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With the increasing importance of light-responsive materials, it is vital to analyze the relationship between function and structural changes induced by light irradiation. Small-angle scattering (SAS) is effective for such structural analysis. However, quantitatively capturing local molecular structure formation and molecular reactions at a scale of less than 1 nm via SAS is difficult. In this study, to analyze the structure of non-equilibrium phenomena in light-responsive materials, a new sample environment has been developed for a time-of-flight small- and wide-angle neutron scattering instrument (TAIKAN), comprising a UV–Vis irradiation system, UV–Vis absorption measurement equipment and photodetector. Simultaneous measurement of small-angle neutron scattering and UV–Vis absorption was achieved. This system was used to demonstrate the in situ observation of UV–Vis irradiation-induced structural change of micelles formed by 4-butylazobenzene-4′-(oxyethyl)trimethylammonium bromide, which is a light-responsive surfactant, in an aqueous solution. The results showed that the present measuring system provides direct information on the interplay between changes in micelle structure and changes in molecular configuration.

Neutron polarization analysis (NPA) for small-angle neutron scattering (SANS) experiments using a pulsed neutron source was successfully achieved by applying a 3He spin filter as a spin analyzer for the neutrons scattered from the sample. The cell of the 3He spin filter gives a weak small-angle scattering intensity (background) and covers a sufficient solid angle for performing SANS experiments. The relaxation time of the 3He polarization is sufficient for continuous use for approximately 2 days, thus reaching the typical duration required for a complete set of SANS experiments. Although accurate evaluation of the incoherent neutron scattering, which is predominantly attributable to the extremely large incoherent scattering cross section of hydrogen atoms in samples, is difficult using calculations based on the sample elemental composition, the developed NPA approach with consideration of the influence of multiple neutron scattering enabled reliable decomposition of the SANS intensity distribution into the coherent and incoherent scattering components. To date, NPA has not been well established as a standard technique for SANS experiments at pulsed neutron sources such as the Japan Proton Accelerator Research Complex (J-PARC) and the US Spallation Neutron Source. It is anticipated that this work will contribute significantly to the accurate determination of the coherent neutron scattering component for scatterers in various types of organic sample systems in SANS experiments at J-PARC, particularly for systems involving competition between the coherent and incoherent scattering intensity.

This study involves the upgrade of a high-resolution position-sensitive detector (HR-PSD) installed on the small-angle neutron scattering spectrometer (SANS-U) at the Japan Atomic Energy Agency. By using both neutron lenses and the HR-PSD, the accessible low-Qlimit can be extended to the order of 10−4 Å−1[Qis the magnitude of the scattering vector defined byQ= (4π/λ)sinθ, where λ and 2θ are the wavelength and the scattering angle, respectively]. The HR-PSD consists of a cross-wired position-sensitive photomultiplier tube (PSPMT) and a commercial ZnS/6LiF scintillator. To improve the experimental efficiency of focusing small-angle neutron scattering (FSANS) experiments, a high-performance ZnS/6LiF scintillator developed at the Japan Atomic Energy Agency has been utilized. For the PSPMT and data-acquisition system installed on SANS-U, the thickness of the ZnS/6LiF scintillator was optimized by measuring the thickness dependence of the pulse-height spectra. Under the experimental conditions of SANS-U, the optimum thickness of the ZnS/6LiF scintillator (ZnS:6LiF = 2:1) was determined to be 0.433 mm by measuring the total counts and peak positions of the pulse-height spectra. Installation of the optimized ZnS/6LiF scintillator improved detection efficiency by 1.39 times over that of a commercial scintillator at the same level of background counts andQresolution in FSANS experiments.

