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A. Miyata

Publications and source records attributed to A. Miyata.

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Contrasting magnetic behavior in MnSc_2X_4 (X = S, Se) spinel compounds investigated by magnetoelastic studies

The spinel compounds MnSc_2X_4 are highly frustrated and candidate materials for vortex-like 3q magnetic states, such as skyrmions, with propagation vectors in the [111] plane. Because of the strong magnetoelastic coupling, we could extract a refined magnetic (H, T) phase diagram for MnSc_2S_4 from ultrasound and dilatometry measurements. We found a variety of magnetic phases, including the skyrmion phase, which is stable down to lowest temperatures. In comparison, we investigated MnSc_2Se_4 , having a larger distance between the magnetic Mn^3+ ions using the same methods. Unlike in MnSc_2S_4 , we found no skyrmion phase and overall a lack of sharp anomalies indicative of phase transitions, neither in dilatometry nor ultrasound nor in specific heat and ac-susceptibility data. Motivated by our findings, we performed model calculations, which reproduced the experimentally observed magnetostriction and specific-heat results reasonably well.

cond-mat.str-el

Large out-of-equilibrium magnetocaloric effect in rare-earth zirconate pyrochlores

We explore the magnetic properties of Nd$_2$Zr$_2$O$_7$ and Pr$_2$Zr$_2$O$_7$ single crystals subjected to pulsed magnetic fields up to 60 T using magnetization and magnetocaloric-effect (MCE) measurements, with initial temperatures ranging from 2 to 31K. The MCE data exhibit pronounced and unconventional hysteresis loops, in which the sample temperature increases during both the up-sweep and down-sweep of the field. In Nd$_2$Zr$_2$O$_7$, the MCE further displays a striking plateau as a function of time, followed by a rapid temperature rise that begins at the maximum applied field, across pulses with differing peak-field strengths. Our magnetization measurements reveal an inferred temperature of the magnetic subsystem that differs significantly from the directly measured sample temperature and exhibits opposite hysteresis: the temperature is higher on the up-sweep than the down-sweep, unlike the direct measurements. These observations indicate a breakdown of thermal equilibrium between magnetic and lattice degrees of freedom on the timescale of the pulse ($\sim 10^{-1}$s). We interpret the results using a phenomenological model involving two thermally coupled subsystems - the magnetic ions and phonons, and a thermal reservoir, which accounts well for the behavior of Pr$_2$Zr$_2$O$_7$. However, it fails to reproduce the plateau seen in Nd$_2$Zr$_2$O$_7$. Agreement with Nd$_2$Zr$_2$O$_7$ data is improved substantially if we allow the thermal coupling between the magnetic and the lattice subsystems to depend on the product $\frac{HdH}{dt}$. Our results reveal anomalously slow heat transfer between magnetic and lattice subsystems and point toward a novel mechanism for dynamically controlling the heat flow in Nd$_2$Zr$_2$O$_7$ via the rate of magnetic field variation.

cond-mat.str-el

Ultrasound measurement technique for the single-turn-coil magnets

Ultrasound is a powerful means to study numerous phenomena of condensed-matter physics as acoustic waves couple strongly to structural, magnetic, orbital, and charge degrees of freedom. In this paper, we present such technique combined with single-turn coils (STC) which generate magnetic fields beyond 100 T with the typical pulse duration of 6 us. As a benchmark of this technique, the ultrasound results for MnCr2S4, Cu6[Si6O18]6H2O, and liquid oxygen are shown. The resolution for the relative sound-velocity change in the STC is estimated as Delta v/v~10^-3, which is sufficient to study various field-induced phase transitions and critical phenomena.

