Showing 1–50 of 272 results for author: Takano, Y

Wide-field NV magnetometry under simultaneous high-pressure and high-temperature conditions

Authors: Masahiro Ohkuma, Eikichi Kimura, Shumpei Ohyama, Miu Tezuka, Ryo Matsumoto, Shinobu Onoda, Yoshihiko Takano, Shintaro Azuma, Kenji Ohta, Keigo Arai

Abstract: We demonstrate wide-field optically detected magnetic resonance (ODMR) under simultaneous high-pressure and high-temperature conditions using nitrogen-vacancy (NV) centers. Although NV-center magnetometry has been widely used for spatially resolved magnetic-field imaging, its application to extreme environments combining pressure and temperature remains challenging. In this work, we show that ODMR… ▽ More We demonstrate wide-field optically detected magnetic resonance (ODMR) under simultaneous high-pressure and high-temperature conditions using nitrogen-vacancy (NV) centers. Although NV-center magnetometry has been widely used for spatially resolved magnetic-field imaging, its application to extreme environments combining pressure and temperature remains challenging. In this work, we show that ODMR can be observed at 5 GPa and 500 K, demonstrating the feasibility of NV spin readout under such combined extreme conditions. We further perform wide-field ODMR of iron at 7 GPa and 500 K, where the stray magnetic field from the sample is spatially visualized through the pressure cell. These results establish NV-center magnetometry as a promising platform for imaging magnetic phenomena in materials under high-pressure and high-temperature environments. △ Less

Submitted 30 June, 2026; v1 submitted 24 June, 2026; originally announced June 2026.

Designing electronic magnetoelectric matter with organic quantum spin trimers

Authors: Yuko Hosokoshi, Christopher P. Aoyama, Zhuowei Zhang, Toshio Ono, Kosuke Takada, Ayaka Higashiguchi, Seitaro Iisaka, Koudai Yamasaki, Hironori Yamaguchi, Shengzhi Zhang, Mohammad Irfan, Minseong Lee, Eun Sang Choi, Yasuyuki Shimura, Toshiro Sakakibara, Zhiyuan Xie, Hiroki Nakano, Yasu Takano, Cristian D. Batista, Yoshitomo Kamiya

Abstract: Magnetoelectric (ME) phenomena are commonly driven by spin-lattice coupling. Here we demonstrate a different route based on frustrated quantum spin trimers that intrinsically intertwine magnetic moments and electric dipoles. Using molecular design principles, we realize a weakly coupled lattice of equilateral $S=1/2$ spin trimers in the organic radical crystal TNN$\cdot$CH$_3$CN. In this material,… ▽ More Magnetoelectric (ME) phenomena are commonly driven by spin-lattice coupling. Here we demonstrate a different route based on frustrated quantum spin trimers that intrinsically intertwine magnetic moments and electric dipoles. Using molecular design principles, we realize a weakly coupled lattice of equilateral $S=1/2$ spin trimers in the organic radical crystal TNN$\cdot$CH$_3$CN. In this material, correlated electronic fluctuations within each trimer generate electric dipoles, while geometrically frustrated intertrimer interactions organize them into collective ME states. Magnetization, thermodynamic, and dielectric measurements reveal multiple magnetic-field-induced phases, including the $1/3$-magnetization plateau marked by pronounced dielectric anomalies. Effective low-energy theories and numerical simulations show that these phenomena are driven by electronically generated trimer dipoles whose collective order is stabilized by frustration relief of the intertrimer interactions, establishing a direct connection between geometric frustration and emergent magnetoelectricity. Our results identify quantum spin trimers as multifunctional building blocks, providing a bottom-up route for designing correlated ME materials from electronically active quantum spin clusters. △ Less

Submitted 8 June, 2026; originally announced June 2026.

Comments: 13 pages, 6 figures; Supplementary Information included

Superconducting Lanthanum Nickel Oxides with Bilayered and Trilayered Crystal Structures

Authors: Hiroya Sakurai, Yoshihiko Takano

Abstract: In 2023, superconductivity in La$_3$Ni$_2$O$_7$ was discovered under high pressures above approximately 14 GPa. In addition to its high transition temperature ($T_{\mathrm{c}} \simeq 80$ K), the structural resemblance to high-$T_{\mathrm{c}}$ cuprates has strongly stimulated research, soon followed by the discovery of superconductivity in La$_4$Ni$_3$O$_{10}$. These compounds belong to the Ruddles… ▽ More In 2023, superconductivity in La$_3$Ni$_2$O$_7$ was discovered under high pressures above approximately 14 GPa. In addition to its high transition temperature ($T_{\mathrm{c}} \simeq 80$ K), the structural resemblance to high-$T_{\mathrm{c}}$ cuprates has strongly stimulated research, soon followed by the discovery of superconductivity in La$_4$Ni$_3$O$_{10}$. These compounds belong to the Ruddlesden--Popper phases, comprising double- and triple-layered NiO$_2$ square lattices separated by LaO rock-salt slabs. Research on these systems has rapidly developed along three major directions, as in other prominent families of superconductors such as the cuprates and iron arsenides: expanding the chemical variety of compounds, enhancing $T_{\mathrm{c}}$ through elemental substitution, and elucidating the superconducting mechanism. These challenges, being closely interconnected, continue to drive the field. The clarification of the pairing mechanism encounters a particular difficulty, since the key experiments must be performed under high pressures. This situation highlights the significance of developing nickel oxides that exhibit superconductivity at much lower pressures, ideally at ambient pressure, which would in turn broaden the scope of chemical tuning and detailed physical characterization. In this context, it is timely and meaningful to summarize the present state of knowledge. Here, we emphasize sample synthesis and characterization, which are already well established and often decisive for progress in unconventional superconductors, while providing a brief overview of the currently available electronic properties. △ Less

Submitted 18 March, 2026; originally announced March 2026.

Comments: The revised version of this paper has been published in J. Phys. Condens. Matter 38 (2026) 073002. DOI: 10.1088/1361-648X/ae4155

Probing the Meissner effect in single crystals of $\mathbf{Bi_2Sr_2Ca_2Cu_3O_{10+δ}}$ via wide-field quantum microscopy under high pressure

Authors: Masahiro Ohkuma, Ryo Matsumoto, Shintaro Adachi, Shinobu Onoda, Takao Watanabe, Kenji Ohta, Yoshihiko Takano, Keigo Arai

Abstract: We investigated the pressure dependence of the superconducting transition temperature ($T_{\rm c}$) in optimally doped Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$ (Bi-2223) single crystals using different pressure-transmitting media. Previous high-pressure studies have reported conflicting behaviors, ranging from a resurgence of $T_{\rm c}$ of optimally doped Bi-2223 in fluid media to an insulating-like tr… ▽ More We investigated the pressure dependence of the superconducting transition temperature ($T_{\rm c}$) in optimally doped Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$ (Bi-2223) single crystals using different pressure-transmitting media. Previous high-pressure studies have reported conflicting behaviors, ranging from a resurgence of $T_{\rm c}$ of optimally doped Bi-2223 in fluid media to an insulating-like transition in solid media. However, a direct comparison of the effects of different pressure-transmitting media is lacking. Here, we employed wide-field quantum microscopy based on nitrogen-vacancy centers to probe the magnetic response under high pressure, utilizing cBN and KBr as media. We observed that a diamagnetic response near 70 K, indicative of the superconducting transition, persisted up to 23 GPa in KBr, whereas it disappeared above 11 GPa and 70 K in cBN. These results demonstrate the high sensitivity of Bi-2223 to the pressure environment and highlight the critical role of hydrostatic pressure in cuprate superconductors. △ Less

Submitted 16 March, 2026; originally announced March 2026.

Orchestration of Heterogeneous Experimental Machines via ROS2 for Automated Bulk Intermetallic Synthesis

Authors: Wei-Sheng Wang, Kensei Terashima, Yoshihiko Takano

Abstract: With advances in informatics applied to materials science, predicting the physical properties of numerous materials has become increasingly feasible, creating a growing demand for their experimental validation. It has been expected that the integration of robotic systems into experimental materials science excels at efficiently performing repetitive and time-consuming tasks without the need for hu… ▽ More With advances in informatics applied to materials science, predicting the physical properties of numerous materials has become increasingly feasible, creating a growing demand for their experimental validation. It has been expected that the integration of robotic systems into experimental materials science excels at efficiently performing repetitive and time-consuming tasks without the need for human intervention, thus significantly increasing throughput and reducing the risk of human error, while there have been a limited number of reports tackled the synthesis process of solid bulk material so far possibly because of the complex as well as a wide variety of processes to deal with. In this paper, we report an automated arc melting system controlled by a robot operating system2 (ROS2). Taking advantage of ROS2, we have constructed a machine that can handle multiple experimental apparatuses simultaneously with flexibility for future expansion of functions. The constructed machine is capable of not only performing repeated operation of a specific process but also dealing with multiple elements for synthesis of intermetallic compounds. The system is expected to accelerate experimental validation of data-driven materials exploration. △ Less

Submitted 15 September, 2025; originally announced September 2025.

