arXiv subjects

Ryuji Tamura

Publications and source records attributed to Ryuji Tamura.

At least 19 recordsLinked to original sources

arXiv2026

Breakdown of Universal Whirling Order in a Heisenberg Tsai-Type Approximant

Noncoplanar whirling magnetic order has recently been proposed as a universal magnetic state in non-Heisenberg Tsai-type quasicrystal approximants. Here, X-ray resonant magnetic scattering measurements on Heisenberg and non-Heisenberg Au-Al-R (R = Gd, Tb) 1/1 approximants reveal a clear breakdown of this universality in the Heisenberg limit. While the non-Heisenberg Au-Al-Tb system is well described by the previously identified whirling magnetic structure, the Heisenberg Au-Al-Gd counterpart exhibits qualitatively different azimuthal-angle dependences that are incompatible with the universal whirling-order model. Despite nearly identical crystal structures and comparable magnetic energy scales, the two systems stabilize distinct antiferromagnetic ground states with the same propagation vector k = (1, 0, 0), demonstrating that the apparent universality of whirling order is not a consequence of Tsai-cluster geometry alone but requires spin anisotropy. These results further reveal the emergence of a competing manifold of nearly degenerate magnetic states in the Heisenberg limit.

cond-mat.str-el↗

arXiv2026

Magnetic ground state of a prototype quasicrystal approximant: a candidate for octahedral spin ice physics

Magnetic ordering in quasicrystals has recently emerged as a fertile ground for discovering unconventional magnetic states beyond the framework of periodic crystals. However, elucidating the microscopic origin of such states remains challenging due to the intrinsic aperiodicity of quasicrystals. Here, we address this issue by investigating the prototypical Tsai-type quasicrystal approximant Cd6Tb, which preserves the essential local geometry and connectivity of icosahedral quasicrystals while allowing detailed structural and magnetic characterization due to its translational periodicity. Using neutron diffraction measurements, we find a noncoplanar multi-k magnetic ground state composed of Ising-like Tb moments arranged on a network of corner-sharing octahedra, the ingredients required to host octahedral spin-ice physics. Remarkably, only one third of the Tb moments develop long-range magnetic order, whereas the remaining moments display strongly reduced static order accompanied by persistent spin dynamics on microsecond timescales, as evidenced by muon spin rotation. This coexistence of ordered and fluctuating moments constitutes a potential realization of magnetic fragmentation - a key prediction of octahedral spin-ice physics - in a quasicrystal-related material.

cond-mat.str-el↗

arXiv2025

Soft and hard x-ray orbital-resolved photoemission study of a strongly correlated Cd-Ce quasicrystal approximant

We have investigated the orbital-dependent electronic states of Cd6Ce, a prototype of strongly correlated rare-earth-based Tsai-type quasicrystals and approximants (ACs) by soft and hard x-ray photoemission spectroscopy. Our results reveal that the 4f orbitals are predominantly hybridized with the valence-band electrons far from the Fermi level (EF), in sharp contrast to the hybridization with conduction electrons at EF seen for the intermetallic Ce-based compounds. This anomalous hybridization should be taken into account in discussing the unresolved magnetic ground state in Cd6Ce. These findings suggest that Cd-based ACs, some of which show the multi-step magnetic transitions, could provide a new platform for investigating novel magnetic properties that cannot be understood within the conventional framework of hybridization at EF.

cond-mat.str-el↗

arXiv2025

Derivation of a non-stoichiometric 1/1 quasicrystal approximant from a stoichiometric 2/1 quasicrystal approximant and maximization of magnetocaloric effect