cond-mat.other

Magnon-phonon interactions in the spinel compound MnSc$_2$Se$_4$

We investigated the magnetic and magnetoelastic properties of MnSc$_2$Se$_4$ single crystals at low temperature under a magnetic field directed along the crystallographic [111] axis. The magnetization data at low temperature show a linear increase with magnetic field, until saturation is reached above 15 T. In ultrasound, a longitudinal acoustic mode shows a softening in field, which is absent for a transverse acoustic mode. We discuss these results using a microscopic model based on the framework of linear spin-wave theory. The magnetic and magnetoelastic data are qualitatively reproduced by considering magnon-phonon interactions arising from exchange-striction coupling between the crystal lattice and spin-wave fluctuations in the zero-temperature limit.

cond-mat.str-el

Unveiling new quantum phases in the Shastry-Sutherland compound SrCu2(BO3)2up to the saturation magnetic field

Under magnetic fields, quantum magnets often undergo exotic phase transitions with various kinds of order. The discovery of a sequence of fractional magnetization plateaus in the Shastry-Sutherland compound SrCu2(BO3)2 has played a central role in the high-field research on quantum materials, but so far this system could only be probed up to half the saturation value of the magnetization. Here, we report the first experimental and theoretical investigation of this compound up to the saturation magnetic field of 140 T and beyond. Using ultrasound and magnetostriction techniques combined with extensive tensor-network calculations (iPEPS), several spin-supersolid phases are revealed between the 1/2 plateau and saturation (1/1 plateau). Quite remarkably, the sound velocity of the 1/2 plateau exhibits a drastic decrease of -50%, related to the tetragonal-to-orthorhombic instability of the checkerboard-type magnon crystal. The unveiled nature of this paradigmatic quantum system is a new milestone for exploring exotic quantum states of matter emerging in extreme conditions.

cond-mat.str-el

Refining magnetic interactions from the magnetic field dependence of spin-wave excitations in magnetoelectric LiFePO$_4$

We investigated the spin excitations of magnetoelectric $\text{LiFePO}_4$ by THz absorption spectroscopy in magnetic fields up to 33$\,$T. By studying their selection rules, we found not only magnetic-dipole, but also electric-dipole active (electromagnons) and magnetoelectric resonances. The magnetic field dependence of four strong low-energy modes is reproduced well by our four-sublattice spin model for fields applied along the three orthorhombic axes. From the fit, we refined the exchange couplings, single-ion anisotropies, and the Dzyaloshinskii-Moriya interaction parameters. Additional spin excitations not described by the mean-field model are observed at higher frequencies. Some of them shows a strong shift with magnetic field, up to 4$\,\text{cm}^{-1}/\text{T}$, when the field is applied along the easy axis. Based on this field dependence, we attribute these high frequency resonances to excitation of higher spin multipoles and of two magnons, which become THz-active due to the low symmetry of the magnetically ordered state.

cond-mat.str-el

Coexistence of antiferromagnetism and ferrimagnetism in adjacent honeycomb layers

Antiferromagnetic and ferro/ferrimagnetic orders are typically exclusive in nature, thus, their co-existence in atomic-scale proximity is expected only in heterostructures. Breaking this paradigm and broadening the range of unconventional magnetic states, we report here on an atomic-scale hybrid spin state, which is stabilized in three-dimensional crystals of the polar antiferromagnet Co$_2$Mo$_3$O$_8$ by magnetic fields applied perpendicular to the \emph{Co} honeycomb layers and possesses a spontaneous in-plane ferromagnetic moment. Our microscopic spin model, capturing the observed field dependence of the longitudinal and transverse magnetization as well as the magnetoelectric/elastic properties, reveals that this novel spin state is composed of an alternating stacking of antiferromagnetic and ferrimagnetic honeycomb layers. The strong intra-layer and the weak inter-layer exchange couplings together with competing anisotropies at octahedral and tetrahedral \emph{Co} sites are identified as the key ingredients to stabilize antiferromagnetic and ferrimagnetic layers in such a close proximity. We show that the proper balance of magnetic interactions can extend the stability range of this hybrid phase down to zero magnetic field. The possibility to realize a layer-by-layer stacking of such distinct spin orders via suitable combinations of microscopic interactions opens a new dimension towards the nanoscale engineering of magnetic states.

