Q-dependent Collective Relaxation Dynamics of Glass-Forming Liquid Ca0.4K0.6(NO3)1.4 Investigated by Wide-Angle Neutron Spin-Echo

Employing wide-angle neutron spin echo spectroscopy, we measured the Q-dependent coherent intermediate scattering function of the prototypical ionic glass former Ca0.4K0.6(NO3)1.4, in the equilibrium and supercooled liquid states beyond the hydrodynamic regime. The data reveal a clear two-step relaxation: an exponential fast process, and a stretched exponential slow alpha process. de Gennes narrowing is observed in all characteristic variables of the alpha process: the relaxation time, amplitude, and stretching exponent. At all length scales probed, the relative amplitude of the alpha-relaxation decreases with increasing temperature and levels off in the normal liquid state. The temperature dependence of the stretching exponent and the relaxation time at different Q's indicate that modifications of the relaxation mechanisms at the local length scales, manifested as temperature independent dynamic heterogeneity and smaller deviations from Arrhenius behavior, have occurred even above the alpha-beta (Johari-Goldstein) bifurcation temperature

Dirac quantum spin liquid emerging in a kagome-lattice antiferromagnet

Emerging quasi-particles with Dirac dispersion in condensed matter physics are analogous to their cousins in high-energy physics in that both of them can be described by the Dirac equation for relativistic electrons. Recently, these Dirac fermions have been widely found in electronic systems, such as graphene and topological insulators. At the conceptual level, since the charge is not a prerequisite for Dirac fermions, the emergence of Dirac fermions without charge degree of freedom has been theoretically predicted to be realized in Dirac quantum spin liquids. In such case, the Dirac quasiparticles are charge-neutral and carry a spin of 1/2, known as spinons. Despite of theoretical aspirations, spectra evidence of Dirac spinons remains elusive. Here we show that the spin excitations of a kagome antiferromagnet, YCu$_3$(OD)$_6$Br$_2$[Br$_{x}$(OD)$_{1-x}$], are conical with a spin continuum inside, which are consistent with the convolution of two Dirac spinons. The spinon velocity obtained from the spin excitations also quantitatively reproduces the low-temperature specific heat of the sample. Interestingly, the locations of the conical spin excitations differ from those calculated by the nearest neighbor Heisenberg model, suggesting an unexpected origin of the Dirac spinons. Our results thus provide strong spectra evidence for the Dirac quantum-spin-liquid state emerging in this kagome-lattice antiferromagnet.Comment: 7 pages, 4 figure

Dimensional reduction by geometrical frustration in a cubic antiferromagnet composed of tetrahedral clusters

Dimensionality is a critical factor in determining the properties of solids and is an apparent built-in character of the crystal structure. However, it can be an emergent and tunable property in geometrically frustrated spin systems. Here, we study the spin dynamics of the tetrahedral cluster antiferromagnet, pharmacosiderite, via muon spin resonance and neutron scattering. We find that the spin correlation exhibits a two-dimensional characteristic despite the isotropic connectivity of tetrahedral clusters made of spin 5/2 Fe3+ ions in the three-dimensional cubic crystal, which we ascribe to two-dimensionalisation by geometrical frustration based on spin wave calculations. Moreover, we suggest that even one-dimensionalisation occurs in the decoupled layers, generating low-energy and one-dimensional excitation modes, causing large spin fluctuation in the classical spin system. Pharmacosiderite facilitates studying the emergence of low-dimensionality and manipulating anisotropic responses arising from the dimensionality using an external magnetic field

Two inherent crossovers of the diffusion process in glass-forming liquids

We report on incoherent quasielastic neutron scattering measurements examining a self-diffusion process in two types of glass-forming liquids, namely a molecular liquid (3-methylpentane) and an ionic liquid [1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide]. We have experimentally demonstrated that both liquids exhibit two crossovers in the momentum transfer ($Q$) dependence of the self-correlation function, which is basically described by the stretched exponential function, exp [ − ( t / τ )$^β$ ] . The first crossover point ($Q$ ≈ 0.2 Å$^{−1}$) corresponds to a crossover from Fickian ( β = 1 ) to non-Fickian ( β ≠ 1 ) diffusion attributed to dynamical correlation. On the other hand, the second one at $Q$ ≈ 0.8 Å$^{−1}$ is associated with the crossover from Gaussian to non-Gaussian behavior. It is remarkable that the stretching exponent β gradually changes in between the two crossover points. We consider that the two crossovers are the universal feature for glass-forming liquids

Optimization and inference of bin widths for histogramming inelastic neutron scattering spectra

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

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

Abstract 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 T N = 2.3 K in the crystalline state, while a spin glass transition occurs at T SG = 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 T SG and gradually disappeared above T SG. 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