The present research introduces a novel strategy for tuning magnetic properties by overcoming the compositional limitation of stoichiometric intermetallic compounds via extension of their stability into a new dimension within valence electron-per-atom (e/a) parameter space. Focusing on approximant crystals (ACs), a "double hetero-valent elemental substitution" is employed in a stoichiometric Ga-Pt-Gd 2/1 AC whereby e/a is lowered from 1.92 to 1.60. Through this approach a new family of stable Ga-based Tsai-type 1/1 ACs with exceptionally wide composition stability within e/a space is derived. Remarkably, magnetic ground state is altered from initially spin-glass to ferromagnetic (FM) with second order phase transition and mean-field-like critical behavior. More importantly, through this strategy, the isothermal magnetic entropy change enhanced significantly and reached a maximum value of -8.7 J/K mol-Gd under a 5 T magnetic field change, even comparable to leading rare-earth magnetocaloric materials including RCo2 phases. These findings demonstrate the high potential of a double hetero-valent elemental substitution for tailoring magnetic properties and magnetocaloric response in stoichiometric compounds, offering a new pathway for designing high-performance magnetic refrigeration materials even beyond the quasicrystals and ACs.

cond-mat.mtrl-sci↗

arXiv2025

Anomalous magnetic response in the Au-Al-Gd 1/1 quasicrystal approximant

The magnetic response of the Tsai-type 1/1 Au-Al-Gd approximant crystals (ACs) was quantitatively investigated in terms of the magnetic entropy change ($\Delta S_{M}$) for different magnetic ground states. A comprehensive $\Delta S_{M}$ map over a wide electron concentration range has been established, demonstrating the detailed variation of $\Delta S_{M}$ across the entire magnetic phase diagram in the Tsai-type 1/1 ACs. Near the boundaries of the ferromagnetic (FM) phase, a clear deviation from the mean-field theory (MFT) was observed in both the Curie temperature ($T_{C}$) and magnetic field ($H$) dependences of the maximum magnetic entropy change ($\Delta S_{M}^{max}$). Contrary to general expectations, a high $\Delta S_{M}^{max}$ (7.2 J/K mol-Gd under a 5 T field variation), even comparable to those of candidate materials for low-temperature magnetic refrigeration, was obtained within the antiferromagnetic (AFM) region near the FM / AFM phase boundary. The unexpected enhancement of $\Delta S_{M}^{max}$ toward the AFM region under high magnetic fields indicates an anomalous magnetic response in the present Tsai-type 1/1 AC, which is presumably associated with the breakdown of the MFT. The present finding suggests that tuning the magnetic ground state across the phase boundary is an effective strategy to enhance $\Delta S_{M}$, even in general rare-earth intermetallic compounds.

cond-mat.mtrl-sci↗

arXiv2025

Identification of Two Distinct Antiferromagnetic Phases in the Au-Al-Gd Quasicrystal Approximant

The structural and physical properties of two single-grain Au-Al-Gd 1/1 approximant crystals (ACs) with analyzed compositions Au73.67Al12.24Gd14.09 and Au74.67Al11.35Gd13.98 were thoroughly investigated. The two variants are iso-structural (cubic, space group: Im-3 undergoing sharp antiferromagnetic (AFM) transitions at TN = 9.6 K and TN = 8.3 K, respectively. Specific heat measurements in both samples evidenced sharp jump at TN, associated with the AFM transition, accompanied by broad Schottky-type anomalies at lower temperatures. Strikingly, the two 1/1 ACs exhibited markedly different responses to applied magnetic fields: one displayed a pronounced metamagnetic anomaly while the other did not. In this regard, variational calculations with adiabatic transformation of the magnetic field in realistic structural models identified the existence of two possible AFM phases: the cuboc phase with a metamagnetic anomaly and the cluster N\'eel phase without it, thereby clearly revealing the possible magnetic structures of the present AFM variants. These findings have led to the establishment of a comprehensive magnetic phase diagram for Heisenberg-type 1/1 ACs. This work not only advances our understanding of magnetic phase transitions in these complex systems but also suggests the existence of a broader spectrum of unexplored magnetic states in Tsai-type materials.

cond-mat.mtrl-sci↗

arXiv2025

Universal whirling magnetic orders in non-Heisenberg Tsai-type quasicrystal approximants