Comments: 13 pages, 5 figures

Optically detected magnetic resonance of nitrogen-vacancy centers in microdiamonds inside nanopolycrystalline diamond anvil cell

Authors: Masahiro Ohkuma, Keigo Arai, Kenji Ohta, Toru Shinmei, Ryo Matsumoto, Yoshihiko Takano, Tetsuo Irifune

Abstract: We demonstrated optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in microdiamonds inside a diamond anvil cell pressurized with nanopolycrystalline diamond (NPD) anvils. NPD exhibits high optical transparency, superior hardness, and low thermal conductivity, making it suitable for optical and spectroscopic measurements under high-pressure and high-temperature conditions… ▽ More We demonstrated optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in microdiamonds inside a diamond anvil cell pressurized with nanopolycrystalline diamond (NPD) anvils. NPD exhibits high optical transparency, superior hardness, and low thermal conductivity, making it suitable for optical and spectroscopic measurements under high-pressure and high-temperature conditions. We observed the ODMR signal from an ensemble of NV centers under conditions where NV centers in microdiamonds served as markers for pressures exceeding 30 GPa, with a culet diameter of 600 $μ$m. We also performed ODMR measurements on multiple microdiamonds sealed inside a sample chamber and found that the resonance frequency varied with the pressure distribution. The combination of NPD and microdiamonds containing NV centers is auspicious for pressure and magnetic sensing under concurrent high-pressure and high-temperature conditions. △ Less

Submitted 22 February, 2026; v1 submitted 17 July, 2025; originally announced July 2025.

Highly anisotropic magnetic phase diagram of the ferromagnetic rare-earth diboride HoB$_{2}$

Authors: Takafumi D. Yamamoto, Hiroyuki Takeya, Kensei Terashima, Akiko T. Saito, Yoshihiko Takano

Abstract: Rare-earth (RE) compounds have been of enormous interest in condensed matter physics as a platform for the exploration of interesting physical phenomena. Here, we report the successful single crystal growth of HoB$_{2}$, which exhibits a paramagnetic (PM)-ferromagnetic (FM) phase transition at 15 K and another phase transition at 11 K, and the discovery of a highly anisotropic magnetic phase diagr… ▽ More Rare-earth (RE) compounds have been of enormous interest in condensed matter physics as a platform for the exploration of interesting physical phenomena. Here, we report the successful single crystal growth of HoB$_{2}$, which exhibits a paramagnetic (PM)-ferromagnetic (FM) phase transition at 15 K and another phase transition at 11 K, and the discovery of a highly anisotropic magnetic phase diagram of this FM diboride. Magnetization measurements suggest that the ferromagnetically ordered moments of Ho$^{3+}$ ions are oriented at a direction tilted by 50 degrees from the ab-plane at 2K, which rotate largely toward the ab-plane direction upon application of a magnetic field, but hardly toward the c-axis direction. Heat capacity and electrical resistivity measurements clearly demonstrate that the low-temperature phase transition at 11 K occurs even under high magnetic fields along the ab-plane direction, whereas it disappears immediately by magnetic fields along the c-axis direction. Moreover, the field-induced crossover phenomenon between FM and PM phases near 15 K is found to be more promoted when applying a magnetic field along the ab-plane direction. The resulting magnetic phase diagram reveals that in-plane magnetic anisotropy is predominant in the present system, which contradicts the previous report of a spin reorientation phenomenon toward the c-axis direction between 11 K and 15 K. Taken together, the present findings suggest the presence of strong competition between in-plane and out-of-plane magnetic anisotropies in HoB$_{2}$, giving rise to the unique FM spin arrangement. △ Less

Submitted 18 June, 2025; originally announced June 2025.

Journal ref: Phys. Rev. B 112, 024423 (2025)

Revisiting the physical properties of (LaS)1+d(NbS2) misfit-layered compounds

Authors: Masanori Nagao, Dan Mouri, Yuki Maruyama, Akira Miura, Yoshihiko Takano, Satoshi Watauchi

Abstract: Electrical transport in polycrystalline and single-crystalline (LaS)1+d(NbS2) misfit-layered compounds was measured. Polycrystalline samples were synthesized using S raw materials of different purities (2N or 6N), and single-crystalline samples were grown using two types of transport agents (2NH4Cl+PbCl2 or NH4Cl) via the chemical vapor transport method. The temperature dependence on resistivity d… ▽ More Electrical transport in polycrystalline and single-crystalline (LaS)1+d(NbS2) misfit-layered compounds was measured. Polycrystalline samples were synthesized using S raw materials of different purities (2N or 6N), and single-crystalline samples were grown using two types of transport agents (2NH4Cl+PbCl2 or NH4Cl) via the chemical vapor transport method. The temperature dependence on resistivity dropped at 1.3-2.0 K for some of the samples, which might be affected by the unknown impurity. (LaS)1+d(NbS2) misfit-layered compounds for the main phase of those obtained samples exhibited no superconductivity above 0.2 K by the resistivity measurement. △ Less

Submitted 30 April, 2025; originally announced May 2025.

Comments: 5 figures, 2 tables

Journal ref: Solid State Communications, vol.403 (2025) 115980

Microscopic evidence for spin-spinless stripe order with reduced Ni moments within $ab$ plane for bilayer nickelate La$_3$Ni$_2$O$_7$ probed by $^{139}$La-NQR

Authors: Mitsuharu Yashima, Nina Seto, Yujiro Oshita, Masataka Kakoi, Hiroya Sakurai, Yoshihiko Takano, Hidekazu Mukuda

Abstract: The intrinsic electronic properties of La$_3$Ni$_2$O$_{7}$ have been selectively investigated by nuclear quadrupole resonance (NQR) at the La(2) site outside the NiO$_2$ bilayers. The La(2)$_{\rm a}$ site of the ideal La$_3$Ni$_2$O$_{7}$ is clearly distinguished from the La(2)$_{\rm b}$ site close to the local defects. Below 150K, almost half of the intrinsic La(2)$_{\rm a}$ sites are dominated by… ▽ More The intrinsic electronic properties of La$_3$Ni$_2$O$_{7}$ have been selectively investigated by nuclear quadrupole resonance (NQR) at the La(2) site outside the NiO$_2$ bilayers. The La(2)$_{\rm a}$ site of the ideal La$_3$Ni$_2$O$_{7}$ is clearly distinguished from the La(2)$_{\rm b}$ site close to the local defects. Below 150K, almost half of the intrinsic La(2)$_{\rm a}$ sites are dominated by a finite internal field within the $ab$ plane, while the other half are dominated by zero internal field. The result is fully consistent with the single spin-spinless stripe order of ($\cdots\uparrow\circ\downarrow\circ\uparrow\circ\cdots$), where the reduced Ni magnetic moments are parallel to the $ab$-plane. Even for the La(2)$_{\rm b}$ site, the result is also explained within the same model by considering the inhomogeneous internal magnetic fields enhanced around the nearby defects such as oxygen vacancies. These findings provide unambiguous microscopic evidence for the single spin-spinless stripe order below 150 K at ambient pressure. △ Less

Submitted 14 March, 2025; v1 submitted 12 March, 2025; originally announced March 2025.

Comments: 6+2 pages, 4+2 figures

Journal ref: J. Phys. Soc. Jpn. 94, 054704 (2025)

Enhancement of superconductivity on thin film of Sn under high pressure

Authors: Misaki Sasaki, Masahiro Ohkuma, Ryo Matsumoto, Toru Shinmei, Tetsuo Irifune, Yoshihiko Takano, Katsuya Shimizu

Abstract: We investigated the pressure effects of a superconductivity on thin films of Sn. Elemental superconductor Sn with a body-centered tetragonal structure, $β$-Sn, exhibits superconductivity below the superconducting transition temperature ($T_{\rm c}=3.72$ K) at ambient pressure. $T_{\rm c}$ of Sn increases with lowering dimension such as in thin film and nanowire growth, or by high-pressure applicat… ▽ More We investigated the pressure effects of a superconductivity on thin films of Sn. Elemental superconductor Sn with a body-centered tetragonal structure, $β$-Sn, exhibits superconductivity below the superconducting transition temperature ($T_{\rm c}=3.72$ K) at ambient pressure. $T_{\rm c}$ of Sn increases with lowering dimension such as in thin film and nanowire growth, or by high-pressure application. For thin films, $T_{\rm c}$ exhibits a slight increase up to approximately 4 K compared to the bulk value, attributable to the crystalline size and lattice disorder. By applying pressure on a bulk Sn, $T_{\rm c}$ initially decreases from 3.72 K as the pressure increases. Further increasing pressure up to 10 GPa, $T_{\rm c}$ increases to 5.3 K with the structural transformation. However, the combination of these effects on thin films of Sn, namely, thin-film growth and pressure effects, remains underexplored. In this study, we combined film-growth and pressure-application techniques to further increase $T_{\rm c}$ using a diamond anvil cell with boron-doped diamond electrodes. The drop of the electrical resistance suggesting the onset of $T_{\rm c}$ on the thin film reached above 6 K in $γ$-Sn phase. Further, the upper critical magnetic field was drastically enhanced. Atomic force microscopy suggests that the refinement of the grain size of the thin film under the non-hydrostatic pressure conditions contributes to stabilizing the higher $T_{\rm c}$ of $γ$-Sn. △ Less

Submitted 27 March, 2025; v1 submitted 29 January, 2025; originally announced January 2025.

Journal ref: Phys. Rev. B 111, 104513 (2025)

High-pressure synthesis of bilayer nickelate Sr$_{3}$Ni$_{2}$O$_{5}$Cl$_{2}$ with tetragonal crystal structure

Authors: Kazuki Yamane, Yoshitaka Matsushita, Shintaro Adachi, Ryo Matsumoto, Kensei Terashima, Takanobu Hiroto, Hiroya Sakurai, Yoshihiko Takano

Abstract: A novel oxychloride, Sr$_{3}$Ni$_{2}$O$_{5}$Cl$_{2}$, was synthesized for the first time under high pressure of 10 GPa at 1400 ${}^\circ$C, motivated by a theoretical prediction of its potential superconductivity under ambient pressure. Small single crystals were used to determine the crystal structure and measure the temperature dependence of electrical resistance. The crystal is isostructural wi… ▽ More A novel oxychloride, Sr$_{3}$Ni$_{2}$O$_{5}$Cl$_{2}$, was synthesized for the first time under high pressure of 10 GPa at 1400 ${}^\circ$C, motivated by a theoretical prediction of its potential superconductivity under ambient pressure. Small single crystals were used to determine the crystal structure and measure the temperature dependence of electrical resistance. The crystal is isostructural with the recently discovered superconductor, La$_{3}$Ni$_{2}$O$_{7}$, in line with the theoretical expectation. △ Less

Submitted 12 December, 2024; originally announced December 2024.

