Signatures of Kitaev Interactions in the van der Waals Ferromagnet VI_{3}.

Materials manifesting the Kitaev model, characterized by bond-dependent interactions on a honeycomb lattice, can host exotic phenomena like quantum spin liquid states and topological magnetic excitations. However, finding such materials remains a formidable challenge. Here, we report high-resolution inelastic neutron scattering measurements performed on VI_{3}, a van der Waals ferromagnetic Mott insulator, covering a wide range of reciprocal space. Our measurements unveil highly anisotropic magnetic excitations in momentum space. Through a comprehensive comparative analysis of various models that incorporate diverse symmetry-allowed magnetic interactions, we find the observed excitations are well captured by a model with a large bond-dependent Kitaev interaction. These results not only help to understand the intriguing properties of VI_{3}, such as the pronounced anomalous thermal Hall effects and strong pressure or structure dependence of magnetism, but also open a new avenue for exploring Kitaev physics.

Role of Exchange Cations and Layer Charge on the Dynamics of Confined Water.

Describing the dynamic behavior of water confined in clay minerals is a fascinating challenge and crucial in many research areas, ranging from materials science and geotechnical engineering to environmental sustainability. Water is the most abundant resource on Earth, and the high reactivity of naturally occurring hydrous clay minerals used since prehistoric times for a variety of applications means that water-clay interaction is a ubiquitous phenomenon in nature. We have attempted to experimentally distinguish the rotational dynamics and translational diffusion of two distinct populations of interlayer water, confined and ultraconfined, in the sodium (Na) forms of two smectite clay minerals, montmorillonite (Mt) and hectorite (Ht). Samples hydrated at a pseudo one-layer hydration (1LH) state under ambient conditions were studied with quasi-elastic neutron scattering (QENS) between 150 and 300 K. Using a simplified revised jump-diffusion and rotation-diffusion model (srJRM), we observed that while interlayer water near the ditrigonal cavity in Ht forms strong H-bonds to both adjacent surface O and structural OH, H-bonding of other more prevalent interlayer water with the surface O is weaker compared to Mt, inducing a higher temperature for dynamical changes of confined water. Given the lower layer charge and faster dynamics observed for Ht compared to Mt, we consider this strong evidence confirming the influence of the interlayer cation and surfaces on confined water dynamics.

Field-tuned quantum effects in a triangular-lattice Ising magnet.

We report thermodynamic and neutron scattering measurements of the triangular-lattice quantum Ising magnet TmMgGaO4 in longitudinal magnetic fields. Our experiments reveal a quasi-plateau state induced by quantum fluctuations. This state exhibits an unconventional non-monotonic field and temperature dependence of the magnetic order and excitation gap. In the high field regime where the quantum fluctuations are largely suppressed, we observed a disordered state with coherent magnon-like excitations despite the suppression of the spin excitation intensity. Through detailed semi-classical calculations, we are able to understand these behaviors quantitatively from the subtle competition between quantum fluctuations and frustrated Ising interactions.

Spin glass behavior and magnetic boson peak in a structural glass of a magnetic ionic liquid.

Glassy magnetic behavior has been observed in a wide range of crystalline magnetic materials called spin glass. Here, we report spin glass behavior in a structural glass of a magnetic ionic liquid, C4mimFeCl4. Magnetization measurements demonstrate that an antiferromagnetic ordering occurs at TN = 2.3 K in the crystalline state, while a spin glass transition occurs at TSG = 0.4 K in the structural glass state. In addition, localized magnetic excitations were found in the spin glass state by inelastic neutron scattering, in contrast to spin-wave excitations in the ordered phase of the crystalline sample. The localized excitation was scaled by the Bose population factor below TSG and gradually disappeared above TSG. This feature is highly reminiscent of boson peaks commonly observed in structural glasses. We suggest the "magnetic" boson peak to be one of the inherent dynamics of a spin glass state.

Gapless spin liquid in a square-kagome lattice antiferromagnet.

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.

Localized Magnetic Excitations in the Fully Frustrated Dimerized Magnet Ba_{2}CoSi_{2}O_{6}Cl_{2}.

Magnetic excitations of the effective spin S=1/2 dimerized magnet Ba_{2}CoSi_{2}O_{6}Cl_{2} have been probed directly via inelastic neutron scattering experiments at temperatures down to 4 K. We observed five types of excitation at 4.8, 5.8, 6.6, 11.4, and 14.0 meV, which are all dispersionless within the resolution limits. The scattering intensities of the three low-lying excitations were found to exhibit different Q dependencies. Detailed analysis has demonstrated that Ba_{2}CoSi_{2}O_{6}Cl_{2} is a two-dimensional spin dimer system described only by a single dimer site, where the triplet excitations are localized owing to the almost perfect frustration of the interdimer exchange interactions and the undimerized spins, even in small concentration, make an essential contribution to the excitation spectrum.