Magnetic orders of non-Heisenberg Tsai-type 1/1 approximant crystals (ACs) in the Au-Ga-Dy system were studied through bulk magnetization, neutron diffraction, and inelastic neutron scattering techniques. The results uncovered noncoplanar, ferromagnetic (FM) and antiferromagnetic (AFM) spin configurations whirling along [111] crystallographic axis, which is analogous to those observed in the Tb- and Ho-contained counterparts. The crystal electric field excitations similar to those in the Tb-based counterpart are also observed indicating the strong Ising-like magnetic anisotropy. These comprehensive experiments and analyses have revealed the existence of a universal mechanism that stabilizes noncoplanar FM and AFM structures in non-Heisenberg Tsai-type ACs, independent of the rare-earth species (Tb, Dy, Ho); FM intra-cluster interactions and strong Ising-like anisotropy.

cond-mat.str-el↗

arXiv2023

Revisit of magnetic orders in 1/1 approximant crystals of Tsai-type quasicrystal from theoretical points of view

The various magnetic orders observed in approximant crystals of Tsai-type quasicrystal are important for deepening our understanding of mysterious magnetism in quasicrystals. Using an icosahedral cluster model with inter-cluster interactions, we give an intuitive explanation of the mechanism of magnetic orders previously reported by classical Monte-Carlo simulations for an approximant-crystal model describing a Gd-based Tsai-type 1/1 approximant crystal.

cond-mat.mtrl-sci↗

arXiv2023

Unveiling exotic magnetic phase diagram of a non-Heisenberg quasicrystal approximant

A magnetic phase diagram of the non-Heisenberg Tsai-type 1/1 Au-Ga-Tb approximant crystal (AC) has been established across a wide electron-per-atom (e/a) range via magnetization and powder neutron diffraction measurements. The diagram revealed exotic ferromagnetic (FM) and antiferromagnetic (AFM) orders that originate from the unique local spin icosahedron common to icosahedral quasicrystals (iQCs) and ACs; The noncoplanar whirling AFM order is stabilized as the ground state at the e/a of 1.72 or less whereas a noncoplanar whirling FM order was found at the larger e/a of 1.80, with magnetic moments tangential to the Tb icosahedron in both cases. Moreover, the FM/AFM phase selection rule was unveiled in terms of the nearest neighbour (J1) and next nearest neighbour (J2) interactions by numerical calculations on a non-Heisenberg single icosahedron. The present findings will pave the way for understanding the intriguing magnetic orders of not only non-Heisenberg FM/AFM ACs but also non-Heisenberg FM/AFM iQCs, the latter of which are yet to be discovered.

cond-mat.str-el↗

arXiv2023

Critical behavior and magnetocaloric effect in Tsai-type 2/1 and 1/1 quasicrystal approximants

Stable Tsai-type quinary 1/1 and 2/1 approximant crystals (ACs) with chemical compositions Au56.25Al10Cu7In13Tb13.75 and Au55.5Al10Cu7In13Tb14.5, respectively, exhibiting ferromagnetic (FM) long-range orders were successfully synthesized and studied for their magnetic properties and magnetocaloric effect. The 1/1 and 2/1 ACs primarily differ in their long-range atomic arrangement and rare earth (RE) distribution, with the latter approaching quasiperiodic order while still preserving periodicity. Analyses based on the scaling principle and Kouvel-Fisher (KF) relations suggested mean-field-like behavior near Curie temperatures in both compounds. From magnetization measurements and the Maxwell equation, a magnetic entropy change of -4.3 and -4.1 J/K mol Tb were derived under a magnetic field change of 7 T for the 1/1 and 2/1 ACs, respectively. The results indicated a prominent role of intra-cluster magnetic interactions on critical behavior and magnetic entropy of the Tsai-type compounds.