Pressure-induced anomalous enhancement in superconducting critical temperature of transition-metal chalcogenide Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$

Authors: Ryo Matsumoto, Akitoshi Nakano, Takafumi D Yamamoto, Kensei Terashima, Kazuki Yamane, Masahiro Ohkuma, Ichiro Terasaki, Yoshihiko Takano

Abstract: The emergence of a second dome in the superconducting phase through pressure-driven manipulation of crystal structures in materials has attracted considerable attention. Transition metal chalcogenides (TMCs) represent a highly promising platform, as the second dome has been observed in several binary compounds. Recently, ternary TMCs such as Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ have exhibited pressure… ▽ More The emergence of a second dome in the superconducting phase through pressure-driven manipulation of crystal structures in materials has attracted considerable attention. Transition metal chalcogenides (TMCs) represent a highly promising platform, as the second dome has been observed in several binary compounds. Recently, ternary TMCs such as Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ have exhibited pressure-induced superconducting domes. In this study, we perform electrical transport measurements of Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ under extremely high pressures exceeding 100 GPa, namely uninvestigated regions in previous reports, to reveal the emergence of the second dome. The superconducting critical temperatures (T$_c$) in both Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ initially decrease with increasing pressure. Subsequently, the Tcs tend to enhance drastically above 100 GPa. Notably, the maximum T$_c$ in Ta$_2$PdS$_6$ is 11.2 K at 130.0 GPa, which is a relatively high record among the TMCs. The emergence of the second dome in Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ opens further motivation for the investigation under extreme conditions beyond the first dome to find hidden ordered phases. △ Less

Submitted 2 November, 2024; originally announced November 2024.

Investigation of superconducting gap of high-entropy telluride AgInSnPbBiTe5

Authors: Asato Seshita, Hirotaka Okabe, Riad Kasem, Yuto Watanabe, Jumpei G. Nakamura, Shoichiro Nishimura, Kensei Terashima, Ryo Matsumoto, Yoshihiko Takano, Aichi Yamashita, Masaki Fujita, Yoshikazu Mizuguchi

Abstract: We performed transverse-field muon spin relaxation/rotation (TF-μSR) on a high-entropy-type (HE-type) superconductor AgInSnPbBiTe5. The emergence of bulk superconducting states was confirmed from magnetic susceptibility, specific heat, and μSR. The superconducting gap 2Δ(0) estimated from μSR was clearly larger than that expected from conventional weak-coupling phonon-mediated model, suggesting th… ▽ More We performed transverse-field muon spin relaxation/rotation (TF-μSR) on a high-entropy-type (HE-type) superconductor AgInSnPbBiTe5. The emergence of bulk superconducting states was confirmed from magnetic susceptibility, specific heat, and μSR. The superconducting gap 2Δ(0) estimated from μSR was clearly larger than that expected from conventional weak-coupling phonon-mediated model, suggesting the strong-coupling nature of superconductivity. In addition, a long penetration depth of 3.21(7) μm was obtained. The strong-coupling nature of superconductivity and the long penetration depth are similar to the trends observed in the other HE-type superconductors (HE alloys and transition-metal zirconides), which may be universal feature of HE-type superconductors. △ Less

Submitted 9 October, 2024; originally announced October 2024.

Comments: 14 pages, 4 figures, Supplementary information

Emergence of Superconductivity at 20 K in Th$_3$P$_4$-type In$_{3-x}$S$_4$ Synthesized by Diamond Anvil Cell with Boron-doped Diamond Electrodes

Authors: Ryo Matsumoto, Kazuki Yamane, Terumasa Tadano, Kensei Terashima, Toru Shinmei, Tetsuo Irifune, Yoshihiko Takano

Abstract: The exploration of superconductors in metastable phases by manipulating crystal structures through high-pressure techniques has attracted significant interest in materials science to achieve a high critical temperature ($T_c$). In this study, we report an emergence of novel superconductivity in a metastable phase of Th$_3$P$_4$-type cubic In$_{3-x}$S$_4$ with remarkably high $T_c$ at 20 K under 45… ▽ More The exploration of superconductors in metastable phases by manipulating crystal structures through high-pressure techniques has attracted significant interest in materials science to achieve a high critical temperature ($T_c$). In this study, we report an emergence of novel superconductivity in a metastable phase of Th$_3$P$_4$-type cubic In$_{3-x}$S$_4$ with remarkably high $T_c$ at 20 K under 45 GPa by using an originally designed diamond anvil cell equipped with boron-doped diamond electrodes, which can perform a high-pressure synthesis and an in-situ electrical transport measurement simultaneously. In-situ structural analysis indicates that the In$_{3-x}$S$_4$ appears partially above 40 GPa without heating. The high-pressure annealing treatment induces complete transformation to the Th$_3$P$_4$-type structure, and the defected concentration of x in In$_{3-x}$S$_4$ decreases with increasing annealing temperature. The $T_c$ in In$_{3-x}$S$_4$ is maximized at x = 0 and approaches 20 K. Electronic band calculations show that the high density of states composed of sulfur and indium bands are located at the conduction band bottom near Fermi energy. The record high $T_c$ in In$_{3-x}$S$_4$ among superconducting sulfides accelerates the further exploration of high $T_c$ materials within the Th$_3$P$_4$-type cubic family by using flexibility in crystal structure. △ Less

Submitted 5 September, 2024; originally announced September 2024.

Phase diagram of pressure-induced high temperature superconductor La$_{3}$Ni$_{2}$O$_{7+δ}$

Authors: Yuta Ueki, Hiroya Sakurai, Hibiki Nagata, Kazuki Yamane, Ryo Matsumoto, Kensei Terashima, Keisuke Hirose, Hiroto Ohta, Masaki Kato, Yoshihiko Takano

Abstract: We successfully synthesized samples of La$_{3}$Ni$_{2}$O$_{7+δ}$ ($δ= -0.50$, $-0.16$, $0.00$, $+0.01$, and $+0.12$) and measured the resistance under extremely high pressures using a diamond anvil cell to establish the electronic phase diagram. A Mott insulating state appears at $δ= -0.50$, where all Ni ions are divalent. With increasing oxygen content, superconductivity appears at $δ= 0.00$ and… ▽ More We successfully synthesized samples of La$_{3}$Ni$_{2}$O$_{7+δ}$ ($δ= -0.50$, $-0.16$, $0.00$, $+0.01$, and $+0.12$) and measured the resistance under extremely high pressures using a diamond anvil cell to establish the electronic phase diagram. A Mott insulating state appears at $δ= -0.50$, where all Ni ions are divalent. With increasing oxygen content, superconductivity appears at $δ= 0.00$ and higher, above approximately 25 GPa, passing through Anderson localization at $δ= -0.16$. The superconducting transition temperature $T_{\mathrm{c}}$ decreases with increasing pressures for both $δ= 0.00$ and $+0.12$, with the pressure dependence of $T_{\mathrm{c}}$ being much stronger in the latter than in the former. △ Less

Submitted 9 August, 2024; originally announced August 2024.

Report number: Journal of the Physical Society of Japan, 94, 013703 (2025)

Journal ref: J. Phys. Soc. Jpn.,. 94, 013703 (2025)

Magnetic properties of AlB$_2$-type holmium silicides and germanides

Authors: G. Eguchi, R. Matsumoto, K. Terashima, Y. Takano

Abstract: Discovery of the large magnetocaloric effect in HoB$_2$ has highlighted the practical advantage of heavy rare-earth ions. Other holmium compounds are of interest, and we here report the synthesis and the magnetic properties of HoSi$_{1.67}$ and HoGe$_{1.67}$ which form the same AlB$_2$-type structure but with vacancies. They are found to show the antiferromagnetic order with the Neel temperature 1… ▽ More Discovery of the large magnetocaloric effect in HoB$_2$ has highlighted the practical advantage of heavy rare-earth ions. Other holmium compounds are of interest, and we here report the synthesis and the magnetic properties of HoSi$_{1.67}$ and HoGe$_{1.67}$ which form the same AlB$_2$-type structure but with vacancies. They are found to show the antiferromagnetic order with the Neel temperature 17.6(2)K for HoSi$_{1.67}$ and 9.9(2)K for HoGe$_{1.67}$, and the magnetic entropy changes at the temperature are 0.05(1)J/cm$^3$K for HoSi$_{1.67}$ and 0.08(1)J/cm$^3$K for HoGe$_{1.67}$. Magnetic orders were suppressed by replacing vacancies with nickel, resulting in an increase of magnetic entropy changes. Distance between the in-plane Ho$^{3+}$ ions appears to be an important parameter leading to the transition between the antiferromagnetic (HoSi$_{1.67}$) and the ferromagnetic (HoB$_2$) order. The finding may aid the exploration of other heavy rare-earth compounds for similar applications. △ Less

Submitted 25 July, 2024; originally announced July 2024.