Evidence for singular-phonon-induced nematic superconductivity in a topological superconductor candidate Sr0.1Bi2Se3.

Superconductivity mediated by phonons is typically conventional, exhibiting a momentum-independent s-wave pairing function, due to the isotropic interactions between electrons and phonons along different crystalline directions. Here, by performing inelastic neutron scattering measurements on a superconducting single crystal of Sr0.1Bi2Se3, a prime candidate for realizing topological superconductivity by doping the topological insulator Bi2Se3, we find that there exist highly anisotropic phonons, with the linewidths of the acoustic phonons increasing substantially at long wavelengths, but only for those along the [001] direction. This observation indicates a large and singular electron-phonon coupling at small momenta, which we propose to give rise to the exotic p-wave nematic superconducting pairing in the MxBi2Se3 (M = Cu, Sr, Nb) superconductor family. Therefore, we show these superconductors to be example systems where electron-phonon interaction can induce more exotic superconducting pairing than the s-wave, consistent with the topological superconductivity.

Triplon band splitting and topologically protected edge states in the dimerized antiferromagnet.

Search for topological materials has been actively promoted in the field of condensed matter physics for their potential application in energy-efficient information transmission and processing. Recent studies have revealed that topologically invariant states, such as edge states in topological insulators, can emerge not only in a fermionic electron system but also in a bosonic system, enabling nondissipative propagation of quasiparticles. Here we report the topologically nontrivial triplon bands measured by inelastic neutron scattering on the spin-1/2 two-dimensional dimerized antiferromagnet Ba2CuSi2O6Cl2. The excitation spectrum exhibits two triplon bands that are clearly separated by a band gap due to a small alternation in interdimer exchange interaction, consistent with a refined crystal structure. By analytically modeling the triplon dispersion, we show that Ba2CuSi2O6Cl2 is the first bosonic realization of the coupled Su-Schrieffer-Heeger model, where the presence of topologically protected edge states is prompted by a bipartite nature of the lattice.

Colossal barocaloric effects in plastic crystals.

Refrigeration is of vital importance for modern society-for example, for food storage and air conditioning-and 25 to 30 per cent of the world's electricity is consumed for refrigeration1. Current refrigeration technology mostly involves the conventional vapour compression cycle, but the materials used in this technology are of growing environmental concern because of their large global warming potential2. As a promising alternative, refrigeration technologies based on solid-state caloric effects have been attracting attention in recent decades3-5. However, their application is restricted by the limited performance of current caloric materials, owing to small isothermal entropy changes and large driving magnetic fields. Here we report colossal barocaloric effects (CBCEs) (barocaloric effects are cooling effects of pressure-induced phase transitions) in a class of disordered solids called plastic crystals. The obtained entropy changes in a representative plastic crystal, neopentylglycol, are about 389 joules per kilogram per kelvin near room temperature. Pressure-dependent neutron scattering measurements reveal that CBCEs in plastic crystals can be attributed to the combination of extensive molecular orientational disorder, giant compressibility and highly anharmonic lattice dynamics of these materials. Our study establishes the microscopic mechanism of CBCEs in plastic crystals and paves the way to next-generation solid-state refrigeration technologies.

Spin correlations of quantum spin liquid and quadrupole-ordered states of Tb2+x Ti2-x O7+y.

Spin correlations of the frustrated pyrochlore oxide Tb2+x Ti2-x O7+y have been investigated by using inelastic neutron scattering on single-crystalline samples (x = -0.007, 0.000, and 0.003), which have the putative quantum-spin-liquid (QSL) or electric-quadrupolar ground states. Spin correlations, which are notably observed in nominally elastic scattering, show short-range correlations around L points [ q = ( 1 2 , 1 2 , 1 2 ) ] , tiny antiferromagnetic Bragg scattering at L and Γ points, and pinch-point-type structures around Γ points. The short-range spin correlations were analyzed using a random-phase approximation (RPA) assuming the paramagnetic state and two-spin interactions among Ising spins. These analyses have shown that the RPA scattering intensity well reproduces the experimental data using temperature- and x-dependent coupling constants of up to tenth-neighbor site pairs. This suggests that no symmetry breaking occurs in the QSL sample and that a quantum treatment beyond the semiclassical RPA approach is required. Implications of the experimental data and the RPA analyses are discussed.

