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We investigate the crystallographic and magnetic properties of a chromium-based thiospinel CuGaCr$_{4}$S$_{8}$. From a synchrotron x-ray diffraction experiment and structural refinement, Cu and Ga atoms are found to occupy the tetrahedral $A$-sites in an alternate way, yielding breathing pyrochlore Cr network. CuGaCr$_{4}$S$_{8}$ undergoes a magnetic transition associated with a structural distortion at 31 K in zero magnetic field, indicating that the spin-lattice coupling is responsible for relieving the geometrical frustration. When applying a pulsed high magnetic field, a sharp metamagnetic transition takes place at 40 T, followed by a 1/2-magnetization plateau up to 103 T. These phase transitions accompany dielectric anomalies, suggesting the presence of helical spin correlations in low-field phases. The density-functional-theory calculation reveals that CuGaCr$_{4}$S$_{8}$ is dominated by antiferromagnetic and ferromagnetic exchange couplings within small and large tetrahedra, respectively, in analogy with CuInCr$_{4}$S$_{8}$. We argue that $A$-site-ordered Cr thiospinels serve as an excellent platform to explore diverse magnetic phases along with pronounced magnetoelastic and magnetodielectric responses., Comment: 12 pages, 13 figures

The mutual coupling of spin and lattice degrees of freedom is ubiquitous in magnetic materials and potentially creates exotic magnetic states in response to the external magnetic field. Particularly, geometrically frustrated magnets serve as a fertile playground for realizing magnetic superstructure phases. Here, we observe an unconventional two-step magnetostructural transition prior to a half-magnetization plateau in a breathing pyrochlore chromium spinel by means of state-of-the-art magnetization and magnetostriction measurements in ultrahigh magnetic fields available up to 600 T. Considering a microscopic magnetoelastic theory, the intermediate-field phase can be assigned to a magnetic superstructure with a three-dimensional periodic array of 3-up-1-down and canted 2-up-2-down spin molecules. We attribute the emergence of the magnetic superstructure to a unique combination of the strong spin-lattice coupling and large breathing anisotropy., Comment: 10 pages, 5 figures, SI: 15 pages, 14 figures

The observation of spinon excitations in the $S=\frac{1}{2}$ triangular antiferromagnet Ca$_3$ReO$_5$Cl$_2$ reveals a quasi-one-dimensional (1D) nature of magnetic correlations, in spite of the nominally 2D magnetic structure. This phenomenon is known as frustration-induced dimensional reduction. Here, we present high-field electron spin resonance spectroscopy and magnetization studies of Ca$_3$ReO$_5$Cl$_2$, allowing us not only to refine spin-Hamiltonian parameters, but also to investigate peculiarities of its low-energy spin dynamics. We argue that the presence of the uniform Dzyaloshinskii-Moriya interaction (DMI) shifts the spinon continuum in momentum space and, as a result, opens a zero-field gap at the $\Gamma$ point. We observed this gap directly. The shift is found to be consistent with the structural modulation in the ordered state, suggesting this material as a perfect model triangular-lattice system, where a pure DMI-spiral ground state can be realized.

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., Comment: 8 pages, 4 figures, 2 tables

The polar magnet CaBaCo$_{4}$O$_{7}$ is known to exhibit the largest magnetic-field-driven electric polarization change ($\Delta P$) associated with an antiferromagnetic (AFM)-ferrimagnetic (FIM) transition in a narrow temperature range between 62 and 69 K. In this work, we investigate the effect of Ni doping on its multiferroic properties, by means of magnetization, electric polarization, dielectric constant, and magnetostriction measurements on single crystals of CaBaCo$_{3.9}$Ni$_{0.1}$O$_{7}$ up to 50 T. In the doped material, two kinds of AFM phases appear below 78 K, accompanying negative $\Delta P$. Upon the application of a magnetic field along any crystallographic axis, giant positive $\Delta P$ of up to $11 \sim 12$ mC/m$^{2}$ is observed along with an AFM-FIM transition in the whole temperature range below 78 K. The giant magnetoelectric effect inherent in CaBaCo$_{4}$O$_{7}$ can be further enhanced just by a small amount of chemical substitution, in terms of (i) increasing the magnitude of $\Delta P$ and (ii) expanding the temperature range in which giant $\Delta P$ appears., Comment: 9 pages, 7 figures, SM: 3 pages, 3 figures

