arXiv subjects

H. Kageyama

Publications and source records attributed to H. Kageyama.

At least 19 recordsLinked to original sources

arXiv2023

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↗

arXiv2022

Local spin dynamics in geometrically frustrated Mo pyrochlore antiferromagnet Lu$_2$Mo$_2$O$_{5-y}$N$_2$

The magnetic ground state of oxynitride pyrochlore Lu$_2$Mo$_2$O$_{5-y}$N$_2$, a candidate compound for the quantum spin liquid ($S=1/2$, Mo$^{5+}$), was studied by muon spin rotation/relaxation experiment. In contrast to Lu$_2$Mo$_2$O$_7$ ($S=1$, Mo$^{4+}$) which exhibits the spin-glass behavior with a freezing temperature $T_g\simeq16$ K, no such spin freezing or long range magnetic order was observed down to 0.3 K. Moreover, two separate magnetic domains were detected below $\sim$13 K, which were characterized by differences in spin dynamics. The first is the "sporadic" spin fluctuation seen in frustrated antiferromagnets, where the amplitude of the hyperfine fields suggests that the excitation comprises a local cluster of unpaired spins. The other is rapid paramagnetic fluctuation, which is only weakly suppressed at low temperatures. In place of the paramagnetic fluctuation, the volume fraction for the sporadic fluctuation steadily increases with decreasing temperature, indicating the formation of an excitation gap with a broad distribution of the gap energy involving null gap.

cond-mat.str-el↗

arXiv2022

Intrinsic suppression of topological thermal Hall effect in an exactly solvable quantum magnet

In contrast to electron (fermion) systems, topological phases of charge neutral bosons have been poorly understood despite recent extensive research on insulating magnets. The most important unresolved issue is how the inevitable inter-bosonic interactions influence the topological properties. It has been proposed that the quantum magnet SrCu$_2$(BO$_3$)$_2$ with an exact ground state serves as an ideal platform for this investigation, as the system is expected to be a magnetic analogue of a Chern insulator with electrons replaced by bosonic magnetic excitations (triplons). Here, in order to examine topologically protected triplon chiral edge modes in SrCu$_2$(BO$_3$)$_2$, we measured and calculated the thermal Hall conductivity $κ_{xy}$. Our calculations show that the sign of $κ_{xy}$ is negative, which is opposite to the previous calculations, and its magnitude is 2$π$ times smaller. No discernible $κ_{xy}$ was observed, which is at most 20-30% of our calculations if present. This implies that even relatively weak inter-particle interactions seriously influence the topological transport properties at finite temperatures. These demonstrate that, in contrast to fermionic cases, the picture of non-interacting topological quasi-particles cannot be naively applied to bosonic systems, calling special attention to the interpretation of the topological bosonic excitations reported for various insulating magnets.

cond-mat.str-el↗

arXiv2017

Excited configurations of hydrogen in the BaTiO$_{3-x}$H$_x$ perovskite lattice associated with hydrogen exchange and transport

Excited configurations of hydrogen in the oxyhydride BaTiO$_{3-x}$H$_x$ ($x=0.1-0.5$), which are considered to be involved in its hydrogen transport and exchange processes, were investigated by positive muon spin relaxation ($μ^+$SR) spectroscopy using muonium (Mu) as a pseudoisotope of hydrogen. Muons implanted into the BaTiO$_{3-x}$H$_x$ perovskite lattice were mainly found in two qualitatively different metastable states. One was assigned to a highly mobile interstitial protonic state, which is commonly observed in perovskite oxides. The other was found to form an entangled two spin-$\frac{1}{2}$ system with the nuclear spin of an H$^-$ ion at the anion site. The structure of the (H,Mu) complex agrees well with that of a neutralized center containing two H$^-$ ions at a doubly charged oxygen vacancy, which was predicted to form in the SrTiO$_{3-δ}$ perovskite lattice by a computational study [Y. Iwazaki $et$ $al$., APL Materials 2, 012103 (2014)]. Above 100 K, interstitial Mu$^+$ diffusion and retrapping to a deep defect were observed, which could be a rate-limiting step of macroscopic Mu/H transport in the BaTiO$_{3-x}$H$_x$ lattice.

cond-mat.mtrl-sci↗

arXiv2014

Resonant Spin Wave Excitation by Terahertz Magnetic Near-field Enhanced with Split Ring Resonator

