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Masaki Gen

Publications and source records attributed to Masaki Gen.

At least 19 recordsLinked to original sources

Tetrahedrally ferromagnetic correlations and a glassy-freezing anomaly in the breathing pyrochlore magnet $\mathrm{AgInCr_4S_8}$ with partial $A$-site disorder

We investigate the chromium breathing pyrochlore sulfide $\mathrm{AgInCr_4S_8}$, a chromium-based thiospinel, by synchrotron x-ray and neutron powder diffraction, dc magnetization, and heat capacity. Diffraction confirms the $F\bar{4}3m$ breathing structure with alternating large and small $\mathrm{Cr_4}$ tetrahedra, a large breathing ratio ($d^\prime/d = 1.106$ at 300 K), and substantial Ag/In intermixing on the $A$ sublattice ($\sim 16\%$). No structural transition or magnetic Bragg peaks are detected down to 1.5 K. An enlarged low-angle difference plot between the 1.5 and 20 K neutron diffraction patterns shows a weak broad diffuse-like enhancement, consistent with short-range or frozen correlated moments within the sensitivity of the present data. Susceptibility yields a positive Weiss temperature $\theta_{\mathrm{W}} = +92$ K and a moment enhancement in 30--60 K, while the magnetic entropy released by $\sim 30$ K approaches a scale of order $R\ln 13$, together consistent with the development of short-range tetrahedral ferromagnetic correlations and an effective $S = 6$ cluster-moment picture. A broad susceptibility cusp with ZFC--FC bifurcation and a low-temperature specific heat anomaly near 9 K indicate a phenomenological glassy-freezing anomaly without long-range order. $\mathrm{AgInCr_4S_8}$ provides a benchmark for the interplay of strong breathing distortion and quenched $A$-site disorder in chromium breathing pyrochlores.

cond-mat.str-el

Magnetoelastic mapping of the high-field phase diagram in the topological cubic helimagnet SrFeO$_{3}$

The cubic perovskite SrFeO$_{3}$ is a prototypical centrosymmetric itinerant magnet that hosts a quadruple-${\mathbf Q}$ hedgehog-antihedgehog lattice and exhibits a complex magnetic-field-temperature phase diagram. Yet, the microscopic mechanism underlying the emergence of its versatile multiple-${\mathbf Q}$ phases remains unresolved. Here, we reveal the field-orientation dependence of the magnetic phase diagram and establish an effective spin Hamiltonian for SrFeO$_{3}$ that incorporates a cubic single-ion anisotropy together with bilinear and biquadratic interactions in momentum space, which originate from the spin-charge coupling. In addition, we observe magnetoelastic signatures of a redistribution of the ligand-hole density upon entering the forced ferromagnetic phase. These findings emphasize the pivotal importance of electronic itinerancy arising from the formation of a ligand-hole band in stabilizing multiple-${\mathbf Q}$ phases.

cond-mat.str-el

Frustration of harmonic and solitonic helimagnetism on the body-centered tetragonal lattice of GdAlSi

The triangular lattice antiferromagnet (TLAF) with nearest-neighbor exchange interaction is a model platform in the field of frustrated magnetism. Here, anharmonic (`up-up-down') and harmonic (`120 degree') magnetic states compete, because the fundamental helimagnetic wave and its higher harmonic are degenerate in energy. We show that a body-centered tetragonal lattice (BCTL) can realize a similar frustration of harmonic and anharmonic helimagnetic states, and that the tetragonal magnetic Weyl semimetal GdAlSi realizes this scenario. In an applied magnetic field, resonant elastic X-ray scattering reveals a competition of harmonic cycloidal and solitonic double-Q states, well consistent with mean-field calculations. Our work provides a new paradigm for frustration physics in BCTL materials.

cond-mat.str-el

Magnetocaloric effect measurements in ultrahigh magnetic fields up to 120 T

We report proof-of-concept measurements of the magnetocaloric effect (MCE) in ultrahigh magnetic fields up to 120 T for the classical spin-ice compound Ho$_{2}$Ti$_{2}$O$_{7}$. Radio-frequency resistivity measurements using an Au$_{16}$Ge$_{84}$ thin-film thermometer enable us to detect a rapid change in the sample temperature associated with a crystal-field level crossing in the high-field region in addition to a giant MCE at low fields. We discuss a possible delay in the temperature response and outline prospects for more precise MCE measurements in destructive pulsed fields.