Comments: 18 pages, 6 figures, 2 tables

Pressure-induced superconductivity in La$_{4}$Ni$_{3}$O$_{10+δ}$ ($δ$ = 0.04 and -0.01)

Authors: Hibiki Nagata, Hiroya Sakurai, Yuta Ueki, Kazuki Yamane, Ryo Matsumoto, Kensei Terashima, Keisuke Hirose, Hiroto Ohta, Masaki Kato, Yoshihiko Takano

Abstract: The superconducting transition temperatures, $T_{\mathrm{c}}$, of La$_{4}$Ni$_{3}$O$_{10+δ}$($δ$ = 0.04 and -0.01) were determined under various pressures up to 124.9 GPa by electrical resistance measurements with a diamond anvil cell. $T_{\mathrm{c}}$ exhibits a strong dependence on oxygen content within the pressure range of approximately 20 GPa and 80 GPa. At 48.0 GPa, $T_{\mathrm{c}}$ of La… ▽ More The superconducting transition temperatures, $T_{\mathrm{c}}$, of La$_{4}$Ni$_{3}$O$_{10+δ}$($δ$ = 0.04 and -0.01) were determined under various pressures up to 124.9 GPa by electrical resistance measurements with a diamond anvil cell. $T_{\mathrm{c}}$ exhibits a strong dependence on oxygen content within the pressure range of approximately 20 GPa and 80 GPa. At 48.0 GPa, $T_{\mathrm{c}}$ of La$_{4}$Ni$_{3}$O$_{10.04}$ peaks at 36 K, marking the highest $T_{\mathrm{c}}$ reported thus far. △ Less

Submitted 27 July, 2024; v1 submitted 30 May, 2024; originally announced May 2024.

Comments: to be published in J. Phys. Soc. Jpn

Report number: Journal of the Physical Society of Japan, 93, 095003 (2024)

Journal ref: J. Phys. Soc. Jpn., 93, 095003 (2024)

Pressure-induced volumetric negative thermal expansion in CoZr2 superconductor

Authors: Yuto Watanabe, Hiroto Arima, Saori Kawaguchi-Imada, Hirokazu Kadobayashi, Kenta Oka, Hidetomo Usui, Ryo Matsumoto, Yoshihiko Takano, Takeshi Kawahata, Chizuru Kawashima, Hiroki Takahashi, Aichi Yamashita, Yoshikazu Mizuguchi

Abstract: We investigate the thermal expansion and superconducting properties of a CuAl2-type (tetragonal) superconductor CoZr2 under high pressures. We perform high-pressure synchrotron X-ray diffraction in a pressure range of 2.9 GPa < P < 10.4 GPa and discover that CoZr2 exhibits volumetric negative thermal expansion under high pressures. Although the uniaxial positive thermal expansion (PTE) along the a… ▽ More We investigate the thermal expansion and superconducting properties of a CuAl2-type (tetragonal) superconductor CoZr2 under high pressures. We perform high-pressure synchrotron X-ray diffraction in a pressure range of 2.9 GPa < P < 10.4 GPa and discover that CoZr2 exhibits volumetric negative thermal expansion under high pressures. Although the uniaxial positive thermal expansion (PTE) along the a-axis is observed under ambient pressure, that is suppressed by pressure, while the large uniaxial negative thermal expansion (NTE) along the c-axis is maintained under the pressure regime. As a result of a combination of the suppressed uniaxial PTE along the a-axis and uniaxial NTE along the c-axis, volumetric negative thermal expansion is achieved under high pressure in CoZr2. The mechanisms of volumetric NTE would be based on the flexible crystal structure caused by the soft Co-Co bond as seen in the iso-structural compound FeZr2, which exhibits uniaxial NTE along the c-axis. We also perform high-pressure electrical resistance measurements of CoZr2 to confirm the presence of superconductivity under the examined pressure regime in the range of 0.03 GPa < P < 41.9 GPa. We confirm the presence of superconductivity under all pressures and observe dome-like shape pressure dependence of superconducting transition temperature. Because of the coexistence of two phenomena, which are volumetric NTE and superconductivity, in CoZr2 under high pressure, the coexistence would be achievable under ambient pressure by tuning chemical compositions after our present observation. △ Less

Submitted 24 October, 2023; v1 submitted 22 October, 2023; originally announced October 2023.

Comments: 22 pages, 7 figures, supporting information

Semi-automatic staging area for high-quality structured data extraction from scientific literature

Authors: Luca Foppiano, Tomoya Mato, Kensei Terashima, Pedro Ortiz Suarez, Taku Tou, Chikako Sakai, Wei-Sheng Wang, Toshiyuki Amagasa, Yoshihiko Takano, Masashi Ishii

Abstract: We propose a semi-automatic staging area for efficiently building an accurate database of experimental physical properties of superconductors from literature, called SuperCon2, to enrich the existing manually-built superconductor database SuperCon. Here we report our curation interface (SuperCon2 Interface) and a workflow managing the state transitions of each examined record, to validate the data… ▽ More We propose a semi-automatic staging area for efficiently building an accurate database of experimental physical properties of superconductors from literature, called SuperCon2, to enrich the existing manually-built superconductor database SuperCon. Here we report our curation interface (SuperCon2 Interface) and a workflow managing the state transitions of each examined record, to validate the dataset of superconductors from PDF documents collected using Grobid-superconductors in a previous work. This curation workflow allows both automatic and manual operations, the former contains ``anomaly detection'' that scans new data identifying outliers, and a ``training data collector'' mechanism that collects training data examples based on manual corrections. Such training data collection policy is effective in improving the machine-learning models with a reduced number of examples. For manual operations, the interface (SuperCon2 interface) is developed to increase efficiency during manual correction by providing a smart interface and an enhanced PDF document viewer. We show that our interface significantly improves the curation quality by boosting precision and recall as compared with the traditional ``manual correction''. Our semi-automatic approach would provide a solution for achieving a reliable database with text-data mining of scientific documents. △ Less

Submitted 16 November, 2023; v1 submitted 19 September, 2023; originally announced September 2023.

Comments: 5 tables, 6 figures, 18 pages

Theoretical analysis on the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure and its experimental examination: comparison with La$_3$Ni$_2$O$_7$

Authors: Hirofumi Sakakibara, Masayuki Ochi, Hibiki Nagata, Yuta Ueki, Hiroya Sakurai, Ryo Matsumoto, Kensei Terashima, Keisuke Hirose, Hiroto Ohta, Masaki Kato, Yoshihiko Takano, Kazuhiko Kuroki

Abstract: We study the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure both theoretically and experimentally, making comparison with the recently discovered high $T_c$ superconductor La$_3$Ni$_2$O$_7$, a bilayer nickelate. Through DFT calculations, we find that a structural phase transition from monoclinic to tetragonal takes place around 10 - 1… ▽ More We study the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure both theoretically and experimentally, making comparison with the recently discovered high $T_c$ superconductor La$_3$Ni$_2$O$_7$, a bilayer nickelate. Through DFT calculations, we find that a structural phase transition from monoclinic to tetragonal takes place around 10 - 15 GPa. Using the tetragonal crystal structure, we theoretically investigate the possibility of superconductivity, where a combination of fluctuation exchange approximation and linearized Eliashberg equation is applied to a six-orbital model constructed from first principles band calculation. The obtained results suggests that La$_4$Ni$_3$O$_{10}$ may also become superconducting under high pressure with $T_c$ comparable to some cuprates, although it is not as high as La$_3$Ni$_2$O$_7$. We also perform experimental studies using our polycrystalline samples of La$_3$Ni$_2$O$_{7.01}$ and La$_4$Ni$_3$O$_{9.99}$. The superconducting transition of La$_3$Ni$_2$O$_{7.01}$, with a maximum onset $T_c$ of 67.0 K at a pressure of 26.5 GPa, is confirmed by a drop in the electrical resistance, as well as the magnetic field dependence of the resistance. Quite interestingly, similar temperature and magnetic field dependencies of the resistance are observed also for La$_4$Ni$_3$O$_{9.99}$, where a drop in the resistance is observed at lower temperatures compared to La$_3$Ni$_2$O$_{7.01}$, under pressures of 32.8 GPa and above. Given the theoretical expectation, the reduction in the resistance can most likely be attributed to the occurrence of superconductivity in La$_4$Ni$_3$O$_{9.99}$. The temperature at which the resistance deviates from a linear behavior, considered as the onset $T_c$, monotonically increases up to 23 K at 79.2 GPa, which is opposite to the pressure dependence of $T_c$ in La3Ni2O7.01. △ Less

Submitted 29 February, 2024; v1 submitted 17 September, 2023; originally announced September 2023.

Comments: 9 pages, 5 figures, Fig.4 added

Formation of random singlets in the nanocrystalline quasi-one-dimensional spin-1/2 antiferromagnet Sr21Bi8Cu2(CO3)2O41

Authors: Yanbo Guo, Xinzhe Hu, Hasan Siddiquee, Kapila Kumarasinghe, Swapnil M. Yadav, Eun Sang Choi, Yasuyuki Nakajima, Yasumasa Takano

Abstract: Induced by quenched disorder, random-singlet states occur in a variety of low-dimensional spin-1/2 antiferromagnets, some of them candidates for quantum spin liquids. Here we report measurements of the specific heat, magnetization, and magnetic susceptibility of nanocrystalline Sr21Bi8Cu2(CO3)2O41, a quasi-one-dimensional spin-1/2 antiferromagnet with alternating bonds. The results uncover the pre… ▽ More Induced by quenched disorder, random-singlet states occur in a variety of low-dimensional spin-1/2 antiferromagnets, some of them candidates for quantum spin liquids. Here we report measurements of the specific heat, magnetization, and magnetic susceptibility of nanocrystalline Sr21Bi8Cu2(CO3)2O41, a quasi-one-dimensional spin-1/2 antiferromagnet with alternating bonds. The results uncover the predominant presence of random-singlet spin pairs in this material, with a logarithmic probability distribution, P(J), of the renormalized, emergent exchange interaction, J, in zero magnetic field and P(J) proportional to 1/J in magnetic fields. We postulate that these unexpected J dependences, in contrast to the usual P(J) \propto 1/$J^γ$ with 0 < $γ$ < 1, and possibly also the dichotomy, arise from the finite size of the nanocrystals. Scaling functions for the specific heat and magnetization reproduce our magnetocaloric-effect data, with no adjustable parameters. △ Less

Submitted 10 September, 2023; v1 submitted 30 August, 2023; originally announced August 2023.