cond-mat.str-el↗

arXiv2023

Atomic structure and magnetism of the Au-Ga-Ce 1/1 approximant crystal

We report a new Au-Ga-Ce 1/1 approximant crystal (AC) which possesses a significantly wide single-phase region of 53 - 70 at% Au and 13.6 - 15.1 at% Ce. Single crystal X-ray structural analyses reveal the existence of two types of structural degrees of freedom, i.e., the Au/Ga mixing sites and the fractional Ce occupancy site: the former enables a large variation in the electron concentration and the latter allows a variation in the occupancy of a magnetic impurity atom at the center of the Tsai-type cluster. Following these findings, the influences of two types of structural modifications on the magnetism are thoroughly investigated by means of magnetic susceptibility and specific heat measurements on the Au-Ga-Ce 1/1 AC. The spin-glass (SG) state is found to be the ground state over the entire single-phase region, showing a robust nature of the SG state against both structural modifications. In addition, a gigantic specific heat (C/T) is commonly observed at low temperatures for all the compositions, which is consistently explained as a consequence of the spin-freezing phenomenon, not of a heavy Fermion behavior as reported elsewhere. Moreover, the origin of the SG state in the 1/1 Au-Ga-Ce AC is attributed to the existence of non-magnetic atom disorder in the Au/Ga mixing sites. Furthermore, a Kondo behavior is observed in the electrical resistivity at low temperatures, which is enhanced by increasing the Ce concentration, verifying that a Ce atom introduced at the cluster center behaves as a Kondo impurity for the first time.

cond-mat.str-el↗

arXiv2023

Superconductivity in a van der Waals layered quasicrystal

van der Waals (vdW) layered transition-metal chalcogenides are attracting significant attention owing to their fascinating physical properties. This group of materials consists of abundant members with various elements, having a variety of different structures. However, all vdW layered materials studied to date have been limited to crystalline materials, and the physical properties of vdW layered quasicrystals have not yet been reported. Here, we report on the discovery of superconductivity in a vdW layered quasicrystal of Ta1.6Te. The electrical resistivity, magnetic susceptibility, and specific heat of the Ta1.6Te quasicrystal fabricated by reaction sintering, unambiguously validated the occurrence of bulk superconductivity at a transition temperature of ~1 K. This discovery can pioneer new research on assessing the physical properties of vdW layered quasicrystals as well as two-dimensional quasicrystals; moreover, it paves the way toward new frontiers of superconductivity in thermodynamically stable quasicrystals, which has been the predominant challenge facing condensed matter physics since the discovery of quasicrystals almost four decades ago.

cond-mat.mtrl-sci↗

arXiv2023

Emergence of long-range magnetic order from spin-glass state by tuning electron density in a stoichiometric Ga-based quasicrystal approximant

This study reports the first observation of ferromagnetic (FM) order in the non-Au-based approximant crystals (ACs) using a novel approach whereby a total electron-per-atom (e/a) ratio of the spin-glass Ga50Pd36Gd14 1/1 AC is lowered by simultaneously substituting certain ratios of a tri-valent Ga and a zero-valent Pd by a mono-valent Au. The emergence of FM order by this method was confirmed via magnetic susceptibility, magnetization, and specific heat measurements. The findings of this study open up vast opportunities in developing long-range magnetic orders from stoichiometric ACs, quasicrystals, and even other RKKY compounds with spin-glass ground state.

cond-mat.str-el↗

arXiv2023

Competition between spin-glass and antiferromagnetic states in Tsai-type 1/1 and 2/1 quasicrystal approximants

Systematic research was performed to investigate magnetic properties of the Tsai-type Ga-Pd-RE (RE = Gd, Tb, Dy, and Ho) systems, where both 1/1 and 2/1 quasicrystal approximants (ACs) are attainable at the same compositions as thermodynamical stable phases. Most of the samples exhibited spin-glass (SG)-like freezing behavior at low temperatures except Ga-Pd-Tb 2/1 AC and Ga-Pd-Ho 1/1 AC. The former showcased antiferromagnetic order at 5.78 K while the latter did not show any anomaly down to 1.8 K. Furthermore, 2/1 ACs were noticed to be less frustrated than their corresponding 1/1 ACs presumably due to the disorder-free environment in the nearest neighbors of the rare earth sites that form a network of distorted octahedron in the 2/1 ACs. The spin dynamic in SG samples was also characterized by means of ac magnetic susceptibility measurements. The results evidenced a weak response of the freezing temperatures to the measurement frequency in the Heisenberg systems, i.e., Gd-contained ACs, in contrast to the non-Heisenberg systems, i.e., Tb, Dy and Ho-contained ACs, where significant dependency is noticed for the latter. The spin-glass samples were further examined by fitting their freezing temperatures to the Vogel-Fulcher law.