cond-mat.str-el

Effect of uniaxial stress on helimagnetic phases in the square-lattice itinerant magnet EuAl$_{4}$

We investigate uniaxial-stress effects on the magnetic phase diagram of the square-lattice itinerant magnet EuAl$_{4}$, where strong coupling among spin, lattice, and charge produces a variety of helimagnetic phases, including rhombic and square skyrmion lattices. Combining resistivity and magnetization measurements with neutron scattering, we find that compressive stresses of only several tens of megapascal along [010] enhance antiferromagnetic character and shorten the magnetic modulation period in the lowest-temperature single-Q spiral state, thereby driving the critical temperatures and fields of multiple phases to higher values. First-principles calculations show that increasing orthorhombic lattice distortion deforms the Fermi surface relevant to the magnetism, providing compelling evidence that Fermi-surface nesting plays a crucial role in stabilizing the helical magnetic modulations in EuAl$_{4}$.

cond-mat.str-el

Unified Description of Spin-Lattice Coupling and Thermodynamics in the Pyrochlore Heisenberg Antiferromagnet

We study an extended model to describe the spin-lattice coupling, incorporating individual vibrations of bonds and atomic sites alongside distance-dependent exchange interactions. The proposed spin Hamiltonian can be effectively considered as an interpolation between two well-established minimum models, the bond-phonon model and the site-phonon model. The extended model, which treats bond phonons and site phonons on comparable footing, well reproduces successive field-induced phase transitions as well as the thermodynamic properties of a three-up-one-down state in the pyrochlore-lattice Heisenberg antiferromagnet, including negative thermal expansion, an enhanced magnetocaloric effect, and a sharp specific-heat peak. The present approach is broadly applicable to various spin models, providing a framework for identifying the primary phonon modes responsible for spin-lattice coupling and for understanding complex magnetic phase diagrams.

cond-mat.str-el

X-ray free-electron laser observation of giant and anisotropic magnetostriction in $\beta$-O$_{2}$ at 110 Tesla

In strong magnetic fields beyond 100 T, the significant Zeeman energy competes with the lattice interactions, where a considerable magnetostriction is expected. However, the microscopic observation of the magnetostriction above 100 T has been hindered due to the short pulse duration of $\mu$-seconds and the coil's destruction. Here, we report the observation of the giant and anisotropic magnetostriction of $\sim 1$ % at 110 T in the spin-controlled crystal, $\beta$-O$_{2}$, by combining the single-shot diffraction of x-ray free-electron laser (XFEL) and the newly developed portable 100 T generator (PINK-02). The very soft and anisotropic response of $\beta$-O$_{2}$ should originate in the competing van der Waals force and exchange interaction, and also the frustration of spin and lattice on the triangular network. The XFEL experiment above 100 T using PINK-02 enables microscopic investigations on materials' properties at high magnetic fields, providing insights into how spins contribute to the stability of crystal structures.

cond-mat.str-el

Triangular lattice magnet GdGa$_2$ with short-period spin cycloids and possible skyrmion phases

The two-dimensional triangular lattice (TAL) is a model system of magnetic frustration and competing interactions, where skyrmion spin vortices can be induced by a vertical magnetic field $B$. We target the binary compound GdGa$_2$ with an undistorted TAL of Gd$^{3+}$ Heisenberg moments. At higher temperature ($T > 5$ K, $B = 0$, phase II), we reveal the cycloidal spin textures in GdGa$_2$ via resonant elastic X-ray scattering (REXS). Further, a transition with strong magneto-elastic response occurs when cooling into the zero-field ground state ($T < 5$ K, phase I). We also report the thermodynamic phase boundaries of $B$-induced magnetic A-phases, which are suppressed by an in-plane magnetic field and which have enhanced resistivity due to the partial opening of a charge gap. In analogy to Gd$_2$PdSi$_3$ and GdRu$_2$Si$_2$, these phases may represent a superposition of various cycloids, possibly a N\'eel skyrmion lattice. Our work lays the basis for further studies of the magnetic phase diagram of GdGa$_2$.