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet CuInCr$_{4}$S$_{8}$ with localized $S=3/2$ Cr$^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here, we unveil that CuInCr$_{4}$S$_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered., Comment: 13 pages, 12 figures. Published in Phys. Rev. Research

We have investigated the magnetic properties of Bi0.5Ca0.5MnO3 under ultrahigh magnetic fields by magnetization measurements. This compound shows the metamagnetic transition which indicates the magnetic field induced charge order melting at the room temperature T = 293 K. We reveled that the temperature dependence of the critical field, where the highest critical field is higher than 100 T. At low temperatures, it has been found that the metamagnetic transitions become broad and vanish in the field ascending process below 70 K. On the other hand, in the field descending process, a clear metamagnetic transition is observed even below 70 K. This unusual behavior can be understood as the gradual charge order melting by magnetic field, and its simultaneous reformation. A coexistence of multiple order parameters can account for the observed characteristic dynamics of the first order phase transition. Finally, we constructed the B-T phase diagram with the unusual critical feature at ultrahigh magnetic fields.

We studied the acoustic properties of liquid oxygen up to 90 T by means of ultrasound measurements. We observed a monotonic decrease of the sound velocity and an asymptotic increase of the sound attenuation when applying magnetic fields. The unusual attenuation, twenty times as large as the zero-field value, suggests strong fluctuations of the local molecular arrangement. We point out that the observed fluctuations are related to a liquid-liquid transition or crossover, from a small-magnetization to a large-magnetization liquid, which is characterized by a local-structure rearrangement. To investigate higher-field properties of liquid oxygen, we performed single-turn-coil experiments up to 180 T by means of the acoustic, dilatometric, magnetic, and optical techniques. We observed only monotonic changes of these properties, reflecting the absence of the proposed liquid-liquid transition in our experimental conditions., Comment: 10 pages, 10 figures. arXiv admin note: text overlap with arXiv:1906.01207

Single-turn coil (STC) technique is a convenient way to generate ultrahigh magnetic fields of more than 100 T. During the field generation, the STC explosively destructs outward due to the Maxwell stress and Joule heating. Unfortunately, the STC does not work at its full potential because it has already expanded when the maximum magnetic field is reached. Here, we propose an easy way to delay the expansion and increase the maximum field by using a mass-loaded STC. By loading clay on the STC, the field profile drastically changes, and the maximum field increases by 4 %. This method offers an access to higher magnetic fields for physical property measurements., Comment: 6 pages, 5 figures, Accepted in Review of Scientific Instruments

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 $C_\mathrm{B}$., Comment: 15 pages, 11 figures

The entire magnetization process of TlCuCl$_3$ has been experimentally investigated up to 100 T employing the single-turn technique. The upper critical field $H_{c2}$ is observed to be 86.1 T at 2 K. A convex slope of the $M$-$H$ curve between the lower and upper critical fields ($H_{c1}$ and $H_{c2}$) is clearly observed, which indicates that a particle-hole symmetry is broken in TlCuCl$_3$. By quantum Monte Carlo simulation and the bond-operator theory method, we find that the particle-hole symmetry breaking results from strong inter-dimer interactions.

The acoustic properties of liquid oxygen have been studied up to 90 T by means of the ultrasound pulse-echo technique. A monotonic decrease of the sound velocity and an asymptotic increase of the acoustic attenuation are observed by applying magnetic fields. An unusually large acoustic attenuation, that becomes 20 times as large as the zero-field value, cannot be explained by the classical theory. These results indicate strong fluctuations of antiferromagnetically coupled local structures. We point out that the observed fluctuations are a precursor of a liquid-liquid transition, from a low-susceptibility to a high-susceptibility liquid, which is characterized by a local-structure rearrangement., Comment: 5 pages, 3 figures

The magnetization process of the orthogonal-dimer antiferromagnet SrCu2(BO3)2 is investigated in high magnetic fields of up to 118 T. A 1/2 plateau is clearly observed in the field range 84 to 108 T in addition to 1/8, 1/4 and 1/3 plateaux at lower fields. Using a combination of state-of-the-art numerical simulations, the main features of the high-field magnetization, a 1/2 plateau of width 24 T, a 1/3 plateau of width 34 T, and no 2/5 plateau, are shown to agree quantitatively with the Shastry-Sutherland model if the ratio of inter- to intra-dimer exchange interactions J'/J=0.63. It is further predicted that the intermediate phase between the 1/3 and 1/2 plateau is not uniform but consists of a 1/3 supersolid followed by a 2/5 supersolid and possibly a domain-wall phase, with a reentrance into the 1/3 supersolid above the 1/2 plateau., Comment: 5 pages + 10 pages supplemental material

