The dynamic magnetic pair-density function (DymPDF) D_ M(r, E) is obtained via the Fourier transform of the dynamic magnetic structure factor, S_ M(Q, E), which is measured using nonpolarized inelastic neutron scattering. While there is a long history of magnetic excitation studies with S_ M(Q, E), there are no reports on D_ M(r, E). In this study, we examine simple magnet models and representative magnet examples, such as FeTiO_3 and YBa_2Cu_3O_6, to investigate the real-space dynamics of D_ M(r, E). We derive the D_ M(r, E) equations for simple magnet models in a low energy limit. By comparing these equations to the simulations, we demonstrate the characteristic energy dependence of real-space local magnon modes, including the transition of the magnon mode from acoustic to optical. Our novel analysis reveals the local magnon modes accompanied by a sign change in each spin-pair correlation at a given energy in nanoscale real space even under non-periodic conditions. This method is unique for studying local magnetic dynamics.

We present a combined experimental and theoretical investigation of the spin dynamics in the iron-based superconductor Ba0.75K0.25Fe2As2. Time-of-flight inelastic neutron scattering measurements reveal the threedimensional (3D) nature of the spin fluctuations, manifested as out-of-plane modulations of the low-energy magnetic intensity. As the energy increases, this 3D-like modulation gradually fades away, leading to a more two-dimensional (2D) profile-a clear signature of a 3D-to-2D crossover in the spin dynamics. By incorporating a realistic 3D electronic band structure derived from density functional theory (DFT), we reproduce the experimentally observed features of the spin susceptibility, including the pronounced out-of-plane modulation at low energies and its gradual evolution into a more 2D character at higher energies. The calculated susceptibility exhibits a peak at the experimental ordering wave vector qAFM= (0.5, 0.5, 1), demonstrating that the DFT-derived 3D model accurately captures the tendency toward out-of-plane antiferromagnetic (AFM) order. Notably, electronic states away from the Fermi level play a crucial role in shaping the susceptibility peak at qAFM, highlighting the limitations of the Fermi surface nesting picture in explaining the out-of-plane AFM instability. The demonstrated agreement between experiment and theory serves as a benchmark for validating the DFT-derived model as a realistic description of the material-specific electronic structure.

We are developing magnetic scattering neutron holography (MNH) using polarized neutrons to visualize elementspecific local magnetic structures in magnetic alloys. In the present study, neutrons were polarized with a 3He spin filter, and the room-temperature ferromagnetic alloy Fe0.08Co0.92 was used for the sample. From the spin dependence of the 200 Bragg reflection, the neutron polarization at the sample, Pn, was evaluated to be approximately 33%, confirming that polarization was preserved from the spin filter to the sample position. MNH measurements were performed twice with opposite neutron spin directions, and the resulting holograms exhibited differences depending on the incident neutron spin. This indicates a preliminary demonstration of the acquisition of holograms including the spin-dependent magnetic scattering term Pn chi M(k). Based on these results, the present study demonstrates the feasibility of observing local magnetic structures with MNH and discusses future improvements to this technique.

We present proof-of-principle experiments of stroboscopic time-of-flight (TOF) neutron diffraction in long pulsed magnetic fields. By utilizing electric double-layer capacitors, we developed a long pulsed magnet for neutron diffraction measurements, which generates pulsed magnetic fields with the full widths at the half maximum of more than $10^2$ ms. The field variation is slow enough to be approximated as a steady field within the time scale of a polychromatic neutron pulse passing through a sample placed in a distance of the order of $10^1$ m from the neutron source. This enables us to efficiently explore the reciprocal space using a wide range of neutron wavelength in high magnetic fields. We applied this technique to investigate field-induced magnetic phases in the triangular lattice antiferromagnets CuFe$_{1-x}$Ga$_x$O$_2$ ($x=0, 0.035$).

The perovskite ferroelectric BaTiO3 has a high dielectric constant, and its ionic polarization has been studied in various ways. Atomic resolution holography is a method to obtain atomic arrangements around specific elements. It is also sensitive to atomic displacement, making it useful for evaluating the polarization at the atomic scale. In particular, neutron holography can be used to observe light elements such as O atoms, which are difficult to observe with X-rays. Thus, the displacement of anions and cations can be discussed using neutron holography. In this study, neutron holography experiments were performed on BaTiO3. We succeeded in observing clear oxygen atomic images around Ti. Based on the calculation of the image intensity as a function of atomic displacement, the displacement of the O atom relative to the Ti atom was 0.23 & Aring; estimated from the observed image intensity of the O atom. Considering the atomic displacement parameter, the difference between the positions of Ti and O atoms in the polarization direction was estimated to be 0.16 & Aring;. This study demonstrates that the observation of the oxygen atoms in BaTiO3 by neutron holography allowed us to evaluate the magnitude of the ionic polarization.