cond-mat.str-el

Perfectly harmonic spin cycloid and multi-$Q$ textures in the Weyl semimetal GdAlSi

A fundamental question concerns how topological electronic states are influenced by many-body correlations, and magnetic Weyl semimetals represent an important material platform to address this problem. However, the magnetic structures realized in these materials are limited, and in particular, no clear example of an undistorted helimagnetic state has been definitively identified. Here, we report clear evidence of a harmonic helimagnetic cycloid with an incommensurate magnetic propagation vector in the Weyl semimetal GdAlSi via resonant elastic X-ray scattering, including rigorous polarization analysis. This cycloidal structure is consistent with the Dzyaloshinskii-Moriya (DM) interaction prescribed by the polar crystal structure of GdAlSi. Upon applying a magnetic field, the cycloid undergoes a transition to a novel multi-$Q$ state. This field-induced, noncoplanar texture is consistent with our numerical spin model, which incorporates the DM interaction and, crucially, anisotropic exchange. The perfectly harmonic Weyl helimagnet GdAlSi serves as a prototypical platform to study electronic correlation effects in periodically modulated Weyl semimetals.

cond-mat.str-el

Electronic Structure of Kramers Nodal-Line Semimetal YAuGe and Anomalous Hall Effect Induced by Magnetic Rare-Earth Substitution

Nodal-line semimetals are a class of topological materials hosting one dimensional lines of band degeneracy. Kramers nodal-line (KNL) metals/semimetals have recently been theoretically recognized as a class of topological states inherent to all non-centrosymmetric achiral crystal lattices. We investigate the electronic structure of candidate KNL semimetal YAuGe by angle-resolved photoemission spectroscopy (ARPES) and quantum oscillations as well as by density functional theory (DFT) calculations. DFT has revealed that YAuGe hosts KNLs on the G-A-L-M plane of the Brillouin zone, that are protected by the time reversal and mirror-inversion symmetries. Through ARPES and quantum oscillations we identify signatures of hole bands enclosing the G point, and the observed splitting of quantum oscillation frequency with angle is attributed to spin-orbit-coupling-induced band splitting away from the KNLs. Furthermore, we show that the degeneracy of the nodal lines along the G-A line is lifted by the time-reversal-symmetry breaking when the Y is substituted by magnetic R ions (R = rare earth). This becomes a source of Berry curvature and contributes to the anomalous Hall effect in magnetic RAuGe. These findings establish RAuGe as a new class of KNL semimetals offering significant potential for engineering of anomalous magnetotransport properties via magnetic rare-earth substitution.

cond-mat.mtrl-sci

Magnetization process of a quasi-two-dimensional quantum magnet: Two-step symmetry restoration and dimensional reduction

We report on a comprehensive thermodynamic study of a quasi-two-dimensional (quasi-2D) quantum magnet Cu$_2$(OH)$_3$Br which in the 2D layer can be viewed as strongly coupled alternating antiferromagnetic and ferromagnetic chains. In an applied magnetic field transverse to the ordered spins below $T_N=9.3$ K, a field-induced phase transition from the 3D ordered to a disordered phase occurs at $B_c=16.3$ T for the lowest temperature, which is featured by an onset of a one-half plateau-like magnetization. By performing quantum Monte Carlo simulations of the relevant 2D model, we find that the plateau-like magnetization corresponds to a partial symmetry restoration and the full polarization in the ferromagnetic chains. Our numerical simulations also show that the magnetization saturation occurs with full symmetry restoration at a much higher field of $B_s \simeq 95$ T, corresponding to a 1D quantum phase transition in the antiferromagnetic chains. We argue that the experimentally observed field-induced phase transition at $B_c$ follows from the partial symmetry restoration and the concomitant dimensional reduction.

cond-mat.str-el

Crystal-field magnetostriction of the spin ice under ultrahigh magnetic fields

We present a comprehensive study of the magnetoelastic properties of the Ising pyrochlore oxide Ho$_{2}$Ti$_{2}$O$_{7}$, known as spin ice, by means of high-field magnetostriction measurements and numerical calculations. When a magnetic field is applied along the crystallographic <111> axis, the longitudinal magnetostriction exhibits a broad maximum in the low-field regime around 30 T, followed by a dramatic lattice contraction due to crystal-field (CF) level crossing at $B_{\rm cf} \sim 65$ T. The transverse magnetostriction exhibits a contrasting behavior, highlighting the anisotropic nature of the CF striction. We identify distinct timescales of spin dynamics and CF-phonon dynamics by applying a magnetic field with different field-sweep rates. Our mean-field calculations, based on a point-charge model, successfully reproduce the overall magnetostriction behavior, revealing the competition between the exchange striction and CF striction. A signature of the CF level crossing is also observed through adiabatic magnetocaloric-effect measurements, consistent with our magnetostriction data.