The valence state of Yb ions in beta-YbAlB4 and its polymorph alpha-YbAlB4 has been investigated by using X-ray absorption and emission spectroscopy in SPring-8 at temperatures from 2 to 280 K. The observed Yb valence is 2.78 +- 0.01 in beta-YbAlB4 at 2 K by using the X-ray emission spectroscopy. The valence is found to gradually increase with increasing temperature toward the trivalent state, and the characteristic temperature of the valence fluctuation is expected to be about 290 K. We also found a small increase in the Yb valence (~0.002) by applying a magnetic field of 32 T at 40 K to beta-YbAlB4., Comment: proceedings of the ICM 2012 (Busan, Korea)

The precision of the values of a magnetic field generated by electromagnetic flux compression was investigated in ultra-high magnetic fields of up to 700 T. In an attempt to calibrate the magnetic field measured by pickup coils, precise Faraday rotation (FR) measurements were conducted on optical (quartz and crown) glasses. A discernible "turn-around" phenomenon was observed in the FR signal as well as the pickup coils before the end of a liner implosion. We found that the magnetic field measured by pickup coils should be corrected by taking into account the high-frequency response of the signal transmission line. Near the peak magnetic field, however, the pickup coils failed to provide reliable values, leaving the FR measurement as the only method to precisely measure an extremely high magnetic fields., Comment: 11 pages, 14 figures

The valence state of Ce in a canonical heavy fermion compound CeRu2Si2 has been investigated by synchrotron X-ray absorption spectroscopy at 1.8 K in high magnetic fields of up to 40 T. The valence was slightly larger than for the pure trivalent state (Ce3+: f1), as expected in heavy fermion compounds, and it decreased toward the trivalent state as the magnetic field was increased. The field-induced valence reduction indicates that the itinerant character of the 4f electrons in CeRu2Si2 was suppressed by a strong magnetic field. The suppression was gradual and showed characteristic magnetic field dependence, which reflects the metamagnetism around Hm \sim 8 T. The itinerant character persisted, even at 40 T (\sim 5Hm), suggesting that the Kondo bound state is continuously broken by magnetic fields and that it should completely collapse at fields exceeding 200 T., Comment: 5 pages, 4 figures, accepted for publication as a Rapid Communication in Physical Review B

We report high resolution single crystal x-ray diffraction measurements of the frustrated pyrochlore magnet Tb2Ti2O7, collected using a novel low temperature pulsed magnet system. This instrument allows characterization of structural degrees of freedom to temperatures as low as 4.4 K, and in applied magnetic fields as large as 30 Tesla. We show that Tb2Ti2O7 manifests intriguing structural effects under the application of magnetic fields, including strongly anisotropic giant magnetostriction, a restoration of perfect pyrochlore symmetry in low magnetic fields, and ultimately a structural phase transition in high magnetic fields. It is suggested that the magnetoelastic coupling thus revealed plays a significant role in the spin liquid physics of Tb2Ti2O7 at low temperatures., Comment: 4 pages, 4 figures, submitted for publication

High-field magnetization, M($H$), on Ni$_{5}$(TeO$_{3}$)$_{4}$X$_{2}$ (X = Br and Cl) were measured by using a pulse magnet. These compounds have a two dimensional crystal structure and a distorted kagome spin frustrated system which is builded by the Ni$^{2+}$ ions ($\textbf{S}$ = 1). The N\'eel transition temperatures are $T_{N} \sim$ 28 and 23 K for X = Br and Cl, respectively. When $T < T_{N}$, we observed a step-like transition at $H_{c} \sim$ 11 and 10 T for X = Br and Cl, respectively. On the other hand, at $T > T_{N}$, the field-dependent magnetization curves behaved like a monotonically increasing straight line up to 55 T. The $H_{c}$ value is close to those obtained by previous spin resonance studies in which a model of spin-flop scenario was proposed to explain the field-dependent resonance spectra. Their model predicts a further transition at around 23 T, however, our observations did not show any plateau behaviors, saturation or other anomalies up to 55 T, suggesting that the further transition possibly exists at a much higher field region., Comment: 7 pages, 4 figures