We have developed instruments for magnetic neutron holography (MNH) using polarized white neutrons to investigate the local magnetic structures of magnetic alloys. We chose the 3He spin filter method as the neutron polarizer to polarize neutrons over a wide wavelength range of up to a few 100 meV. We developed a magnet device to saturate the magnetizations of ferromagnetic samples, and instruments to transport polarized neutrons from a 3He spin filter to the MNH sample. The neutron polarization, , at the beginning of the MNH experiments was confirmed to be 0.46, which is feasible for MNH. Using the developed instruments, we obtained preliminary results for the room-temperature ferromagnetic alloy Fe0.08Co0.92. Technical problems encountered in the experiments and ways to overcome them are discussed. Based on these results, we believe that MNH that use polarized neutrons is promising.

We investigated neutron flux at a sample position and energy resolution of a direct-geometry disk-chopper spectrometer AMATERAS under various chopper conditions and compared them with simulations and calculations. The measured flux was comparable to that of similar high-flux spectrometers. The resolution when using a pulse-shaping chopper correlated well with the analytical calculations, including the thickness of the disk chopper, the sample size, and the penetration depth into the detector. The results show that the chopper, placed at the intermediate distance of the primary spectrometer, functions as a pulse shaper that optimizes the flux and resolution below the incident energy of 10 meV.

Photoresponsive materials are garnering attention because of their applications toward building a sustainable society. A recently developed fast-photoresponsive amphiphilic lophine dimer (3TEG-LPD) responds rapidly to light, making it a promising candidate for drug-delivery systems. In this study, the mechanism of structural changes induced by ultraviolet (UV) irradiation in 3TEG-LPD micelles in an aqueous solution was investigated via an in situ time-resolved small-angle neutron scattering (SANS) technique. Since subsecond resolution was necessary to observe the structural changes in the 3TEG-LPD micelles, stroboscopic SANS analysis was employed to obtain scattering profiles with a time width of 0.5 s. The structural parameters were quantitatively determined by performing a model-fitting analysis of the SANS results. The stroboscopic SANS results showed that upon UV irradiation, the axial ratio and pseudo-aggregation number of the 3TEG-LPD micelles increased by 1.8 and 1.6 times, respectively, whereas the number of water molecules per surfactant molecule decreased. This finding suggested that the change in the shape of the micelles from spherical to ellipsoidal shape was accompanied by dehydration. Under the present UV irradiation conditions, this structural change of the micelle occurred rapidly during the first 30 s after the start of UV irradiation. Each structural parameter recovered exponentially and reversibly during the recovery process after the cessation of UV irradiation. The changes in these parameters were analyzed in terms of kinetics by comparing them with the changes in the molecular structure. We found that the change of the micelles proceeds approximately twice as fast as the association of the molecule. Furthermore, from the perspective of the critical packing parameter consideration, the SANS analysis revealed that the UV-induced changes in 3TEG-LPD micelles are dominated by the enthalpy contribution. This finding is expected to be useful for developing new materials for various applications.

Spin-contrast-variation (SCV) small-angle neutron scattering (SANS) is a technique to determine the nanostructure of composite materials from the scattering of polarized neutrons that changes with proton polarization of samples. The SCV-SANS enabled us to determine structure of nanoice crystals that were generated in rapidly frozen sugar solutions by separating the overlapped signals from the nanoice crystals and frozen amorphous solutions. In the frozen glucose solution, we found that the nanoice crystals formed a planar structure with a radius larger than several tens of nanometers and a thickness of 2.5 ± 0.5 nm, which was close to the critical nucleation size of ice crystals in supercooled water. This result suggests that the glucose molecules were preferentially bound to a specific face of nanoice crystals and then blocked the crystal growth perpendicular to that face.

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.

The dynamics of water and agarose molecules in an agarose aqueous solution has been studied by means of quasielastic neutron scattering (QENS). The dynamic structure factor S (Q,E) of the agarose aqueous solution was fitted well to the sum of the Lorentz and delta function. The former is attributed to the diffusive motion of water molecules and the latter to the local vibrational motion of agarose molecules. The self-diffusion coefficient D of water molecules was obtained from the Q-dependence of the width of the Lorentz function, while the mean square displacement of agarose molecules was obtained from the Q-dependence of the intensity of the delta term. In the cooling direction, both D and decreased with decreasing temperature and showed discontinuous changes around the thermal gelation temperature (around 314 K). In the heating direction, however, D and did not show the obvious change below 343 K, indicating a large hysteresis effect. The present results of and D revealed that the thermal gelation suppresses the motion of the polymer and accelerates the diffusion of water molecules. The activation energy Ea of the diffusion of water in the sol state is the same as that of bulk water, but the Ea in the gel state is clearly smaller than that of bulk water.

