Seiko Ohira-Kawamura

Magnetic and non-magnetic phases of a quantum spin liquid

A quantum spin-liquid phase is an intriguing possibility for a system of strongly interacting magnetic units in which the usual magnetically ordered ground state is avoided owing to strong quantum fluctuations. It was first predicted theoretically for a triangular-lattice model with antiferromagnetically coupled S = 1/2 spins. Recently, materials have become available showing persuasive experimental evidence for such a state. Although many studies show that the ideal triangular lattice of S = 1/2 Heisenberg spins actually orders magnetically into a three-sublattice, non-collinear 120° arrangement, quantum fluctuations significantly reduce the size of the ordered moment. This residual ordering can be completely suppressed when higher-order ring-exchange magnetic interactions are significant, as found in nearly metallic Mott insulators. The layered molecular system κ-(BEDT-TTF)2Cu2(CN)3 is a Mott insulator with an almost isotropic, triangular magnetic lattice of spin-1/2 BEDT-TTF dimers that provides a prime example of a spin liquid formed in this way. Despite a high-temperature exchange coupling, J, of 250 K (ref. 6), no obvious signature of conventional magnetic ordering is seen down to 20 mK (refs 7, 8). Here we show, using muon spin rotation, that applying a small magnetic field to this system produces a quantum phase transition between the spin-liquid phase and an antiferromagnetic phase with a strongly suppressed moment. This can be described as Bose–Einstein condensation of spin excitations with an extremely small spin gap. At higher fields, a second transition is found that suggests a threshold for deconfinement of the spin excitations. Our studies reveal the low-temperature magnetic phase diagram and enable us to measure characteristic critical properties. We compare our results closely with current theoretical models, and this gives some further insight into the nature of the spin-liquid phase.

AMATERAS: A Cold-Neutron Disk Chopper Spectrometer

AMATERAS is a new disk-chopper-type spectrometer installed at Materials and Life Science Experimental Facility (MLF) of J-PARC. AMATERAS is equipped with an extra chopper for pulse shaping at the upstream position, in addition to a monochromating chopper, which conventional chopper spectrometers at pulsed source have. Owing to the use of these choppers and the high peak intensity from a coupled moderator source at MLF, the AMATERAS design realizes high-intensity and high-energy-resolution measurements in quasielastic and inelastic neutron scattering experiments. The spectrometer had the first neutron beam in May 2009. During the course of commissioning, the performance of the spectrometer was confirmed by conducting test experiments. AMATERAS is now open to users and is producing scientific outputs.

Relationship between Torsion and Anisotropic Exchange Coupling in a TbIII-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 Ĵ = (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.

Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH 3 NH 3 PbI 3

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.

Temperature and Ag Doping Effect on Magnetic Excitations in the Quasi-Two-Dimensional Triangular Lattice Antiferromagnet CuCrO2 Studied by Inelastic Neutron Scattering

We have studied magnetic excitations in quasi-two-dimensional triangular lattice antiferromagnets CuCrO 2 and Cu 0.85 Ag 0.15 CrO 2 by inelastic neutron scattering. CuCrO 2 has two types of magnetic excitations: one is highly dispersive, while the other is less dispersive and spreads over a wide Q range. With increasing temperature, the weight of the latter component transfers to a lower energy, and the spin dynamics becomes a mixture of a disordered spin wave and another diffuse component. Ag doping induces a similar spin dynamics even at 5 K. This manifests the impact of Ag doping on magnetic correlations and gives a clue to understanding the unconventional spin state in the Ag-doped CuCrO 2 .

Spin-nematic interaction in the multiferroic compound Ba2CoGe2O7.

We demonstrate the existence of the spin-nematic interactions in an easy-plane type antiferromagnet Ba2CoGe2O7 by exploring the magnetic anisotropy and spin dynamics. The combination of neutron scattering and magnetic susceptibility measurements reveals that the origin of the in-plane anisotropy is an antiferro-type interaction of the spin-nematic operator. The relation between the nematic operator and the electric polarization in the ligand symmetry of this compound is presented. The introduction of the spin-nematic interaction is useful to understand the physics of spin and electric dipole in multiferroic compounds.

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.

Spinon, soliton, and breather in the spin-12antiferromagnetic chain compoundKCuGaF6

Elementary excitations of the S=1/2 one-dimensional antiferromagnet KCuGaF_6 were investigated by inelastic neutron scattering in zero and finite magnetic fields perpendicular to the (1, 1, 0) plane combined with specific heat measurements. KCuGaF

Development of Spin Correlations in the Geometrically Frustrated Triangular-Lattice Heisenberg Antiferromagnet CuCrO2

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