Retreat from Stress: Rattling in a Planar Coordination.

Thermoelectric devices convert heat flow to charge flow, providing electricity. Materials for highly efficient devices must satisfy conflicting requirements of high electrical conductivity and low thermal conductivity. Thermal conductivity in caged compounds is known to be suppressed by a large vibration of guest atoms, so-called rattling, which effectively scatters phonons. Here, the crystal structure and phonon dynamics of tetrahedrites (Cu,Zn)12 (Sb,As)4 S13 are studied. The results reveal that the Cu atoms in a planar coordination are rattling. In contrast to caged compounds, chemical pressure enlarges the amplitude of the rattling vibration in the tetrahedrites so that the rattling atom is squeezed out of the planar coordination. Furthermore, the rattling vibration shakes neighbors through lone pairs of the metalloids, Sb and As, which is responsible for the low thermal conductivity of tetrahedrites. These findings provide a new strategy for the development of highly efficient thermoelectric materials with planar coordination.

Structure of the magnetic excitations in the spin-1/2 triangular-lattice Heisenberg antiferromagnet Ba3CoSb2O9.

A spin-1/2 triangular-lattice Heisenberg antiferromagnet (TLHAF) is a prototypical frustrated quantum magnet, which exhibits remarkable quantum many-body effects that arise from the synergy between spin frustration and quantum fluctuation. The ground-state properties of a spin-1/2 TLHAF are theoretically well understood. However, the theoretical consensus regarding the magnetic excitations is limited. The experimental study of the magnetic excitations in spin-1/2 TLHAFs has also been limited. Here we show the structure of magnetic excitations in the spin-1/2 TLHAF Ba3CoSb2O9 investigated by inelastic neutron scattering. Significantly different from theoretical expectations, the excitation spectrum has a three-stage energy structure. The lowest-energy first stage is composed of dispersion branches of single-magnon excitations. The second and third stages are dispersive continua accompanied by a columnar continuum extending above 10 meV, which is six times larger than the exchange interaction J = 1.67 meV. Our results indicate the shortcomings of the current theoretical framework.Two-dimensional frustrated magnets are heavily studied because theories predict that quantum effects may lead to the emergence of fractionalized excitations. Ito et al. use inelastic neutron scattering to show that the excitation spectrum of Ba3CoSb2O9 disagrees with current theoretical expectations.

Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH3NH3PbI3.

Perovskite CH3NH3PbI3 exhibits outstanding photovoltaic performances, but the understanding of the atomic motions remains inadequate even though they take a fundamental role in transport properties. Here, we present a complete atomic dynamic picture consisting of molecular jumping rotational modes and phonons, which is established by carrying out high-resolution time-of-flight quasi-elastic and inelastic neutron scattering measurements in a wide energy window ranging from 0.0036 to 54 meV on a large single crystal sample, respectively. The ultrafast orientational disorder of molecular dipoles, activated at ∼165 K, acts as an additional scattering source for optical phonons as well as for charge carriers. It is revealed that acoustic phonons dominate the thermal transport, rather than optical phonons due to sub-picosecond lifetimes. These microscopic insights provide a solid standing point, on which perovskite solar cells can be understood more accurately and their performances are perhaps further optimized.

Spontaneous decays of magneto-elastic excitations in non-collinear antiferromagnet (Y,Lu)MnO3.

Magnons and phonons are fundamental quasiparticles in a solid and can be coupled together to form a hybrid quasi-particle. However, detailed experimental studies on the underlying Hamiltonian of this particle are rare for actual materials. Moreover, the anharmonicity of such magnetoelastic excitations remains largely unexplored, although it is essential for a proper understanding of their diverse thermodynamic behaviour and intrinsic zero-temperature decay. Here we show that in non-collinear antiferromagnets, a strong magnon-phonon coupling can significantly enhance the anharmonicity, resulting in the creation of magnetoelastic excitations and their spontaneous decay. By measuring the spin waves over the full Brillouin zone and carrying out anharmonic spin wave calculations using a Hamiltonian with an explicit magnon-phonon coupling, we have identified a hybrid magnetoelastic mode in (Y,Lu)MnO3 and quantified its decay rate and the exchange-striction coupling term required to produce it.

Difference in the hydration water mobility around F-actin and myosin subfragment-1 studied by quasielastic neutron scattering.