Excitation of antiferromagnetic spin waves in HoFeO$_{3}$ crystal combined with a split ring resonator (SRR) is studied using terahertz (THz) electromagnetic pulses. The magnetic field in the vicinity of the SRR induced by the incident THz electric field component excites and the Faraday rotation of the polarization of a near-infrared probe pulse directly measures oscillations that correspond to the antiferromagnetic spin resonance mode. The good agreement of the temperature-dependent magnetization dynamics with the calculation using the two-lattice Landau-Lifshitz-Gilbert equation confirms that the spin wave is resonantly excited by the THz magnetic near-field enhanced at the LC resonance frequency of the SRR, which is 20 times stronger than the incident magnetic field.

physics.optics↗

arXiv2013

Magnetization of SrCu2(BO3)2 in ultrahigh magnetic fields up to 118 T

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.

cond-mat.str-el↗

arXiv2013

S wave superconductivity in newly discovered superconductor BaTi$_2$Sb$_2$O revealed by $^{121/123}$Sb-NMR/Nuclear Quadrupole Resonance measurements

We report the $^{121/123}$Sb-NMR/nuclear quadrupole resonance (NQR) measurements on the newly-discovered superconductor BaTi$_2$Sb$_2$O with a two-dimensional Ti$_2$O square-net layer formed with Ti$^{3+}$ (3$d^1$). NQR measurements revealed that the in-plane four-fold symmetry is broken at the Sb site below $T_{\rm A} \sim$ 40 K, without an internal field appearing at the Sb site. These exclude a spin-density wave (SDW)/ charge density wave (CDW) ordering with incommensurate correlations, but can be understood with the commensurate CDW ordering at $T_{\rm A}$. The spin-lattice relaxation rate $1/T_1$, measured at the four-fold symmetry breaking site, decreases below superconducting (SC) transition temperature $T_{\rm c}$, indicative of the microscopic coexistence of superconductivity and the CDW/SDW phase below $T_{\rm A}$. Furthermore, $1/T_1$ of $^{121}$Sb-NQR shows a coherence peak just below $T_{\rm c}$ and decreases exponentially at low temperatures. These results are in sharp contrast with those in cuprate and iron-based superconductors, and strongly suggest that its SC symmetry is classified to an ordinary s-wave state.

cond-mat.supr-con↗

arXiv2010

Superfluid Density and Field-Induced Magnetism in Ba(Fe1-xCox)2As2 and Sr(Fe1-xCox)2As2 Measured with Muon Spin Relaxation

We report muon spin rotation ($μ$SR) measurements of single crystal Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ and Sr(Fe$_{1-x}$Co$_x$)$_2$As$_2$. From measurements of the magnetic field penetration depth $λ$ we find that for optimally- and over-doped samples, $1/λ(T\to 0)^2$ varies monotonically with the superconducting transition temperature T$_{\rm C}$. Within the superconducting state we observe a positive shift in the muon precession signal, likely indicating that the applied field induces an internal magnetic field. The size of the induced field decreases with increasing doping but is present for all Co concentrations studied.

cond-mat.supr-con↗

arXiv2010

Ferromagnetically coupled Shastry-Sutherland quantum spin singlets in (CuCl)LaNb$_2$O$_7$

Using inelastic neutron scattering, x-ray, neutron diffraction, and the first-principle calculation techniques, we show that the crystal structure of the two-dimensional quantum spin system (CuCl)LaNb$_2$O$_7$ is orthorhombic with $Pbam$ symmetry in which CuCl$_4$O$_2$ octahedra are tilted from their high symmetry positions and the Cu$^{2+} (s = 1/2)$ ions form a distorted square lattice. The dominant magnetic interactions are the fourth nearest neighbor antiferromagnetic interactions with a Cu-Cl--Cl-Cu exchange path, which lead to the formation of spin singlets. The two strongest interactions between the singlets are ferromagnetic, which makes (CuCl)LaNb$_2$O$_7$ the first system of ferromagnetically coupled Shastry-Sutherland quantum spin singlets.

cond-mat.str-el↗

arXiv2009

$μ$SR studies of the frustrated quasi-2d square-lattice spin system Cu(Cl,Br)La(Nb,Ta)$_{2}$O$_{7}$: evolution from spin-gap to antiferromagnetic state