Absence of Tc-Pinning Phenomenon Under High Pressure in High-Entropy REO0.5F0.5BiS2 Layered Superconductor

Authors: Yoshikazu Mizuguchi, Kazuki Yamane, Ryo Matsumoto, Kazuhisa Hoshi, Aichi Yamashita, Akira Miura, Yuki Nakahira, Hirokazu Kadobayashi, Saori I. Kawaguchi, Yoshihiko Takano

Abstract: Recently, robustness of superconductivity (transition temperature, Tc) under high pressures has been observed in high-entropy alloy (HEA), bcc-type Ti-Zr-Hf-Nb-Ta, and HEA-type compounds (Ag,In,Sn,Pb,Bi)Te with a NaCl-type structure. Since those materials have three-dimensional crystal structure, investigation on the pressure dependence of Tc of low-dimensional materials is needed to understand th… ▽ More Recently, robustness of superconductivity (transition temperature, Tc) under high pressures has been observed in high-entropy alloy (HEA), bcc-type Ti-Zr-Hf-Nb-Ta, and HEA-type compounds (Ag,In,Sn,Pb,Bi)Te with a NaCl-type structure. Since those materials have three-dimensional crystal structure, investigation on the pressure dependence of Tc of low-dimensional materials is needed to understand the phenomena. Here, we investigated the superconducting properties and the crystal structure of BiS2-based layered system REO0.5F0.5BiS2. Although the robustness of Tc was induced in MTe with increasing M-site configurational entropy, the increase in RE-site configurational entropy does not induce robustness of Tc under high pressures in REO0.5F0.5BiS2. The crystal structure of HEA-type REO0.5F0.5BiS2 was confirmed as monoclinic P21/m, which is the same space group as the zero-entropy counterpart LaO0.5F0.5BiS2. The results suggest that an increase in configurational entropy at blocking layers do not affect crystal structure and superconducting properties under high pressures in the BiS2-based layered system. △ Less

Submitted 11 September, 2023; v1 submitted 8 August, 2023; originally announced August 2023.

Comments: 10 pages, 4 figures, to appear in JPSJ

Experimental exploration of ErB$_2$ and SHAP analysis on a machine-learned model of magnetocaloric materials for materials design

Authors: Kensei Terashima, Pedro Baptista de Castro, Akiko T Saito, Takafumi D Yamamoto, Ryo Matsumoto, Hiroyuki Takeya, Yoshihiko Takano

Abstract: Stimulated by a recent report of a giant magnetocaloric effect in HoB$_2$ found via machine-learning predictions, we have explored the magnetocaloric properties of a related compound ErB$_2$, that has remained the last ferromagnetic material among the rare-earth diboride (REB$_2$) family with unreported magnetic entropy change |ΔSM|. The evaluated $|ΔS_M|$ at field change of 5 T in ErB$_2$ turned… ▽ More Stimulated by a recent report of a giant magnetocaloric effect in HoB$_2$ found via machine-learning predictions, we have explored the magnetocaloric properties of a related compound ErB$_2$, that has remained the last ferromagnetic material among the rare-earth diboride (REB$_2$) family with unreported magnetic entropy change |ΔSM|. The evaluated $|ΔS_M|$ at field change of 5 T in ErB$_2$ turned out to be as high as 26.1 (J kg$^{-1}$ K$^{-1}$) around the ferromagnetic transition (${T_C}$) of 14 K. In this series, HoB$_2$ is found to be the material with the largest $|ΔS_M|$ as the model predicted, while the predicted values showed a deviation with a systematic error compared to the experimental values. Through a coalition analysis using SHAP, we explore how this rare-earth dependence and the deviation in the prediction are deduced in the model. We further discuss how SHAP analysis can be useful in clarifying favorable combinations of constituent atoms through the machine-learned model with compositional descriptors. This analysis helps us to perform materials design with aid of machine learning of materials data. △ Less

Submitted 26 June, 2023; originally announced June 2023.

Comments: 9 pages, 10 figures. Accepted manuscript. Published by Taylor & Francis in STAM:Methods, available at https://doi.org/10.1080/27660400.2023.2217474

Journal ref: Science and Technology of Advanced Materials: Methods 3:1, 2217474 (2023)

Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C$_{2}$H$_{5}$)$_{3}$NH]$_{2}$Cu$_{2}$(C$_{2}$O$_{4}$)$_{3}$

Authors: C. Dissanayake, A. C. Jacko, K. Kumarasinghe, R. Munir, H. Siddiquee, W. J. Newsome, F. J. Uribe-Romo, E. S. Choi, S. Yadav, X. -Z. Hu, Y. Takano, S. Pakhira, D. C. Johnston, Q. -P. Ding, Y. Furukawa, B. J. Powell, Y. Nakajima

Abstract: We report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin liquid candidate: the hyper-honeycomb Cu oxalate framework compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$. The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to $T\sim$ 180 mK in zero magnetic field. We observe a large linear-in-$T$ contri… ▽ More We report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin liquid candidate: the hyper-honeycomb Cu oxalate framework compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$. The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to $T\sim$ 180 mK in zero magnetic field. We observe a large linear-in-$T$ contribution to the specific heat $γT$, $γ= 98(1)$ mK/mol K$^{2}$, at low temperatures, indicative of the presence of fermionic excitations despite the Mott insulating state. The low-$T$ specific heat is strongly suppressed by applied magnetic fields $H$, which induce an energy gap, $Δ(H)$, in the spin-excitation spectrum. We use the four-component relativistic density-functional theory (DFT) to calculate the magnetic interactions, including the Dzyaloshinskii-Moriya antisymmetric exchange, which causes an effective staggered field acting on one copper sublattice. The magnitude and field dependence of the field-induced gap, $Δ(H) \propto H^{2/3}$, are accurately predicted by the soliton mass calculated from the sine-Gordon model of weakly coupled antiferromagnetic Heisenberg chains with all parameters determined by our DFT calculations. Thus our experiment and calculations are entirely consistent with a model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ in which anisotropic magnetic exchange interactions due to Jahn-Teller distortion cause one copper sublattice to dimerize, leaving a second sublattice of weakly coupled antiferromagnetic chains. We also show that this model quantitatively accounts for the measured temperature-dependent magnetic susceptibility. Thus [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ is a canonical example of a one-dimensional spin-1/2 Heisenberg antiferromagnet and not a resonating-valence-bond quantum spin liquid, as previously proposed. △ Less

Submitted 23 June, 2023; originally announced June 2023.

Comments: 8 pages, 6 figures

Journal ref: Phys. Rev. B 108, 134418 (2023)

Coexistence of symmetry-protected topological order and Neel order in the spin-1/2 ladder antiferromagnet C9H18N2CuBr4

Authors: Tao Hong, Imam Makhfudz, Xianglin Ke, Andrew F. May, Andrey A. Podlesnyak, Daniel Pajerowski, Barry Winn, Merce Deumal, Yasumasa Takano, Mark M. Turnbull

Abstract: Topological phases of matter are beyond the paradigm of Landau's symmetry breaking and have challenged our understanding of condensed matter systems. Here we report a new type of symmetry-protected topological phase of matter in the spin-1/2 coupled two-leg ladder antiferromagnet C9H18N2CuBr4, DLCB for short. In this two-sublattice antiferromagnet with a weak easy-axis anisotropy, we find no evide… ▽ More Topological phases of matter are beyond the paradigm of Landau's symmetry breaking and have challenged our understanding of condensed matter systems. Here we report a new type of symmetry-protected topological phase of matter in the spin-1/2 coupled two-leg ladder antiferromagnet C9H18N2CuBr4, DLCB for short. In this two-sublattice antiferromagnet with a weak easy-axis anisotropy, we find no evidence of a conventional spin-flop transition in the magnetization with the magnetic field applied parallel to the easy axis at T=0.4 K, well below TN=2.0 K. Moreover, the temperature dependence of the gapped transverse excitations across TN indicates that they are not the conventional S=1 magnons associated with explicit symmetry breaking. Instead, the thermal renormalization of the gap energy shows a remarkable agreement with a calculation for the three-dimensional O(3) nonlinear sigma model. Accordingly, the spin gap in DLCB is not due to the spin anisotropy but to the separation between a spin singlet state and a triplet excited state. Since an antiferromagnetic spin-1/2 ladder systems can be mapped onto the spin-1 chain, the notion of the Haldane gap is proposed to explain the opening of the spin gap in DLCB. Therefore, the ground state of DLCB is best described as a quantum superposition of a Haldane phase and a Neel-ordered phase, which resembles the quantum state of a qubit in quantum computing. Our results indicate the presence of a symmetry-protected topological order coexisting with an antiferromagnetic order in this material. △ Less

Submitted 16 February, 2024; v1 submitted 9 June, 2023; originally announced June 2023.