cond-mat.str-el

Contrasting magnetothermal conductivity in sibling Co-based honeycomb-lattice antiferromagnets

Honeycomb-lattice antiferromagnets have attracted wide attention for exploration of exotic heat transport and their interplay with magnetic excitations. In this work, we have revealed a contrasting behavior in the magneto-thermal conductivity (MTC) between two Co-based honeycomb-lattice magnets Co4M2O9 (M = Nb, Ta), despite their identical lattice structures and quite similar magnetism. Co4Ta2O9 exhibits enhanced MTC of about 550% at 9 T of an in-plane magnetic field, comparable to other honeycomb-magnets, while MTC for Co4Nb2O9 reaches only ~30%. This marked difference is ascribed to distinct features in the field-induced evolution of magnetic excitations that resonantly scatter phonons. This finding sheds light on implicit impacts of non-magnetic ions on thermal transport, and hints at the potential for broad heat-transport tunability while preserving magnetism and lattice structures.

cond-mat.str-el

Spin-lattice-coupled helical magnetic order in breathing pyrochlore magnets, CuAlCr$_{4}$S$_{8}$ and CuGaCr$_{4}$S$_{8}$

We report low-temperature powder X-ray and neutron diffraction studies on breathing pyrochlore magnets Cu$M$Cr$_{4}$S$_{8}$ ($M$ = Al, Ga), which undergo a magnetic transition at $T_{\rm N} \approx$ 21 and 31 K for {$M$ = Al and Ga, respectively. X-ray diffraction reveals that the magnetic transition accompanies a structural transition from cubic $F{\overline 4}3m$ to polar orthorhombic $Imm2$ symmetry for both the compounds, with larger distortion observed for $M$ = Ga at low temperatures. Neutron diffraction reveals incommensurate magnetic modulation ${\mathbf Q} = (q_{\rm IC}, 0.5, 0)$ in the orthorhombic setting, where $q_{\rm IC} \approx$ 0.39 and 0.31 for $M$ = Al and Ga, respectively. Our magnetic-structure analysis suggests cycloid-type magnetic order but not proper-screw type for both the compounds. We find strong correlation between the local spin configuration and Cr-Cr bond lengths, indicating that the spin-lattice coupling as well as the magnetic frustration play an important role in determining the ground state. Cu$M$Cr$_{4}$S$_{8}$ potentially offers a platform to explore magnetoelectric effects arising from the helimagnet driven electric polarity.

cond-mat.mtrl-sci

Metamagnetism and anomalous magnetotransport properties in rare-earth-based polar semimetals $R$AuGe ($R =$ Dy, Ho, and Gd)

We report the magnetic, magnetoelastic, and magnetotransport properties of single crystals of polar magnets $R$AuGe ($R=$ Dy, Ho, and Gd), grown by Au-Ge self-flux. Magnetization and magnetostriction measurements reveal multi-step metamagnetic transitions for the $c$-axis magnetic field ($H\parallel c$) for DyAuGe and HoAuGe, suggesting magnetic frustration in the triangular lattice of $R$ ions. The magnetic phase diagrams have clarified a close connection between the magnetoelastic property and the emergence of the intermediate metamagentic phase. The magnetic-field dependence of the resistivity and Hall resistivity reveal the semimetallic transport dominated by hole-type carriers, consistent with the behavior in a nonmagnetic analogue YAuGe. We also identify a signature of an anomalous Hall effect (AHE) proportional to the field-induced magnetization in $R=$ Dy, Ho, and Gd. GdAuGe shows magnetic and transport behavior as reported in a previous study using Bi-flux grown single crystals, while the self-flux grown crystal shows larger magnetoresistance ($\sim$ 345\%, at 1.8 K and 9 T) due to higher hole-type carrier mobility ($\sim$ 6400 cm$^2$/Vs). Using the two-band model analysis considering the mobility change during the magnetization process, we extract the anomalous Hall conductivity: $\sim 1200$ S/cm and $\sim 530$ S/cm for $R=$ Dy and Ho, respectively, at 1.8 K with 9 T for $H\parallel c$. The magnitude of conductivity suggests a contribution of intrinsic origin, possibly related to the Berry curvature in the electron bands induced by the time-reversal symmetry breaking and the polar lattice.

