Search

Observation of a quantum spin liquid (QSL) state is one of the most important goals in condensed-matter physics, as well as the development of new spintronic devices that support next-generation industries. The QSL in two dimensional quantum spin systems is expected to be due to geometrical magnetic frustration, and thus a kagome-based lattice is the most probable playground for QSL. Here, we report the first experimental results of the QSL state on a square-kagome quantum antiferromagnet, KCu6AlBiO4(SO4)5Cl. Comprehensive experimental studies via magnetic susceptibility, magnetisation, heat capacity, muon spin relaxation (μSR), and inelastic neutron scattering (INS) measurements reveal the formation of a gapless QSL at very low temperatures close to the ground state. The QSL behavior cannot be explained fully by a frustrated Heisenberg model with nearest-neighbor exchange interactions, providing a theoretical challenge to unveil the nature of the QSL state., There exist many theoretical models of frustrated quantum magnetism, most of which lack convincing experimental realisations. Here the authors combine several experimental methods to argue that KCu6AlBiO4(SO4)5Cl behaves as a square-kagome-lattice quantum Heisenberg antiferromagnet.

Neutron scattering experiments have been performed to elucidate magnetic properties of the quasicrystal approximant Au

Determination of crystal system and space group in the initial stages of crystal structure analysis forms a bottleneck in material science workflow that often requires manual tuning. Herein we propose a machine-learning (ML)-based approach for crystal system and space group classification based on powder X-ray diffraction (XRD) patterns as a proof of concept using simulated patterns. Our tree-ensemble-based ML model works with nearly or over 90% accuracy for crystal system classification, except for triclinic cases, and with 88% accuracy for space group classification with five candidates. We also succeeded in quantifying empirical knowledge vaguely shared among experts, showing the possibility for data-driven discovery of unrecognised characteristics embedded in experimental data by using an interpretable ML approach.

In the present study, we show that time-consuming manual tuning of parameters in the Rietveld method, one of the most frequently used crystal structure analysis methods in materials science, can be automated by considering the entire trial-and-error process as a blackbox optimisation problem. The automation is successfully achieved using Bayesian optimisation, which outperforms both a human expert and an expert-system type automation despite the absence of expertise. This approach stabilises the analysis quality by eliminating human-origin variance and bias, and can be applied to various analysis methods in other areas which also suffer from similar tiresome and unsystematic manual tuning of extrinsic parameters and human-origin variance and bias.

Magnetic excitations in the metallic antiferromagnet F e 0.5 M n 0.5 were investigated using the inelastic neutron scattering technique at low temperatures well below the antiferromagnetic transition temperatures ( T N ). The observed peak positions in low energies well sit on the antiferromagnetic dispersion relation reported in the early study. However, the peak positions in higher energies shift to higher energies than that of the antiferromagnetic spin wave dispersion relation. This behavior is the same as one of the behaviors suggesting that the spin waves merge with the continuum of the individual particle-hole excitations at higher energies in F e 0.7 M n 0.3 .

Neutron scattering experiments have been performed to elucidate magnetic properties of the quasicrystal approximant Au$_{70}$Si$_{17}$Tb$_{13}$, consisting of icosahedral spin clusters in a body-centered-cubic lattice. Bulk magnetic measurements performed on the single crystalline sample unambiguously confirm long-range ordering at $T_{\rm C} = 11.6 \pm 1$ K. In contrast to the simple ferromagnetic response in the bulk measurements, single crystal neutron diffraction confirms a formation of intriguing non-collinear and non-coplanar magnetic order. The magnetic moment direction was found to be nearly tangential to the icosahedral cluster surface in the local mirror plane, which is quite similar to that recently found in the antiferromagnetic quasicrystal approximant Au$_{72}$Al$_{14}$Tb$_{14}$. Inelastic neutron scattering on the powdered sample exhibits a very broad peak centered at $\hbar \omega \simeq 4$ meV. The observed inelastic spectrum was explained by the crystalline-electric-field model taking account of the chemical disorder at the fractional Au/Si sites. The resulting averaged anisotropy axis for the crystalline-electric-field ground state is consistent with the ordered moment direction determined in the magnetic structure analysis, confirming that the non-coplanar magnetic order is stabilized by the local uniaxial anisotropy., Comment: 14 pages, 10 figures, 3 tables

The High Resolution Chopper Spectrometer (HRC) installed at MLF, J-PARC provides opportunities for dynamical studies of materials over a wide energy-momentum space with high resolution. Three types of inelastic neutron scattering experiments can be performed with the HRC: high-resolution experiments in a conventional energy-momentum space, eV neutron spectroscopy, and neutron Brillouin scattering (NBS). Some results have been obtained using these techniques. The NBS option makes the HRC different from other chopper spectrometers. Coherent excitations in non-single-crystal samples can be observed with NBS. On the HRC, NBS experiments were made feasible by reducing the background noise at low scattering angles, and some results were obtained.

Neutron Brillouin scattering (NBS) experiments can be performed on the High Resolution Chopper Spectrometer (HRC). Recently, an intensity gain of a factor 2.4 with an improved resolution for NBS has been obtained by improving the detector system, the Fermi chopper, and the collimator system. This improved performance provides opportunities for intense studies of dynamics in condensed matter by using non-single-crystal samples.