We report muon spin relaxation ($μ$SR) and magnetic susceptibility measurements on Cu(Cl,Br)La(Nb,Ta)$_{2}$O$_{7}$, which demonstrate: (a) the absence of static magnetism in (CuCl)LaNb$_{2}$O$_{7}$ down to 15 mK confirming a spin-gapped ground state; (b) phase separation between partial volumes with a spin-gap and static magnetism in (CuCl)La(Nb,Ta)$_{2}$O$_{7}$; (c) history-dependent magnetization in the (Nb,Ta) and (Cl,Br) substitution systems; (d) a uniform long-range collinear antiferromagnetic state in (CuBr)LaNb$_{2}$O$_{7}$; and (e) a decrease of Néel temperature with decreasing Br concentration $x$ in Cu(Cl$_{1-x}$Br$_{x}$)LaNb$_{2}$O$_{7}$ with no change in the ordered Cu moment size for $0.33 \leq x \leq 1$. Together with several other $μ$SR studies of quantum phase transitions in geometrically-frustrated spin systems, the present results reveal that the evolution from a spin-gap to a magnetically ordered state is often associated with phase separation and/or a first order phase transition.

cond-mat.str-el↗

arXiv2008

Antiferromagnetic Nuclear Resonance in the Quasi-Two-Dimensional (CuBr)LaNb2O7

We report nuclear magnetic resonance (NMR) studies in the antiferromagnetic state of the quasi-two-dimensional (CuBr)LaNb2O7. The NMR spectra at zero magnetic field and 4.2 K indicate a unique Cu and Br sites with an internal field of 5.7 T (at Cu) and 16.4 T (at Br), confirming a magnetic order. For the large internal field at the Br sites to be compatible with the collinear antiferromagnetic order observed by neutron diffraction experiments (N. Oba et al., J. Phys. Soc. Jpn. 75, (2006) 113601), the Br atoms must move significantly off the center of the square of the Cu sublattice so that the Br nuclei couple predominantly to two parallel Cu moments. While invalidating the frustrated J1-J2 model defined on a C4-symmetric square lattice, our results are compatible with the structural model proposed for (CuCl)LaNb2O7 by Yoshida et al. (J. Phys. Soc. Jpn. 76 (2007) 104703).

cond-mat.str-el↗

arXiv2008

Superconductivity coexisting with phase-separated static magnetic order in (Ba,K)Fe$_{2}$As$_{2}$, (Sr,Na)Fe$_{2}$As$_{2}$ and CaFe$_{2}$As$_{2}$

The recent discovery and subsequent developments of FeAs-based superconductors have presented novel challenges and opportunities in the quest for superconducting mechanisms in correlated-electron systems. Central issues of ongoing studies include interplay between superconductivity and magnetism as well as the nature of the pairing symmetry reflected in the superconducting energy gap. In the cuprate and RE(O,F)FeAs (RE = rare earth) systems, the superconducting phase appears without being accompanied by static magnetic order, except for narrow phase-separated regions at the border of phase boundaries. By muon spin relaxation measurements on single crystal specimens, here we show that superconductivity in the AFe$_{2}$As$_{2}$ (A = Ca,Ba,Sr) systems, in both the cases of composition and pressure tunings, coexists with a strong static magnetic order in a partial volume fraction. The superfluid response from the remaining paramagnetic volume fraction of (Ba$_{0.5}$K$_{0.5}$)Fe$_{2}$As$_{2}$ exhibits a nearly linear variation in T at low temperatures, suggesting an anisotropic energy gap with line nodes and/or multi-gap effects.

cond-mat.supr-con↗

arXiv2008

NMR evidence for the persistence of spin-superlattice above the 1/8 magnetization plateau in SrCu2(BO3)2

We present 11B NMR studies of the 2D frustrated dimer spin system SrCu2(BO3)2 in the field range 27-31 T covering the upper phase boundary of the 1/8 magnetization plateau, identified at 28.4 T. Our data provide a clear evidence that above 28.4 T the spin-superlattice of the 1/8 plateau is modified but does not melt even though the magnetization increases. Although this is precisely what is expected for a supersolid phase, the microscopic nature of this new phase is much more complex. We discuss the field-temperature phase diagram on the basis of our NMR data.

cond-mat.str-el↗

arXiv2007

Field dependence of the quantum ground state in the Shastry-Sutherland system SrCu$_2$(BO$_3$)$_2$

We present magnetic torque measurements on the Shastry-Sutherland quantum spin system SrCu$_2$(BO$_3$)$_2$ in fields up to 31 T and temperatures down to 50 mK. A new quantum phase is observed in a 1 T field range above the 1/8 plateau, in agreement with recent NMR results. Since the presence of the DM coupling precludes the existence of a true Bose-Einstein condensation and the formation of a supersolid phase in SrCu$_2$(BO$_3$)$_2$, the exact nature of the new phase in the vicinity of the plateau remains to be explained. Comparison between magnetization and torque data reveals a huge contribution of the Dzyaloshinskii-Moriya interaction to the torque response. Finally, our measurements demonstrate the existence of a supercooling due to adiabatic magnetocaloric effects in pulsed field experiments.