cond-mat.str-el

Field-induced valence fluctuation in YbB$_{12}$

We performed high-magnetic-field ultrasonic experiments on YbB$_{12}$ up to 59 T to investigate the valence fluctuations in Yb ions. In zero field, the longitudinal elastic constant $C_{11}$, the transverse elastic constants $C_{44}$ and $\left( C_{11} - C_{12} \right)/2$, and the bulk modulus $C_\mathrm{B}$ show a hardening with a change of curvature at around 35 K indicating a small contribution of valence fluctuations to the elastic constants. When high magnetic fields are applied at low temperatures, $C_\mathrm{B}$ exhibits a softening above a field-induced insulator-metal transition signaling field-induced valence fluctuations. Furthermore, at elevated temperatures, the field-induced softening of $C_\mathrm{B}$ takes place at even lower fields and $C_\mathrm{B}$ decreases continuously with field. Our analysis using the multipole susceptibility based on a two-band model reveals that the softening of $C_\mathrm{B}$ originates from the enhancement of multipole-strain interaction in addition to the decrease of the insulator energy gap. This analysis indicates that field-induced valence fluctuations of Yb cause the instability of the bulk modulus $C_\mathrm{B}$.

cond-mat.str-el

Magnetic structure and high-field magnetization of the distorted kagome lattice antiferromagnet Cs$_2$Cu$_3$SnF$_{12}$

High-resolution time-of-flight powder neutron diffraction and high-field magnetization were measured to investigate the magnetic structure and existence of a field-induced magnetic phase transition in the distorted kagome antiferromagnet Cs$_2$Cu$_3$SnF$_{12}$. Upon cooling from room temperature, the compound undergoes a structural phase transition at $T_\textrm{t}=185$ K from the rhombohedral space group $R\bar{3}m$ with the perfect kagome spin network to the monoclinic space group $P2_1/n$ with the distorted kagome planes. The distortion results in three inequivalent exchange interactions among the $S=1/2$ Cu$^{2+}$ spins that magnetically order below $T_\textrm{N}=20.2$ K. Magnetization measured with a magnetic field applied within the kagome plane reveals small in-plane ferromagnetism resulting from spin canting. On the other hand, the out-of-plane magnetization does not show a clear hysteresis loop of the ferromagnetic component nor a prominent anomaly up to 170 T, with the exception of the subtle knee-like bend around 90 T, which could indicate the 1/3 magnetization plateau. The combined analysis using the irreducible representations of the magnetic space groups and magnetic structure refinement on the neutron powder diffraction data suggests that the magnetic moments order in the magnetic space group $P2_1'/n'$ with the all-in-all-out spin structure, which by symmetry allows for the in-plane canting, consistent with the in-plane ferromagnetism observed in the magnetization.

cond-mat.str-el

Magnetoelastic study on the frustrated quasi-one-dimensional spin-1/2 magnet LiCuVO$_4$

We investigated the magnetoelastic properties of the quasi-one-dimensional spin-1/2 frustrated magnet LiCuVO$_4$. Longitudinal-magnetostriction experiments were performed at 1.5 K in high magnetic fields of up to 60 T applied along the $b$ axis, i.e., the spin-chain direction. The magnetostriction data qualitatively resemble the magnetization results, and saturate at $H_{\text{sat}} \approx 54$ T, with a relative change in sample length of $ΔL/L \approx 1.8\times10^{-4}$. Remarkably, both the magnetostriction and the magnetization evolve gradually between $H_{\text{c3}} \approx 48$ T and $H_{\text{sat}}$, indicating that the two quantities consistently detect the spin-nematic phase just below the saturation. Numerical analyses for a weakly coupled spin-chain model reveal that the observed magnetostriction can overall be understood within an exchange-striction mechanism. Small deviations found may indicate nontrivial changes in local correlations associated with the field-induced phase transitions.