cond-mat.mtrl-sci↗

arXiv2023

Atomic structure of the unique antiferromagnetic 2/1 quasicrystal approximant

The atomic structure of the recently discovered antiferromagnetic Ga50Pd35.5Tb14.5 2/1 approximant to quasicrystal with the space group of Pa-3(No. 205), a = 23.1449(0) angstrom was determined by means of a single crystal X-ray diffraction. The refined structure model revealed two main building units, namely, a Tsai-type rhombic triacontahedron (RTH) cluster with three concentric inner shells and an acute rhombohedron filling the gaps in between the RTH clusters. One of the interesting findings was a very low number of chemically mixed sites in the structure, which amount to only 7.40 % of the all the atomic sites within an RTH cluster. In particular, a disorder-free environment was noticed within a nearest neighbor of an isolated Tb3+ ion, which is presumably one of the main contributors in enhancing antiferromagnetic order in the present compound. The second significant finding was the observance of an orientationally ordered trigonal pyramid-like unit with a height of 4.2441(7) angstrom at the center of the RTH cluster, which has never been observed in Tsai-type compounds before. Such unit is noticed to bring structural distortion to outer shells, in particular, to the surrounding dodecahedron cage being another possible contributor of the antiferromagnetic order establishment in the present compound. The results, therefore, are suggestive of a possible link between chemical/positional order and the antiferromagnetic order establishment.

cond-mat.mtrl-sci↗

arXiv2022

Structural and magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$

Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antiferromagnetic phase, the magnetic moments are aligned almost perpendicular to a pseudo five-fold symmetry axis, which should correspond to the easy-axis direction of a Tb atom. The magnetic properties similar to those of Au$_{72}$Al$_{14}$Tb$_{14}$ in spite of the difference in the electron-per-atom ratio suggest the robustness of the easy-axis anisotropy against the chemical substitution of the nonmagnetic atoms.

cond-mat.str-el↗

arXiv2022

Hexagonal and trigonal quasiperiodic tilings

Exploring nonminimal-rank quasicrystals, which have symmetries that can be found in both periodic and aperiodic crystals, often provides new insight into the physical nature of aperiodic long-range order in models that are easier to treat. Motivated by the prevalence of experimental systems exhibiting aperiodic long-range order with hexagonal and trigonal symmetry, we introduce a generic two-parameter family of 2-dimensional quasiperiodic tilings with such symmetries. We focus on the special case of trigonal and hexagonal Fibonacci, or golden-mean, tilings, analogous to the well studied square Fibonacci tiling. We first generate the tilings using a generalized version of de Bruijn's dual grid method. We then discuss their interpretation in terms of projections of a hypercubic lattice from six dimensional superspace. We conclude by concentrating on two of the hexagonal members of the family, and examining a few of their properties more closely, while providing a set of substitution rules for their generation.

cond-mat.soft↗

arXiv2020

Classical and Quantum Magnetic Ground States on an Icosahedral Cluster

Recent discovery of various magnetism in Tsai-type quasicrystalline approximants, in whose alloys rare-earth ions located on icosahedral apices are coupled with each other via the Ruderman--Kittel--Kasuya--Yosida interaction, opens an avenue to find novel magnetism originating from the icosahedral symmetry. Here we investigate classical and quantum magnetic states on an icosahedral cluster within the Heisenberg interactions of all bonds. Simulated annealing and numerical diagonalization are performed to obtain the classical and quantum ground states. We obtain qualitative correspondence of classical and quantum phase diagrams. Our study gives a good starting point to understand the various magnetism in not only quasicrystalline approximants but also quasicrystals.

cond-mat.other↗