X-ray magnetic circular dichroism (XMCD) at the Eu L-edge (2p->5d) in two compounds exhibiting valence fluctuation, namely EuNi2(Si0.18Ge0.82)2 and EuNi2P2, has been investigated at pulsed high magnetic fields of up to 40 T. A distinct XMCD peak corresponding to the trivalent state (Eu3+; f6), whose ground state is nonmagnetic (J=0), was observed in addition to the main XMCD peak corresponding to the magnetic (J=7/2) divalent state (Eu2+; f7). This result indicates that the 5d electrons belonging to both valence states are magnetically polarized. It was also found that the ratio P5d(3+)/P5d(2+) between the polarization of 5d electrons (P5d) in the Eu3+ state and that of Eu2+ is ~ 0.1 in EuNi2(Si0.18Ge0.82)2 and ~ 0.3 in EuNi2P2 at magnetic fields where their macroscopic magnetization values are the same. The possible origin of the XMCD of the Eu3+ state and an explanation of the dependence of P5d(3+)/P5d(2+) on the material are discussed in terms of hybridization between the conduction electrons and the f electrons., Comment: 4 pages, 3 figures. accepted for publication in Physical Review Letters

Resonant magnetic x-ray diffraction experiments on the Shastry-Sutherland lattice TbB$_4$ were carried out under strong pulsed magnetic fields up to 30 T. TbB$_4$ exhibits a multi-step magnetization process above 16 T when magnetic fields are applied along the c-axis. We examined the intensity of the 010 magnetic reflection as a function of magnetic field and found that the magnetization plateau phases are accompanied by large XY components of magnetic moments, in contrast to normal fractional magnetization plateau phases. The magnetization was calculated using a simple spin model deduced from the above result. Finally we propose that frustration is the key to understanding the observed multi-step magnetization., Comment: 4 pages, 3 figures

We present a theoretical and experimental study on electronic and magneto-optical properties of p-type paramagnetic InMnAs dilute magnetic semiconductor alloys and ferromagnetic p-type InMnAs/(Al,Ga)Sb thin films in ultrahigh (> 100 T) external magnetic fields \textbf{B}. We use an 8 band Pidgeon-Brown model generalized to include the wavevector dependence of the electronic states along B as well as s-d and p-d exchange interactions with localized Mn d-electrons. In paramagnetic p-InMnAs alloys, we compute the spin-dependent electronic structure as a function of Mn doping and examine how the valence band structure depends on parameters such as the sp-d exchange interaction strength and effective masses. The cyclotron resonance (CR) and magneto-optical properties of InMnAs are computed using Fermi's golden rule. In addition to finding strong CR for hole-active polarization in p-type InMnAs, we also find strong CR for electron-active polarization. The electron-active CR in the valence bands results from transitions between light and heavy hole Landau levels and is seen in experiments. In ferromagnetic p-InMnAs/(Al,Ga)Sb, two strong CR peaks are observed which shift with position and increase in strength as the Curie temperature is approached from above. This transition takes place well above the Curie temperature and can be attributed to the increase in magnetic ordering at low temperatures., Comment: 15 pages, 17 figures

We report the first high-field x-ray diffraction experiment using synchrotron x-rays and pulsed magnetic fields exceeding 30 T. Lattice deformation due to a magnetic-field-induced valence transition in YbInCu4 is studied. It has been found that the Bragg reflection profile at 32 K changes significantly at around 27 T due to the structural transition. In the vicinity of the transition field the low-field and the high-field phases are observed simultaneously as the two distinct Bragg reflection peaks: This is a direct evidence of the fact that the field-induced valence state transition is the first order phase transition. The field-dependence of the low-field-phase Bragg peak intensity is found to be scaled with the magnetization., Comment: 5 pages, 6 figures, submitted to J. Phys. Soc. Jpn

We have carried out an ultrahigh-field cyclotron resonance study of p-type In1-xMnxAs films, with Mn composition x ranging from 0% to 2.5%, grown on GaAs by low-temperature molecular-beam epitaxy. Pulsed magnetic fields up to 500 T were used to make cyclotron resonance observable in these low-mobility samples. The clear observation of hole cyclotron resonance is direct evidence of the existence of a large number of itinerant, effective-mass-type holes rather than localized d-like holes. It further suggests that the p-d exchange mechanism is more favorable than the double exchange mechanism in this narrow gap InAs-based dilute magnetic semiconductor. In addition to the fundamental heavy-hole and light-hole cyclotron resonance absorption appearing near the high-magnetic-field quantum limit, we observed many inter-Landau-level absorption bands whose transition probabilities are stronglydependent on the sense of circular polarization of the incident light., Comment: 8 pages, 10 Postscript figures