cond-mat.str-el

Incommensurate broken helix induced by nonstoichiometry in the axion insulator candidate EuIn$_{2}$As$_{2}$

Zintl phase EuIn$_{2}$As$_{2}$ has garnered growing attention as an axion insulator candidate, triggered by the identification of a commensurate double-${\mathbf Q}$ broken-helix state in previous studies, however, its periodicity and symmetry remain subjects of debate. Here, we perform resonant x-ray scattering experiments on EuIn$_{2}$As$_{2}$, revealing an incommensurate nature of the broken-helix state, where both the wave number and the amplitude of the helical modulation exhibit systematic sample dependence. Furthermore, the application of an in-plane magnetic field brings about a fanlike state that appears to preserve the double-${\mathbf Q}$ nature, which might be attributed to multiple-spin interactions in momentum space. We propose that the itinerant character of EuIn$_{2}$As$_{2}$, most likely induced by Eu deficiency, gives rise to the helical modulation and impedes the realization of a theoretically-predicted axion state with the collinear antiferromagnetic order.

cond-mat.str-el

Canted antiferromagnetism in a spin-orbit coupled $S_{\text{eff}} = 3/2$ triangular-lattice magnet DyAuGe

Exploration of nontrivial magnetic states induced by strong spin-orbit interaction is a central topic of frustrated magnetism. Extensive studies are concentrated on rare-earth-based magnets and 4d/5d transition metal compounds, which are mostly described by an effective spin $S_{\text{eff}} = 1/2$ for the Kramers doublet of the lowest crystal-electric-field levels. Variety of magnetic orderings may be greatly enhanced when magnetic dipolar moments intertwined with multipolar degrees of freedom which are described by higher-rank tensors and often require the magnetic ions with $S_{\text{eff}} > 1/2$. Here, our synchrotron x-ray diffraction near the Dy $L_3$ edge has unveiled a canted antiferromagnetic ground state arising from a quasi-quartet ($S_{\text{eff}} = 3/2$) of 4f electrons in a triangular-lattice (TL) rare-earth intermetallics DyAuGe. Magnetic moment and electric-quadrupole moment are closely interlocked and noncollinear magnetic-dipole alignment is induced by antiferroic electric-quadrupole (AFQ) ordering in the TL layers. The correlation between the AFQ and canted magnetic structures is further confirmed by phase transitions in an in-plane magnetic field. These findings offer insights into the emergence of nontrivial magnetic states in frustrated TL systems described beyond the $S_{\text{eff}} = 1/2$.

cond-mat.str-el

Cluster rearrangement by chiral charge order in lacunar spinel GaNb$_4$Se$_8$

Transition-metal atoms with d electrons sometimes form clusters in crystals, which significantly affects the physical properties. Such a cluster formation frequently accompanies a change in the crystal system, leading to the presence of domains with different crystal orientations. In particular, the cubic symmetry is rarely retained after the cluster formation. Here, we identify a cubic-to-cubic phase transition in lacunar spinel GaNb$_4$Se$_8$, where the change in the lattice parameter is less than 0.0001%. Each Nb$^{3.25+}$ tetramer with seven 4d electrons is distorted into a Nb$^{3+}$ trimer and a Nb$^{4+}$ monomer induced by charge disproportionation among Nb ions. While the Nb$^{3+}$ trimer with six 4d electrons forms spin-singlets in the sigma-bonding orbitals for three Nb-Nb bonds, a localized S=1/2 spin remains on the Nb$^{4+}$ ion. Furthermore, a local electric dipole moment is induced along the three-fold rotation axis of each distorted tetramer by the cluster rearrangement. The electric dipole moments are regularly arranged to maintain the cubic symmetry, giving rise to chiral order.

cond-mat.str-el