Comments: 4 figures in the main text and 9 figures in the Supplementary Material. Any comments are welcome

Effects of equivalent composition on superconducting properties of high-entropy REOBiS$_2$ (RE = La, Ce, Pr, Nd, Sm, Gd) single crystals

Authors: Yuma Fujita, Masanori Nagao, Akira Miura, Daisuke Urushihara, Yoshikazu Mizuguchi, Yuki Maruyama, Satoshi Watauchi, Yoshihiko Takano, Isao Tanaka

Abstract: Superconductors are influenced by high-entropy alloys (HEAs); these have been investigated in various functional materials. REOBiS$_2$ (RE = La, Ce, Pr, Nd, Sm, and Gd in different combinations) single crystals with HEAs at the RE-site were successfully grown using the flux method. The obtained crystals were plate-shaped (1 mm$^2$) with a well-developed c-plane. Ce was present in both trivalent (C… ▽ More Superconductors are influenced by high-entropy alloys (HEAs); these have been investigated in various functional materials. REOBiS$_2$ (RE = La, Ce, Pr, Nd, Sm, and Gd in different combinations) single crystals with HEAs at the RE-site were successfully grown using the flux method. The obtained crystals were plate-shaped (1 mm$^2$) with a well-developed c-plane. Ce was present in both trivalent (Ce$^{3+}$) and tetravalent (Ce$^{4+}$) electronic configurations; the concentration of Ce$^{4+}$ at the RE-site was approximately 10 at% in all single crystals. The single crystals showed superconducting transition temperature with zero resistivity within 1.2-4.2 K. The superconducting transition temperature, superconducting anisotropy, electronic specific heat coefficient, and Debye temperature of the crystals were not correlated with the mixed entropy at the RE-site. Except for the electronic specific heat coefficient, the variation of these parameters as a function of mixed entropy showed different trends for equivalent and non-equivalent RE element compositions. Thus, the configuration of RE elements influences the superconducting properties of REOBiS$_2$ single crystals, alluding to a method of modulating transition temperatures. △ Less

Submitted 11 April, 2023; originally announced April 2023.

Journal ref: Physica C, vol.608 (2023) 1354254

Tunable magnetic and magnetocaloric properties by thermal annealing in ErCo2 atomized particles

Authors: Takafumi D. Yamamoto, Akiko T. Saito, Hiroyuki Takeya, Kensei Terashima, Takenori Numazawa, Yoshihiko Takano

Abstract: Processing magnetocaloric materials into magnetic refrigerants with appropriate shapes is essential for the development of magnetic refrigeration systems. In this context, the impact of processing on the physical properties of magnetocaloric materials is one of the important issues. Here, we investigate the crystallographic, magnetic, and magnetocaloric properties of gas-atomized particles of the… ▽ More Processing magnetocaloric materials into magnetic refrigerants with appropriate shapes is essential for the development of magnetic refrigeration systems. In this context, the impact of processing on the physical properties of magnetocaloric materials is one of the important issues. Here, we investigate the crystallographic, magnetic, and magnetocaloric properties of gas-atomized particles of the intermetallic compound ErCo$_{2}$, a giant magnetocaloric material for low-temperature applications. The results demonstrate that the physical properties of ErCo$_{2}$ are significantly changed by atomization and subsequent thermal annealing. In the as-atomized particles, the magnetic transition temperature increases from 34 to 56 K and the phase transition changes from first order to second order. The thermal annealing shifts the transition temperature back to the original one and restores the first-order phase transition characteristic. The changes in magnetic properties are closely related to those in crystallographic properties, suggesting the importance of the magneto-structural coupling. The magnetic entropy change $-ΔS_{M}$ of the particles can be tuned in size, shape, and peak temperature depending on the annealing conditions. The peak value of $-ΔS_{M}$ varies in the range of 9--33 J kg$^{-1}$ K$^{-1}$ for a magnetic field change of 0--5 T. All the ErCo$_{2}$ atomized particles have magnetocaloric properties comparable or superior to other promising candidates for low-temperature magnetic refrigerants. △ Less

Submitted 15 November, 2022; originally announced November 2022.

Comments: Journal of Alloys and Compounds (in press)

Journal ref: J. Alloys Compd. 935, 168040 (2023)

Automatic extraction of materials and properties from superconductors scientific literature

Authors: Luca Foppiano, Pedro Baptista de Castro, Pedro Ortiz Suarez, Kensei Terashima, Yoshihiko Takano, Masashi Ishii

Abstract: The automatic extraction of materials and related properties from the scientific literature is gaining attention in data-driven materials science (Materials Informatics). In this paper, we discuss Grobid-superconductors, our solution for automatically extracting superconductor material names and respective properties from text. Built as a Grobid module, it combines machine learning and heuristic a… ▽ More The automatic extraction of materials and related properties from the scientific literature is gaining attention in data-driven materials science (Materials Informatics). In this paper, we discuss Grobid-superconductors, our solution for automatically extracting superconductor material names and respective properties from text. Built as a Grobid module, it combines machine learning and heuristic approaches in a multi-step architecture that supports input data as raw text or PDF documents. Using Grobid-superconductors, we built SuperCon2, a database of 40324 materials and properties records from 37700 papers. The material (or sample) information is represented by name, chemical formula, and material class, and is characterized by shape, doping, substitution variables for components, and substrate as adjoined information. The properties include the Tc superconducting critical temperature and, when available, applied pressure with the Tc measurement method. △ Less

Submitted 22 November, 2022; v1 submitted 25 October, 2022; originally announced October 2022.

Comments: 20 pages, 11 figures, 8 tables

Journal ref: STAM:M, 2023, VOL. 3, NO. 1, 2153633

Polarization analysis of terahertz emission from Bi-2212 cross-whisker intrinsic Josephson junction and its refractive index

Authors: Yoshito Saito, Istuhiro Kakeya, Yoshihiko Takano

Abstract: Polarization analyses of the terahertz (THz) emission from Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ whisker crystals used for superconducting THz emitters were conducted. The THz emission mode was estimated by a simple polarization measurement, and a simulation study was conducted to examine the validity of the polarization analysis. The refractive index of whisker crystals revealed through the polariz… ▽ More Polarization analyses of the terahertz (THz) emission from Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ whisker crystals used for superconducting THz emitters were conducted. The THz emission mode was estimated by a simple polarization measurement, and a simulation study was conducted to examine the validity of the polarization analysis. The refractive index of whisker crystals revealed through the polarization analyses was greater than that of bulk single crystals and agreed well with our previous THz emission report. The simulation study suggested the complex plasma excitation mode of the THz emission, and an interpretation of the refractive index obtained in this study is provided. △ Less

Submitted 24 October, 2022; v1 submitted 18 September, 2022; originally announced September 2022.

Comments: Submitted to Applied Physics Letters (Accepted: 24 Oct 2022)

Glassy atomic vibrations and blurry electronic structures created by local structural disorders in high-entropy metal telluride superconductors

Authors: Yoshikazu Mizuguchi, Hidetomo Usui, Rei Kurita, Kyohei Takae, Md. Riad Kasem, Ryo Matsumoto, Kazuki Yamane, Yoshihiko Takano, Yuki Nakahira, Aichi Yamashita, Yosuke Goto, Akira Miura, Chikako Moriyoshi

Abstract: The motivation of this work is our recent observation of the robustness of superconductivity in a High-entropy (HE) superconductor Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te (CsCl-type) to external pressure. The superconducting transition temperature (Tc) of Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te is almost constant with pressure, described as robustness of superconductivity to pressure, whereas the PbTe with zero configura… ▽ More The motivation of this work is our recent observation of the robustness of superconductivity in a High-entropy (HE) superconductor Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te (CsCl-type) to external pressure. The superconducting transition temperature (Tc) of Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te is almost constant with pressure, described as robustness of superconductivity to pressure, whereas the PbTe with zero configurational entropy of mixing exhibits a clear decrease in Tc with pressure. Here, we investigated the atomic displacement parameters (Uiso), the atomic-vibration characteristics, and the electronic states of metal tellurides (MTe) with various configurational entropy of mixing (DSmix) at the M site. The Uiso for the M site is clearly increased by M-site alloying with DSmix > 1.1R, which is the evidence of local disorder introduced by the increase in DSmix via the solution of three or more M elements. The revealed vibrational density of states (DOS) shows a remarkable broadening with DSmix > 1.1R, which indicates glassy characteristics of atomic vibration in HE MTe with a NaCl-type structure (low-pressure phase). On the electronic states of the CsCl-type (high-pressure) phases, where the robustness of Tc is observed, blurry electronic band structure appears with increasing DSmix, which indicates the evolution of blurry (glassy) electronic states in HE MTe with the CsCl-type structure. The estimated electronic DOS at Fermi energy cannot explain the changes in Tc for HE MTe when assuming conventional electron-phonon superconductivity, but the conventional explanation seems to work for PbTe. Therefore, the pairing mechanisms in MTe with DSmix > 1.1R are affected by glassy phonon and/or blurry electronic states in MTe, and the robustness of superconductivity would be originating from unique electron-phonon coupling. △ Less

Submitted 5 September, 2022; originally announced September 2022.