cond-mat.str-el↗

arXiv2007

Magnetic and Structural Studies of the Quasi-Two-Dimensional Spin-Gap System (CuCl)LaNb2O7

We report magnetization, nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and transmission electron microscopy (TEM) studies on the quasi-two-dimensional spin-gap system (CuCl)LaNb2O7, a possible candidate for the J1-J2 model on a square lattice. A sharp single NQR line is observed at the Cu and Cl sites, indicating that both Cu and Cl atoms occupy a unique site. However, the electric field gradient tensors at the Cu, Cl, and La sites do not have axial symmetry. This is incompatible with the reported crystal structure. Thus the J1-J2 model has to be modified. We propose alternative two-dimensional dimer models based on the NMR, NQR, and TEM results. The value of the hyperfine coupling constant at the Cu sites indicates that the spin density is mainly on the d(3z2-r2) orbital (z parallel c). At 1.5 K, Cu- and Nb-NMR signals disappear above the critical field Bc1 = 10.3 T determined from the onset of the magnetization, indicating a field-induced magnetic phase transition at Bc1.

cond-mat.str-el↗

arXiv2007

Impurity-induced singlet breaking in SrCu2(BO3)2

We have performed $μ$SR studies on single crystals of SrCu$_2$(BO$_3$)$_2$, a quasi-two-dimensional spin system with a spin singlet ground state. We observe two different muon sites which we associate with muons located adjacent to the two inequivalent O sites. One site, presumed to be located in the Cu-O-Cu superexchange path, exhibits a large increase in the frequency shift with decreasing temperature which is unaffected by the singlet formation, indicating that the muon has locally broken the singlet bond. We have also performed $μ$SR on single crystals of SrMg$_{0.05}$Cu$_{1.95}$(BO$_3$)$_2$, Sr$_{0.96}$La$_{0.04}$Cu$_2$(BO$_3$)$_2$, and Sr$_{0.95}$Na$_{0.05}$Cu$_2$(BO$_3$)$_2$. We have found that the frequency shifts of these doped samples are equivalent and contain three branches at low temperatures. Two of these branches map on to the branches observed in the pure sample reasonably well and so we attribute the third branch to effect of the dopants. Specifically, this third branch represents the case when the muon sits at a site in the superexchange path lacking a corresponding singlet, due to it already being broken as a result of doping. This then leads to the conclusion that singlets are broken in this system when it is doped both in and out of the CuBO$_3$ planes.

cond-mat.str-el↗

arXiv2005

Symmetry and light coupling to phononic and collective magnetic excitations in SrCu_2(BO_3)_2

We perform a low temperature Raman scattering study of phononic and collective spin excitations in the orthogonal dimers compound SrCu_2(BO_3)_2, focussing on the symmetry and the effects of external fields on the magnetic modes. The zero field symmetry and the behavior in magnetic fields of the elementary and bound magnetic triplet states are experimentally determined. We find that a minimal 4-spin cluster forming the unit cell is able to describe the symmetry as well as the anisotropic dispersions in external fields of the spin gap multiplet branches around 24 cm^{-1}. We identify two Raman coupling mechanisms responsible for the distinct resonance behavior of these magnetic modes and we show that one of these can be ascribed to an effective intra-dimer Dzyaloshinskii-Moriya spin interaction. Our data also suggest a possible explanation for the existence of a strongly bound two-triplet state in the singlet sector which has an energy below the spin gap. The low temperature phononic spectra suggest strong spin-phonon coupling and show intriguing quasi-degeneracy of modes in the context of the present crystal structure determination.

cond-mat.str-el↗

arXiv2005

Field-Induced Effects of Anisotropic Magnetic Interactions in SrCu2(BO3)2

We observed a field-induced staggered magnetization in the 2D frustrated dimer-singlet spin system SrCu2(BO3)2 by 11B NMR, from which the magnitudes of the intradimer Dzyaloshinsky-Moriya interaction and the staggered g-tensor were determined. These anisotropic interactions cause singlet-triplet mixing and eliminate a quantum phase transition at the expected critical field Hc for gap closing. They also provide a quantitative account for some puzzling phenomena such as the onset of a uniform magnetization below the and the persistence of the excitation gap above Hc. The gap was accurately determined from the activation energy of the nuclear relaxation rate.

cond-mat.str-el↗