Hydration water is essential for a protein to perform its biological function properly. In this study, the dynamics of hydration water around F-actin and myosin subfragment-1 (S1), which are the partner proteins playing a major role in various cellular functions related to cell motility including muscle contraction, was characterized by incoherent quasielastic neutron scattering (QENS). The QENS measurements on the D2O- and H2O-solution samples of F-actin and S1 provided the spectra of hydration water, from which the translational diffusion coefficient (DT), the residence time (τT), and the rotational correlation time (τR) were evaluated. The DT value of the hydration water of S1 was found to be much smaller than that of the hydration water of F-actin while the τT values were similar between S1 and F-actin. On the other hand, the τR values of the hydration water of S1 was found to be larger than that of the hydration water of F-actin. It was also found that the DT and τR values of the hydration water of F-actin are similar to those of bulk water. These results suggest a significant difference in mobility of the hydration water between S1 and F-actin: S1 has the typical hydration water, the mobility of which is reduced compared with that of bulk water, while F-actin has the unique hydration water, the mobility of which is close to that of bulk water rather than the typical hydration water around proteins.

Relationship between Torsion and Anisotropic Exchange Coupling in a Tb(III)-Radical-Based Single-Molecule Magnet.

The incorporation of paramagnetic ligands within rare-earth ion clusters exhibiting large magnetic anisotropy has provided significant advancement in the design of single-molecule magnets (SMMs) with large blocking temperatures. However, the exchange interaction in such systems is complex and difficult to probe by conventional magnetometry techniques, and little is known about the structural relationships. Inelastic neutron scattering and terahertz electron paramagnetic resonance measurements are used complimentarily to investigate the large exchange interaction between a rare earth-radical pair in a Tb(III)-based SMM complex. The origin of the exchange interaction is investigated for two molecular species in the crystallographic unit cell that exhibit different bonding structures between Tb(III) and a 2pyNO radical. A correlation between the Tb-O-N-C torsion angles and the magnitudes of exchange couplings is found. Interestingly, a large nondegeneracy within the ground-state doublet is present for the larger torsion angle species. It is essential to consider the balance of two channels of exchange coupling, 2p-4f hybridization and 2p-5d charge transfer, to explain this characteristic behavior. The former channel gives the antiferromagnetic interaction, and the latter gives the ferromagnetic one. When an effective J = (1)/2 Ising-type Hamiltonian is applied, the exchange couplings are evaluated to be antiferromagnetic J(z) = 9.89 meV (79.8 cm(-1)) for the low torsion angle (3.8°) species and J(z) = 7.39 meV (59.6 cm(-1)) for the larger torsion angle (15.8°) species. It is also found that a small percentage of the transverse exchange component must be included for the larger torsion angle to account for the observed nondegenerate ground state. The symmetry of the exchange couplings is discussed by considering the characters of d and f orbitals.

Internal dynamics of F-actin and myosin subfragment-1 studied by quasielastic neutron scattering.

Various biological functions related to cell motility are driven by the interaction between the partner proteins, actin and myosin. To obtain insights into how this interaction occurs, the internal dynamics of F-actin and myosin subfragment-1 (S1) were characterized by the quasielastic neutron scattering measurements on the solution samples of F-actin and S1. Contributions of the internal motions of the proteins to the scattering spectra were separated from those of the global macromolecular diffusion. Analysis of the spectra arising from the internal dynamics showed that the correlation times of the atomic motions were about two times shorter for F-actin than for S1, suggesting that F-actin fluctuates more rapidly than S1. It was also shown that the fraction of the immobile atoms is larger for S1 than for F-actin. These results suggest that F-actin actively facilitates the binding of myosin by utilizing the more frequent conformational fluctuations than those of S1.

Mode-distribution analysis of quasielastic neutron scattering and application to liquid water.

A quasielastic neutron scattering (QENS) experiment is a particular technique that endeavors to define a relationship between time and space for the diffusion dynamics of atoms and molecules. However, in most cases, analyses of QENS data are model dependent, which may distort attempts to elucidate the actual diffusion dynamics. We have developed a method for processing QENS data without a specific model, wherein all modes can be described as combinations of the relaxations based on the exponential law. By this method, we can obtain a distribution function B(Q,Γ), which we call the mode-distribution function (MDF), to represent the number of relaxation modes and distributions of the relaxation times in the modes. The deduction of MDF is based on the maximum entropy method and is very versatile in QENS data analysis. To verify this method, reproducibility was checked against several analytical models, such as that with a mode of distributed relaxation time, that with two modes closely located, and that represented by the Kohlrausch-Williams-Watts function. We report the first application to experimental data of liquid water. In addition to the two known modes, the existence of a relaxation mode of water molecules with an intermediate time scale has been discovered. We propose that the fast mode might be assigned to an intermolecular motion and the intermediate motion might be assigned to a rotational motion of the water molecules instead of to the fast mode.