluation, the focusing supermirror was installed at the SOFIA neutron reflectometer, showing high neutron reflectivity and giving minimal beam width of 0.34 mm in FWHM. Because of the large beam divergence accepted by the mirror, the count rate with the focusing mirror was 3.3 times higher than that obtained using conventional two-slit collimation.

Figure correction of a metallic ellipsoidal neutron focusing mirror.

An increasing number of neutron focusing mirrors is being adopted in neutron scattering experiments in order to provide high fluxes at sample positions, reduce measurement time, and/or increase statistical reliability. To realize a small focusing spot and high beam intensity, mirrors with both high form accuracy and low surface roughness are required. To achieve this, we propose a new figure correction technique to fabricate a two-dimensional neutron focusing mirror made with electroless nickel-phosphorus (NiP) by effectively combining ultraprecision shaper cutting and fine polishing. An arc envelope shaper cutting method is introduced to generate high form accuracy, while a fine polishing method, in which the material is removed effectively without losing profile accuracy, is developed to reduce the surface roughness of the mirror. High form accuracy in the minor-axis and the major-axis is obtained through tool profile error compensation and corrective polishing, respectively, and low surface roughness is acquired under a low polishing load. As a result, an ellipsoidal neutron focusing mirror is successfully fabricated with high form accuracy of 0.5 µm peak-to-valley and low surface roughness of 0.2 nm root-mean-square.

New fabrication method for an ellipsoidal neutron focusing mirror with a metal substrate.

We propose an ellipsoidal neutron focusing mirror using a metal substrate made with electroless nickel-phosphorus (NiP) plated material for the first time. Electroless NiP has great advantages for realizing an ellipsoidal neutron mirror because of its amorphous structure, good machinability and relatively large critical angle of total reflection for neutrons. We manufactured the mirror by combining ultrahigh precision cutting and fine polishing to generate high form accuracy and low surface roughness. The form accuracy of the mirror was estimated to be 5.3 µm P-V and 0.8 µm P-V for the minor-axis and major-axis direction respectively, while the surface roughness was reduced to 0.2 nm rms. The effect of form error on focusing spot size was evaluated by using a laser beam and the focusing performance of the mirror was verified by neutron experiments.

Distribution of glass transition temperature in multilayered poly(methyl methacrylate) thin film supported on a Si substrate as studied by neutron reflectivity.

We studied the distribution of glass transition temperature (Tg) through neutron reflectivity in a poly(methyl methacrylate) (PMMA) thin film supported on a silicon substrate with a five-layered PMMA thin film consisting of deuterated-PMMA and hydrogenated-PMMA. The depth distribution of Tg was successfully observed in the PMMA thin film. Compared to the previously reported distribution of Tg in a polystyrene thin film, the presence of a long-range interfacial effect, supposedly caused by an interaction between PMMA and the substrate, is considered to be responsible for the differences in both the distribution of Tg and the thickness dependence of Tg in both polymers. Therefore, it is expected that the thickness dependence of Tg reported for single-layered polymer thin films can, in principle, be understood from the viewpoint of the difference in the depth distribution of Tg.

Distributions of glass-transition temperature and thermal expansivity in multilayered polystyrene thin films studied by neutron reflectivity.

We performed neutron reflectivity measurements on multilayered polymer thin films consisting of alternatively stacked deuterated polystyrene (d-PS) and hydrogenated polystyrene (h-PS) layers ∼200 Å thick as a function of temperature covering the glass-transition temperature T(g), and we found a wide distribution of T(g) as well as a distribution of the thermal expansivity α within the thin films, implying the dynamic heterogeneity of the thin films along the depth direction. The reported anomalous film thickness dependences of T(g) and α were reasonably understood in terms of the distributions, showing that the surface mobile layer and the bottom hard interfacial layer are, respectively, responsible for the depressions of T(g) and α with decreasing film thickness. The molecular mobility in each layer is also discussed in relation to the distribution of T(g), based on the results on mutual diffusion at the layer interface.

Interfacial width in polymer bilayer films prepared by double-spin-coating and flotation methods.

A spin-coating method with the aid of selective solvents has been used to construct multilayer structures for organic devices under the assumption that the solvents do not invade a preformed structure. To confirm the assumption, we examined the interfacial width (lambda(i)) of model polymer bilayers, composed of polystyrene and perdeuterated poly(methyl methacrylate), prepared by spin-coating and flotation methods. Neutron reflectivity measurements revealed that the lambda(i) value was larger for the spin-coating method than for the flotation method. These results cast doubt on the validity of the assumption. This knowledge should be kept in mind when this method is applied to construct multilayer structures.

Control of dispersion state of silsesquioxane nanofillers for stabilization of polystyrene thin films.

The influence of the dispersion states of the nanofillers on the dewetting behavior of the polymer thin film was investigated. Polyhedral oligomeric silsesquioxanes (POSS) with various substituents were added into polystyrene (PS) thin films as the nanofillers. The dewetting rate of the films drastically changed with the surface substituents of POSS additives. Neutron reflectivity measurements indicated that the difference of the dewetting rate was associated with the dispersion state of POSS additives in the films. POSS with phenethyl groups (PhPOSS), which homogeneously dispersed into the films, resulted in the decrease of the glass transition temperature of PS and the enhancement of the dewetting of the films. POSS with a fluoroalkyl group (CpPOSS-R f) segregated to the film surface and showed the retardation of the dewetting by the decrease of the surface energy of the film. POSS with hydroxyl groups (CpPOSS-2OH) segregated to the film surface and film-substrate interface and led to the elimination of the dewetting, suggesting the importance of the interfacial segregation for the inhibition of dewetting. These results revealed the strong relationship between the dispersion state of the nanofillers and the dewetting of the nanofilled films.

Nonsolvents cause swelling at the interface with poly(methyl methacrylate) films.

Density profiles of a perdeuterated poly(methyl methacrylate) (dPMMA) film spin-coated on a substrate in water, hexane, and methanol, which are "nonsolvents" for dPMMA, were examined along the direction normal to the interface by specular neutron reflectivity (NR). The interfaces of dPMMA with the liquids were diffuse in comparison with the pristine interface with air; the interfacial width with water was thicker than that with hexane. Interestingly, in water, the dPMMA film was composed of a swollen layer and the interior region, which also contained water, in addition to the diffused layer. The interface of dPMMA with hexane was sharper than that with water. Although there were slight indications of a swollen layer for the dPMMA in hexane, the solvent molecules did not penetrate significantly into the film. On the other hand, in methanol, the whole region of the dPMMA film was strikingly swollen. To conserve mass, the swelling of the film by the nonsolvents is accompanied by an increase in the film thickness. The change in the film thickness estimated by NR was in excellent accord with the results of direct observations using atomic force microscopy (AFM). The modulus of dPMMA in the vicinity of the interfaces with liquids was also examined on the basis of force-distance curves measured by AFM. The modulus decreased closer to the outermost region of the film. The extent to which the modulus decreased in the interfacial region was consistent with the amount of liquid sorbed into the film.