We investigated the diffusion dynamics of liquid benzene as a basic molecular liquid. Quasielastic neutron scattering (QENS) was utilized to elucidate the overall behavior of molecular diffusion in liquid benzene. Mode distribution analysis, which does not require specific model assumptions and can describe molecular dynamics by QENS as a distribution of Lorentz functions, revealed that the diffusion of benzene molecules is represented by three dynamic modes. The Q-dependencies of the scattering intensity and the relaxation time were analyzed using diffusion models constructed to match each dynamic mode. (1) The slowest mode is translational diffusion, described as continuous diffusion rather than jump diffusion. (2) The intermediate-speed mode is rotational diffusion, which is due to the three-dimensional reorientation of benzene molecules with a jump angle of approximately 90 degrees. (3) The fastest mode involves local fluctuations, which may originate from translational oscillations and librations of the benzene crystal. The overall picture of the diffusion dynamics and characteristics of the individual modes were clarified without using a model, which is a new approach in the field of diffusion dynamics of molecular liquids.

4SEASONS is a direct geometry time-of-flight spectrometer installed in the Materials and Life Science Experimental Facility, the Japan Proton Accelerator Research Complex. It is used to study atomic and spin dynamics in the energy range of 100 meV to 102 meV. Since more than a decade has crossed after the first inelastic scattering experiment, it is essential to consider upgrading the instrument to improve its flexibility and performance. In this paper, we discuss the possible medium-term upgrades of key components of the instrument like the chopper system, which are achievable with the current technology and at reasonable cost. Herein, we demonstrated that 4SEASONS can improve the energy resolution by a factor of two, remove frame overlap of adjacent incident energies, significantly improve the asymmetry in the pulse shape, and increase the flux by a factor of ∼1.5, without major technical difficulties.

The local structure around boron doped in 6H-type silicon carbide (SiC) was investigated using neutron holography. Three-dimensional atomic images reconstructed from multiple-wavelength holograms revealed the boron substitution for both silicon and carbon. To determine boron locations accurately, we calculated holograms with varying occupancies of six different sites and fit image intensities with those obtained from experimental holograms by the steepest descent method. As a result, it was found that boron atoms were selectively located at the Si–C-cubic site layer. Furthermore, boundaries right above the boron locations were suggested from the absence of atomic images in the upper region of reconstruction.

In many neutron scattering experiments, 3He-gas position-sensitive detectors (PSDs) are employed to obtain high-quality data. However, the exact position where a neutron is detected cannot be determined if two or more neutrons are simultaneously captured at different positions. This results in noise and degrades the quality of the data. In particular, such noise is a serious source of spurious scattering in inelastic neutron scattering instruments equipped with a large number of long PSDs recently developed at pulsed neutron sources. Herein, we introduce a pulse-width-discriminating PSD system that monitors the pulse width and height of the collected data. The system utilizes previously developed neutron-readout boards and removes instances of two or more simultaneous captures from the data to significantly improve the performance of PSDs. We also propose a new program to monitor the pulse width from PSD data using a hardware function implemented for other purposes. We confirm that the noise decreases to a level almost equal to that of the background. Although the developed program is applied to an inelastic scattering experiment, it is applicable to other types of experiments in which mispositioned signals should be eliminated as noise.

Spin excitation of an ilmenite FeTiO 3 powder sample is measured by time-of-flight inelastic neutron scattering. The dynamic magnetic pair-density function D M ( r, E ) is obtained from the dynamic magnetic structure factor S M ( Q, E ) by the Fourier transformation. The real space spin dynamics exhibit magnon mode transitions in the spin–spin correlation with increasing energy from no-phase-shift to π-phase-shift. The mode transition is well reproduced by a simulation using the reciprocal space magnon dispersions. This analysis provides a novel opportunity to study the local spin dynamics of various magnetic systems.

A data-driven bin-width optimization for the histograms of measured data sets based on inhomogeneous Poisson processes was developed in a neurophysiology study [Shimazaki & Shinomoto (2007). Neural Comput. 19, 1503-1527], and a subsequent study [Muto, Sakamoto, Matsuura, Arima & Okada (2019). J. Phys. Soc. Jpn, 88, 044002] proposed its application to inelastic neutron scattering (INS) data. In the present study, the results of the method on experimental INS time-of-flight data collected under different measurement conditions from a copper single crystal are validated. The extrapolation of the statistics on a given data set to other data sets with different total counts precisely infers the optimal bin widths on the latter. The histograms with the optimized bin widths statistically verify two fine-spectral-feature examples in the energy and momentum transfer cross sections: (i) the existence of phonon band gaps; and (ii) the number of plural phonon branches located close to each other. This indicates that the applied method helps in the efficient and rigorous observation of spectral structures important in physics and materials science like novel forms of magnetic excitation and phonon states correlated to thermal conductivities.