Accurate determination of carrier densities in ferromagnetic semiconductors by Hall measurements is hindered by the anomalous Hall effect, and thus alternative methods are being sought. Here, we propose that cyclotron resonance (CR) is an excellent method for carrier density determination for InMnAs-based magnetic structures. We develop a theory for electronic and magneto-optical properties in narrow gap InMnAs films and superlattices in ultrahigh magnetic fields oriented along [001]. In n-type InMnAs films and superlattices, we find that the e-active CR peak field is pinned at low electron densities and then begins to shift rapidly to higher fields above a critical electron concentration allowing the electron density to be accurately calibrated. In p-type InMnAs, we observe two h-active CR peaks due to heavy and light holes. The lineshapes depend on temperature and line broadening. The light hole CR requires higher hole densities and fields. Analyzing CR lineshapes in p-films and superlattices can help determine hole densities., Comment: 4 pages, 4 figures

We report the observation of hole cyclotron resonance (CR) in InMnAs/(Al,Ga)Sb heterostructures in a wide temperature range covering both the paramagnetic and ferromagnetic phases. We observed two pronounced resonances that exhibit drastic changes in position, linewidth, and intensity at a temperature higher than the Curie temperature, indicating possible local magnetic ordering or clustering. We attribute the two resonances to the fundamental CR transitions expected for delocalized valence-band holes in the quantum limt. Using an 8-band {\bf k$\cdot$p} model, which incorporates ferromagnetism within a mean-field approximation, we show that the temperature-dependent CR peak shift is a direct measure of the carrier-Mn exchange interaction. Significant line narrowing was observed at low temperatures, which we interpret as the suppression of localized spin fluctuations., Comment: 4 pages, 5 figures

We present a theory for electronic and magneto-optical properties of n-type In(1-x)Mn(x)As magnetic alloy semiconductors in a high magnetic field, B. We use an 8-band Pidgeon-Brown model generalized to include the wavevector (Kz) dependence of the electronic states as well as s-d and p-d exchange interactions with localized Mn d-electrons. Calculated conduction-band Landau levels exhibit effective masses and g factors that are strongly dependent on temperature, magnetic field, Mn concentration (x), and Kz. Cyclotron resonance (CR) spectra are computed using Fermi's golden rule and compared with ultrahigh-magnetic-field (> 50 T) CR experiments, which show that the electron CR peak position is sensitive to x. Detailed comparison between theory and experiment allowed us to extract s-d and p-d exchange parameters, alpha and beta. we find that not only alpha but also beta affects the electron mass because of the strong interband coupling in this narrow gap semiconductor. In addition, we derive analytical expressions for the effective masses and g facors within the 8-band model. Results indicate that (alpha - beta) is the crucial parameter that determines the exchange interaction correction to the cyclotron masses. These findings sould be useful for designing novel devices based on ferromagnetic semiconductors., Comment: 19 pages, 13 figures

We report the first observation of hole cyclotron resonance (CR) in ferromagnetic InMnAs/GaSb heterostructures both in the high-temperature paramagnetic phase and the low-temperature ferromagnetic phase. We clearly resolve two resonances that exhibit strong temperature dependence in position, linewidth, and intensity. We attribute the two resonances to the so-called fundamental CR transitions expected for delocalized holes in the valence band in the magnetic quantum limit, demonstrating the existence of $p$-like itinerant holes that are describable within the Luttinger-Kohn effective mass theory., Comment: 3 figures. Proceedings of the 26th International Conference on the Physics of Semiconductors

We have carried out an ultrahigh field cyclotron resonance study of $n$-type In$_{1-x}$Mn$_x$As films, with Mn composition $x$ ranging from 0 to 12%, grown on GaAs by low temperature molecular beam epitaxy. We observe that the electron cyclotron resonance peak shifts to lower field with increasing $x$. A detailed comparison of experimental results with calculations based on a modified Pidgeon-Brown model allows us to estimate the {\em s-d} and {\em p-d} exchange coupling constants, $\alpha$ and $\beta$, for this important III-V dilute magnetic semiconductor system., Comment: 4 pages, 4 figures