cond-mat.str-el

Spin-lattice coupling in a ferrimagnetic spinel: The exotic $H$-$T$ phase diagram of MnCr$_2$S$_4$ up to 110 T

In antiferromagnets, the interplay of spin frustration and spin-lattice coupling has been extensively studied as the source of complex spin patterns and exotic magnetism. Here, we demonstrate that, although neglected in the past, the spin-lattice coupling is essential to ferrimagnetic spinels as well. We performed ultrahigh-field magnetization measurements up to 110 T on a Yafet-Kittel ferrimagnetic spinel, MnCr$_2$S$_4$, which was complemented by measurements of magnetostriction and sound velocities up to 60 T. Classical Monte Carlo calculations were performed to identify the complex high-field spin structures. Our minimal model incorporating spin-lattice coupling accounts for the experimental results and corroborates the complete phase diagram, including two new high-field phase transitions at 75 and 85 T. Magnetoelastic coupling induces striking effects: An extremely robust magnetization plateau is embedded between two unconventional spin-asymmetric phases. Ferrimagnetic spinels provide a new platform to study asymmetric and multiferroic phases stabilized by spin-lattice coupling.

cond-mat.str-el

Magnetization beyond the Ising limit of Ho$_2$Ti$_2$O$_7$

We report that the local Ising anisotropy in pyrochlore oxides - the crucial requirement for realizing the spin-ice state - can be broken by means of high magnetic fields. For the case of the well-established classical spin-ice compound Ho$_2$Ti$_2$O$_7$ the magnetization exceeds the angle-dependent saturation value of the Ising limit using ultra-high fields up to 120 T. However, even under such extreme magnetic fields full saturation cannot be achieved. Crystal-electric-field calculations reveal that a level crossing for two of the four ion positions leads to magnetization steps at 55 and 100 T. In addition, we show that by using a field sweep rate in the range of the spin-relaxation time the dynamics of the spin system can be probed. Exclusively at 25 ns/T a new peak of the susceptibility appears around 2 T. We argue, this signals the cross-over between spin-ice and polarized correlations.

cond-mat.str-el

The impact of the halide cage on the electronic properties of fully inorganic caesium lead halide perovskites

Perovskite solar cells with record power conversion efficiency are fabricated by alloying both hybrid and fully inorganic compounds. While the basic electronic properties of the hybrid perovskites are now well understood, key electronic parameters for solar cell performance, such as the exciton binding energy of fully inorganic perovskites, are still unknown. By performing magneto transmission measurements, we determine with high accuracy the exciton binding energy and reduced mass of fully inorganic CsPbX$_3$ perovskites (X=I, Br, and an alloy of these). The well behaved (continuous) evolution of the band gap with temperature in the range $4-270$\,K suggests that fully inorganic perovskites do not undergo structural phase transitions like their hybrid counterparts. The experimentally determined dielectric constants indicate that at low temperature, when the motion of the organic cation is frozen, the dielectric screening mechanism is essentially the same both for hybrid and inorganic perovskites, and is dominated by the relative motion of atoms within the lead-halide cage.

physics.app-ph

Ultrahigh magnetic field spectroscopy reveals the band structure of the 3D topological insulator Bi$_2$Se$_3$

We have investigated the band structure at the $Γ$ point of the three-dimensional (3D) topological insulator Bi$_2$Se$_3$ using magneto-spectroscopy over a wide range of energies ($0.55-2.2$\,eV) and in ultrahigh magnetic fields up to 150\,T. At such high energies ($E>0.6$\,eV) the parabolic approximation for the massive Dirac fermions breaks down and the Landau level dispersion becomes nonlinear. At even higher energies around 0.99 and 1.6 eV, new additional strong absorptions are observed with a temperature and magnetic-field dependence which suggest that they originate from higher band gaps. Spin orbit splittings for the further lying conduction and valence bands are found to be 0.196 and 0.264 eV.

cond-mat.mes-hall