We developed control and visualization programs, YUI and HANA, for High- Resolution Chopper spectrometer (HRC) installed at BL12 in MLF, J-PARC. YUI is a comprehensive program to control DAQ-middleware, the accessories, and sample environment devices. HANA is a program for the data transformation and visualization of inelastic neutron scattering spectra. In this paper, we describe the basic system structures and unique functions of these programs from the viewpoint of users., 9 pages, 4 figures

We investigated the iron-based ladder compounds (Ba,$\mathrm{Cs}){\mathrm{Fe}}_{2}{\mathrm{Se}}_{3}$. Their parent compounds ${\mathrm{BaFe}}_{2}{\mathrm{Se}}_{3}$ and ${\mathrm{CsFe}}_{2}{\mathrm{Se}}_{3}$ have different space groups, formal valences of Fe, and magnetic structures. Electrical resistivity, specific heat, magnetic susceptibility, x-ray diffraction, and powder neutron diffraction measurements were conducted to obtain a temperature and composition phase diagram of this system. Block magnetism observed in ${\mathrm{BaFe}}_{2}{\mathrm{Se}}_{3}$ is drastically suppressed with Cs doping. In contrast, stripe magnetism observed in ${\mathrm{CsFe}}_{2}{\mathrm{Se}}_{3}$ is not so fragile against Ba doping. A new type of magnetic structure appears in intermediate compositions, which is similar to stripe magnetism of ${\mathrm{CsFe}}_{2}{\mathrm{Se}}_{3}$, but interladder spin configuration is different. Intermediate compounds show insulating behavior, nevertheless a finite $T$-linear contribution in specific heat was obtained at low temperatures.

High-pressure electrical resistance measurements were performed for iron-based ladder material Ba1-xCsxFe2Se3 (x = 0.25 and 0.65) using a diamond anvil cell (DAC). Recent high-pressure study revealed that iron-based ladder material BaFe2S3 exhibits an insulator- metal transition and superconductivity, and this discovery would provide important insight for understanding the mechanism of iron-based superconductors. Therefore, it is intriguing to investigate the high-pressure properties for the iron-based ladder material Ba1-xCsxFe2Se3 system. The parent compounds BaFe2Se3 and CsFe2Se3 show insulating and magnetic ordering features. For Ba1-xCsxFe2Se3 system, no magnetic ordering is observed for x = 0.25 and minimum charge gap was estimated for x = 0.65. The insulator-metal transitions are observed in both materials.

Electrical resistivity measurements have been performed on the iron-based ladder compounds Ba$_{1-x}$Cs$_x$Fe$_2$Se$_3$ ($x$ = 0, 0.25, 0.65, and 1) under high pressure. A cubic anvil press was used up to 8.0 GPa, whereas further higher pressure was applied using a diamond anvil cell up to 30.0 GPa. Metallic behavior of the electrical conductivity was confirmed in the $x$ = 0.25 and 0.65 samples for pressures greater than 11.3 and 14.4 GPa, respectively, with the low-temperature $\log T$ upturn being consistent with weak localization of 2D electrons due to random potential. At pressures higher than 23.8 GPa, three-dimensional Fermi-liquid-like behavior was observed in the latter sample. No metallic conductivity was observed in the parent compounds BaFe$_2$Se$_3$ ($x $ = 0) up to 30.0 GPa and CsFe$_2$Se$_3$ ($x$ = 1) up to 17.0 GPa. The present results indicate that the origins of the insulating ground states in the parent and intermediate compounds are intrinsically different; the former is a Mott insulator, whereas the latter is an Anderson insulator owing to the random substitution of Cs for Ba., Comment: 5 pages, 3 figures

Since the discovery, research on iron-based superconductivity (SC) has become one of the main streams in condensed matter physics [1]. The interplay between structure, magnetism and SC is one of most intriguing subjects of this field. The common structural feature is the presence of square planar sheets of Fe atoms coordinated tetrahedrally by pnictogens or chalcogens. They have been, at the early stage, realized in the ZrCuSiAs (1111), ThCr2Si2 (122), anti-PbO (11) and Cu2Sb (111) structures. To gain further insight into the mechanism of the SC and variation of magnetic orders, investigation of Fe-based compounds with a separate spatial dimension is important. This is because the dimensionality should influence magnetism and can control itinerancy of electrons by changing Fermi surface topology. As spin ladders in copper oxides shed a new light on the mechanism of SC, a study on an analogue with ladder geometry among Fe-based compounds is highly desired. Here we report our recent studies of iron-based ladder compounds AFe2X3 (A = K, Rb, Cs, Ba; X = S, Se, Te) [2,3]. Crystal structure is novel, comprising of FeX4 tetrahedra with channels which host A atoms, and four-fold coordinated Fe2+ ions form two-leg ladder geometry. Unlike most of parent compounds of the Fe-based SCs, the ladder compounds are insulating down to the lowest measured temperature. Through bulk properties and neutron diffraction measurements, a variety of magnetic structures and low dimensional characteristics were elucidated. These would provide a clue of the SC realized in a separate dimension systems. The description of theory that accounts for the observed magnetic structures will be also presented.