The small-angle neutron scattering spectrometer SANS-U at the research reactor (JRR-3) of the Japan Atomic Energy Agency, Tokai, Japan, has been successfully upgraded. This major upgrade was undertaken in order to install a high-resolution position-sensitive detector consisting of a cross-wired position-sensitive photomultiplier tube combined with a ZnS/6LiF scintillator on the SANS-U spectrometer. Without changing the total length of the spectrometer, the aim was to extend the accessible low-Qlimit (Qis the magnitude of the scattering vector) and to shorten the measurement time by employing focusing small-angle neutron scattering (FSANS). By using both spherical MgF2biconcave lenses and the new high-resolution position-sensitive detector, the accessible low-Qlimit was extended from 2.5 × 10−3to 3.8 × 10−4 Å−1. As a result, SANS-U can continuously cover a wideQrange from 3.8 × 10−4to 0.35 Å−1with a wavelength of 7 Å. FSANS can be utilized not only to improve the accessible low-Qlimit but also to increase the intensity of incident neutrons passing through the sample in the conventionalQrange from 2.5 × 10−3to 0.35 Å−1. The use of `high-intensity' FSANS also allowed a reduction of the measuring time by approximately 1/3.16 by increasing the incident neutron intensity.

Aspherical neutron lenses are discussed in detail as focusing elements for existing small-angle neutron scattering (SANS) diffractometers. The conceptual design can be obtained by analytical equations, while computer simulations provide the intensity distribution of the primary beam, which is strongly correlated with the instrumental resolution and the minimal momentum transferQ. For large illuminated sample/lens areas of 50 mm diameter the aspherical lens design is essential, while spherical lenses are limited toca20 mm diameter with a 60% spherical aberration for standard SANS experiments. Scattering experiments on different samples proved the applicability and revealed the resolution limits of the two lens types. From theoretical considerations it is proposed that lens cooling can be used to reduce the thermal diffuse scattering.

SANS-J (a pinhole small-angle neutron scattering spectrometer at research reactor JRR3, Tokai, Japan) was reconstructed as a focusing and polarized neutron small-angle scattering spectrometer (SANS-J-II). By employing focusing lenses of a biconcave MgF2 crystal or of a sextupole permanent magnet and a high-resolution photomultiplier, the minimum accessible magnitude of the scattering vector qmin was improved from 3 × 10−3 A−1 to an ultra-small-angle scattering (USAS) of 3 × 10−4 A−1. Compared with a Bonse–Hart double-crystal method, the advantages of focusing USAS are the efficient detection of anisotropic USAS with an area detector, an improvement in q resolution Δq/q at conventional magnitudes of the scattering vector q ~ 10−3 A−1 and a gain in neutron flux in the conventional q region of q ~ 10−3 A−1.

In order to extend an upper q-limit [q is the magnitude of the scattering vector q, defined by q = (4π/λ)sinθ, where λ and 2θ are the wavelength and the scattering angle, respectively], high-angle 3He sub-detectors were installed on a focusing and polarized neutron small-angle scattering spectrometer (SANS-J-II) at JRR-3, Tokai, Japan. Consequently, the upper q-limit was improved from 0.2 to 2.0 A−1. To quantitatively discriminate spin incoherent scattering from hydrogen or to perform nuclear spin polarization contrast variation, a remanent supermirror analyser is also available on the high-angle sub-detector. By combining a focusing ultra-small-angle scattering, realised by compound and/or magnetic lens and high-resolution area detector, SANS-J-II is able to cover from 3 × 10−4 to 2.0 A−1 (four orders of magnitude of q), which benefits investigation of hierarchically ordered systems, found widely in hard, soft and bio-materials.

We have constructed a focusing-geometry small-angle neutron scattering (FSANS) instrument, SANS-J-II, with two kinds of neutron focusing device: a series of compound refractive lenses made of MgF2 and a magnetic neutron lens based on an extended Halbach-type sextupole magnet. In this study, we investigated the performance of the FSANS instrument with the magnetic neutron lens. The intensity distribution of a direct neutron beam focused on the detector plane by the magnetic neutron lens had a ratio of the peak height to the background level of \sim\!6\times 10^4 for a polarized neutron beam with a polarization degree of \sim \!0.99. It is found that a minimum value of the measurable q range [where q is the modulus of the scattering vector and is defined as q = (4\pi/\lambda)\sin(\theta/2), where \theta is the scattering angle and \lambda is the neutron wavelength], q_{\rm min}, of 6.5 \times 10^{-4} A−1 can be achieved by the FSANS instrument with the magnetic neutron lens using neutrons with \lambda = 6.6 A and \Delta \lambda/\lambda = 0.13 for the full width at half maximum.