Comments: 25 pages, 5 figures, Supplemental Information

Magnetic, thermal, and magnetocaloric properties of the holmium trialuminide HoAl$_{3}$ with polytypic phases

Authors: Takafumi D. Yamamoto, Pedro Baptista de Castro, Kensei Terashima, Akiko T. Saito, Hiroyuki Takeya, Yoshihiko Takano

Abstract: We investigate the magnetic, thermal, and magnetocaloric properties of the intermetallic HoAl$_{3}$ compounds with two different crystal structures. The room-temperature equilibrium trigonal phase HoAl$_{3}$ undergoes an antiferromagnetic (AFM) transition at the Neel temperature $T^{\rm tri}_{\rm N} =$ 9.8 K. The AFM ordering of the compound is strong against the magnetic field, so that inverse ma… ▽ More We investigate the magnetic, thermal, and magnetocaloric properties of the intermetallic HoAl$_{3}$ compounds with two different crystal structures. The room-temperature equilibrium trigonal phase HoAl$_{3}$ undergoes an antiferromagnetic (AFM) transition at the Neel temperature $T^{\rm tri}_{\rm N} =$ 9.8 K. The AFM ordering of the compound is strong against the magnetic field, so that inverse magnetocaloric effect (MCE) is found even under a magnetic field change of 0-50 kOe. The high-pressure cubic phase HoAl3, prepared by a rapid-solidification process, is antiferromagnetically ordered below $T^{\rm cub}_{\rm N} =$ 15 K. Magnetic and specific heat measurements reveal that this long-range AFM state becomes unstable as the temperature drops and then it is replaced by a magnetic glassy state below a spin freezing temperature $T_{\rm f} =$ 11 K. The successive changes in magnetic state result in complicated temperature and field dependence of the MCE at low temperatures. △ Less

Submitted 8 August, 2022; originally announced August 2022.

Comments: Journal of Magnetism and Magnetic Materials Accepted

Journal ref: J. Magn. Magn. Mater. 562 (2022) 169801

Neural networks for a quick access to a digital twin of scanning physical properties measurements

Authors: Kensei Terashima, Pedro Baptista de Castro, Miren Garbiñe Esparza Echevarria, Ryo Matsumoto, Takafumi D Yamamoto, Akiko T Saito, Hiroyuki Takeya, Yoshihiko Takano

Abstract: For performing successful measurements within limited experimental time, efficient use of preliminary data plays a crucial role. This work shows that a simple feedforward type neural networks approach for learning preliminary experimental data can provide quick access to simulate the experiment within the learned range. The approach is especially beneficial for physical properties measurements wit… ▽ More For performing successful measurements within limited experimental time, efficient use of preliminary data plays a crucial role. This work shows that a simple feedforward type neural networks approach for learning preliminary experimental data can provide quick access to simulate the experiment within the learned range. The approach is especially beneficial for physical properties measurements with scanning on multiple axes, where derivative or integration of data are required to obtain the objective quantity. Due to its simplicity, the learning process is fast enough for the users to perform learning and simulation on-the-fly by using a combination of open-source optimization techniques and deep-learning libraries. Here such a tool for augmenting the experimental data is proposed, aiming to help researchers to decide the most suitable experimental conditions before performing costly experiments in real. Furthermore, this tool can also be used from the perspective of taking advantage of reutilizing and repurposing previously published data, accelerating data-driven exploration of functional materials. △ Less

Submitted 22 June, 2022; originally announced June 2022.

Comments: 19 pages, 5 figures + 7 pages of Supporting Information

Journal ref: Digital Discovery, Advance article (2023)

Effect of Non-stoichiometry on Magnetocaloric Properties of HoB2 Gas-Atomized Particles

Authors: Takafumi D. Yamamoto, Takeya Hiroyuki, Pedro Baptista de Castro, Akiko T. Saito, Kensei Terashima, Takenori Numazawa, Yoshihiko Takano

Abstract: We fabricate gas-atomized particles by inductively melting electrode rods of HoB2-x (x = -0.3, 0, 0.3, and 1.0) and investigate the effect of non-stoichiometry on the phase fraction, microstructure, and physical properties. Shifting the stoichiometric ratio of the electrode rod to the B (Ho)-rich side increases HoB4 (Ho) phase in the resulting atomized particles. Even if the atomized particles con… ▽ More We fabricate gas-atomized particles by inductively melting electrode rods of HoB2-x (x = -0.3, 0, 0.3, and 1.0) and investigate the effect of non-stoichiometry on the phase fraction, microstructure, and physical properties. Shifting the stoichiometric ratio of the electrode rod to the B (Ho)-rich side increases HoB4 (Ho) phase in the resulting atomized particles. Even if the atomized particles contain 15-20 weight percent (wt.%) of the impurity phase, the influence of which on the physical properties is less severe: the maximum value of the magnetic entropy change is only reduced by 10% compared to HoB2.0 particles. We further find that the ductile Ho phase exists so as to fill the space between the brittle HoB2 phases in the atomized particles, which may be beneficial to the mechanical properties of the particles. Our findings suggest that it would be better to use the Ho-rich electrode rods than the stoichiometric ones to produce HoB2-x particles with more suitable properties as a magnetic refrigerant for magnetic refrigeration systems. △ Less

Submitted 26 May, 2022; originally announced May 2022.

Journal ref: IEEE Transactions on Magnetics 58 (2022) 2501406

Magnetocaloric particles of the Laves phase compound HoAl2 prepared by electrode induction melting gas atomization

Authors: Takafumi D. Yamamoto, Hiroyuki Takeya, Akiko T. Saito, Kensei Terashima, Takenori Numazawa, Yoshihiko Takano

Abstract: Processing magnetocaloric materials into magnetic refrigerant particles is an essential issue in developing high-performance magnetic refrigerators. Here, we succeed in stably producing magnetocaloric particles of the promising material HoAl2 by a newly devised method based on electrode induction melting gas atomization process. The particle size range is on the order of submillimeter, which is su… ▽ More Processing magnetocaloric materials into magnetic refrigerant particles is an essential issue in developing high-performance magnetic refrigerators. Here, we succeed in stably producing magnetocaloric particles of the promising material HoAl2 by a newly devised method based on electrode induction melting gas atomization process. The particle size range is on the order of submillimeter, which is suitable for practical refrigeration systems. The resulting particles with less contamination have good morphological, magnetic, and magnetocaloric properties: (i) almost spherical shapes with few internal pores, (ii) a sharp ferromagnetic transition around 30 K, and (iii) a large magnetocaloric effect comparable to the bulk counterpart. These features suggest the HoAl$_{2}$ gas-atomized particles have the potential of use as a magnetic refrigerant. The presented method can be applied not only to HoAl2 but also to other brittle magnetocaloric materials with high melting points, facilitating the production of various magnetic refrigerants needed to develop magnetic refrigerators for hydrogen liquefaction. △ Less

Submitted 25 April, 2022; originally announced April 2022.

Journal ref: J. Magn. Magn. Mater. 547 (2022) 168906

Gas-atomized particles of giant magnetocaloric compound HoB2 for magnetic hydrogen liquefiers

Authors: Takafumi D. Yamamoto, Hiroyuki Takeya, Akiko T. Saito, Kensei Terashima, Pedro Baptista de Castro, Takenori Numazawa, Yoshihiko Takano

Abstract: The processing of promising magnetocaloric materials into spheres is one of the important issues on developing high-performance magnetic refrigeration systems. In the present study, we achieved in producing spherical particles of a giant magnetocaloric compound HoB2 by a crucible-free gas atomization process, despite its high melting point of 2350 C. The particle size distribution ranges from 100… ▽ More The processing of promising magnetocaloric materials into spheres is one of the important issues on developing high-performance magnetic refrigeration systems. In the present study, we achieved in producing spherical particles of a giant magnetocaloric compound HoB2 by a crucible-free gas atomization process, despite its high melting point of 2350 C. The particle size distribution ranges from 100 to 710 micrometers centered at 212-355 micrometers with the highest yield of 14-20wt% of total melted electrode, which is suitable for magnetic refrigeration systems. The majority of the resulting particles are mostly spherical with no contamination during the processing, while unique microstructures are observed on the surface and inside. These spherical particles exhibit sharp magnetic transitions and huge magnetic entropy change of 0.34 J cm^{-3} K^{-1} for a magnetic field change of 5 T at 15.5 K. The high sphericality and the high magnetocaloric performance suggest that the HoB2 gas-atomized particles have good potential as magnetic refrigerants for use in magnetic refrigerators for hydrogen liquefaction. △ Less

Submitted 22 April, 2022; originally announced April 2022.

Comments: 6pages(double column), 6 figures

Journal ref: Applied Physics A 127, 301 (2021)

Adiabatic temperature change in ErAl2/metal PIT wires: A practical method for estimating the magnetocaloric response of magnetocaloric composites

Authors: Takafumi D. Yamamoto, Hiroyuki Takeya, Kensei Terashima, Suguru Iwasaki, Pedro Baptista de Castro, Takenori Numazawa, Yoshihiko Takano

Abstract: We report the adiabatic temperature change in ErAl2 magnetocaloric wires fabricated by a powder-in-tube (PIT) process. The adiabatic temperature change of the PIT wires is found to be determined by not only the volume fraction of ErAl2 core but also the magnitude relationship between the specific heat of the ErAl2 core and the metal sheath. We propose a quantitative analysis method for calculating… ▽ More We report the adiabatic temperature change in ErAl2 magnetocaloric wires fabricated by a powder-in-tube (PIT) process. The adiabatic temperature change of the PIT wires is found to be determined by not only the volume fraction of ErAl2 core but also the magnitude relationship between the specific heat of the ErAl2 core and the metal sheath. We propose a quantitative analysis method for calculating the temperature and core volume fraction dependence of adiabatic temperature change in the PIT wire, whose formula is applicable to also various magnetocaloric composites, useful to estimate the magnetocaloric response prior to fabrication. △ Less

Submitted 20 April, 2022; originally announced April 2022.

Comments: 14 pages, 5 figures

Journal ref: Journal of Magnetism and Magnetic Materials 513 (2020) 167207

Investigation of superconductivity in Ce-doped (La,Pr)OBiS2 single crystals

Authors: Masanori Nagao, Yuji Hanada, Akira Miura, Yuki Maruyama, Satoshi Watauchi, Yoshihiko Takano, Isao Tanaka

Abstract: Single crystals of Ce-doped (La,Pr)OBiS2 superconductors, multinary rare-earth elements substituted ROBiS2, were successfully grown. The grown crystals typically had a size of 1-2 mm and a plate-like shape with a well-developed c-plane. The c-axis lattice constants of the obtained (La,Ce,Pr)OBiS2 single crystals were approximately 13.6-13.7 A, and the superconducting transition temperature was 1.2… ▽ More Single crystals of Ce-doped (La,Pr)OBiS2 superconductors, multinary rare-earth elements substituted ROBiS2, were successfully grown. The grown crystals typically had a size of 1-2 mm and a plate-like shape with a well-developed c-plane. The c-axis lattice constants of the obtained (La,Ce,Pr)OBiS2 single crystals were approximately 13.6-13.7 A, and the superconducting transition temperature was 1.23-2.18 K. Valence fluctuations of Ce and Pr were detected through X-ray absorption spectroscopy analysis. In contrast to (Ce,Pr)OBiS2 and (La,Ce)OBiS2, the superconducting transition temperature of (La,Ce,Pr)OBiS2 increased with increasing concentrations of the tetravalent state at the R-site. △ Less

Submitted 19 April, 2022; originally announced April 2022.

Journal ref: Materials, vol.15 (2022) 2977

Lattice Anharmonicity in BiS2-Based Layered Superconductor RE(O,F)BiS2 (RE = La, Ce, Pr, Nd)

Authors: Fysol Ibna Abbas, Kazuhisa Hoshi, Aichi Yamashita, Yuki Nakahira, Yosuke Goto, Akira Miura, Chikako Moriyoshi, Yoshihiro Kuroiwa, Kensei Terashima, Ryo Matsumoto, Yoshihiko Takano, Yoshikazu Mizuguchi

Abstract: We studied Grüneisen parameter (γG) to investigate lattice anharmonicity in a layered BiS2-based superconductor system REO1-xFxBiS2 (RE = La, Ce, Pr, Nd), where in-plane chemical pressure was tuned by substituting the RE elements. With increasing in-plane chemical pressure, bulk modulus remarkably increases, and a high γG is observed for RE = Nd. The dependence of γG on in-plane chemical pressure… ▽ More We studied Grüneisen parameter (γG) to investigate lattice anharmonicity in a layered BiS2-based superconductor system REO1-xFxBiS2 (RE = La, Ce, Pr, Nd), where in-plane chemical pressure was tuned by substituting the RE elements. With increasing in-plane chemical pressure, bulk modulus remarkably increases, and a high γG is observed for RE = Nd. The dependence of γG on in-plane chemical pressure exhibits a good correlation with Tc, and a higher Tc is achieved when γG is large for RE = Nd. In addition, γG shows a slight decrease by a decrease of F concentration (x) in REO1-xFxBiS2. Our results show that the anharmonic vibration of Bi along the c-axis is present in REO1-xFxBiS2, and the enhancement of the anharmonicity is positively linked to superconducting Tc and pairing mechanisms. △ Less

Submitted 22 March, 2022; originally announced March 2022.

Comments: 15 pages, 5 figures

Journal ref: J. Phys. Soc. Jpn. 91, 074706 (2022)

Estimation of Grüneisen parameter of high-entropy-alloy-type functional materials

Authors: F. I. Abbas, Y. Nakahira, A. Yamashita, Md. R. Kasem, M. Yoshida, Y. Goto, A. Miura, K. Terashima, R. Matsumoto, Y. Takano, C. Moriyoshi, Y. Mizuguchi

Abstract: In functional materials like thermoelectric materials and superconductors, the interplay between functionality, electronic structure, and phonon characteristics is one of the key factors to improve functionality and to understand the mechanisms. In the first part of this article, we briefly review investigations on lattice anharmonicity in functional materials by Grüneisen parameter (γG). One can… ▽ More In functional materials like thermoelectric materials and superconductors, the interplay between functionality, electronic structure, and phonon characteristics is one of the key factors to improve functionality and to understand the mechanisms. In the first part of this article, we briefly review investigations on lattice anharmonicity in functional materials by Grüneisen parameter (γG). One can find that the γG can be a good scale for large lattice anharmonicity and for detecting a change in anharmonicity amplitude in functional materials. Then, we show original results on estimation of γG for recently-developed high-entropy-alloy-type (HEA-type) functional materials with a layered structure and a NaCl-type structure. As a common trend between those two systems with two- and three-dimensional structures, we find that γG increases by a slight increase in configurational entropy of mixing (ΔSmix), and then γG decreases with increasing ΔSmix in high-entropy region. △ Less

Submitted 25 February, 2022; originally announced February 2022.

Comments: 11 pages, 5 figures

Journal ref: Condens. Matter 7, 34 (2022)

High-pressure synthesis of superconducting Sn$_{3}$S$_{4}$ using diamond anvil cell with boron-doped diamond heater

Authors: Ryo Matsumoto, Kensei Terashima, Satoshi Nakano, Kazuki Nakamura, Sayaka Yamamoto, Takafumi D. Yamamoto, Takahiro Ishikawa, Shintaro Adachi, Tetsuo Irifune, Motoharu Imai, Yoshihiko Takano

Abstract: High-pressure techniques open exploration of functional materials in broad research fields. An established diamond anvil cell with a boron-doped diamond heater and transport measurement terminals has performed the high-pressure synthesis of a cubic Sn$_{3}$S$_{4}$ superconductor. X-ray diffraction and Raman spectroscopy reveal that the Sn$_{3}$S$_{4}$ phase is stable in the pressure range of P>5 G… ▽ More High-pressure techniques open exploration of functional materials in broad research fields. An established diamond anvil cell with a boron-doped diamond heater and transport measurement terminals has performed the high-pressure synthesis of a cubic Sn$_{3}$S$_{4}$ superconductor. X-ray diffraction and Raman spectroscopy reveal that the Sn$_{3}$S$_{4}$ phase is stable in the pressure range of P>5 GPa in a decompression process. Transport measurement terminals in the diamond anvil cell detect a metallic nature and superconductivity in the synthesized Sn$_{3}$S$_{4}$ with a maximum onset transition temperature of 13.3 K at 5.6 GPa. The observed pressure-T$_{c}$ relationship is consistent with that from the first-principles calculation. The observation of superconductivity in Sn$_{3}$S$_{4}$ opens further materials exploration under high temperature and pressure conditions. △ Less

Submitted 14 February, 2022; originally announced February 2022.

Protonation-induced discrete superconducting phases in bulk FeSe single crystals

Authors: Yan Meng, Xiangzhuo Xing, Xiaolei Yi, Bin Li, Nan Zhou, Meng Li, Yufeng Zhang, Wei Wei, Jiajia Feng, Kensei Terashima, Yoshihiko Takano, Yue Sun, Zhixiang Shi

Abstract: The superconducting transition temperature, $T_{\rm{c}}$, of FeSe can be significantly enhanced several-fold by applying pressure, electron doping, intercalating spacing layer, and reducing dimensionality. Various ordered electronic phases, such as nematicity and spin density waves, have also been observed accompanying high-$T_{\rm{c}}$ superconductivity. Investigation on the evolution of the elec… ▽ More The superconducting transition temperature, $T_{\rm{c}}$, of FeSe can be significantly enhanced several-fold by applying pressure, electron doping, intercalating spacing layer, and reducing dimensionality. Various ordered electronic phases, such as nematicity and spin density waves, have also been observed accompanying high-$T_{\rm{c}}$ superconductivity. Investigation on the evolution of the electronic structure with $T_{\rm{c}}$ is essential to understanding electronic behavior and high-$T_{\rm{c}}$ superconductivity in FeSe and its derived superconductors. In this report, we have found a series of discrete superconducting phases, with a maximum $T_{\rm{c}}$ up to 44 K, in H$^+$-intercalated FeSe single crystals using an ionic liquid gating method. Accompanied with the increase of $T_{\rm{c}}$, suppression of the nematic phase and evolution from non-Fermi-liquid to Fermi-liquid behavior was observed. An abrupt change in the Fermi surface topology was proposed to explain the discrete superconducting phases. A band structure that favors the high-$T_{\rm{c}}$ superconducting phase was also revealed. △ Less

Submitted 23 December, 2021; originally announced December 2021.

Comments: 23 pages, 8 figures

Journal ref: Physical Review B 105, 134506 (2022)

Robustness of superconductivity to external pressure in high-entropy-alloy-type metal telluride AgInSnPbBiTe5

Authors: Md. Riad Kasem, Yuki Nakahira, Hitoshi Yamaoka, Ryo Matsumoto, Aichi Yamashita, Hirofumi Ishii, Nozomu Hiraoka, Yoshihiko Takano, Yosuke Goto, Yoshikazu Mizuguchi

Abstract: High-entropy-alloy (HEA) superconductors are a new class of disordered superconductors. In this study, we investigate the robustness of superconducting states in HEA-type metal telluride (MTe; M = Ag, In, Sn, Pb, Bi) under high pressure. PbTe exhibits a structural transition from a NaCl-type to an orthorhombic Pnma structure at low pressures, and further transitions to a CsCl-type structure at hig… ▽ More High-entropy-alloy (HEA) superconductors are a new class of disordered superconductors. In this study, we investigate the robustness of superconducting states in HEA-type metal telluride (MTe; M = Ag, In, Sn, Pb, Bi) under high pressure. PbTe exhibits a structural transition from a NaCl-type to an orthorhombic Pnma structure at low pressures, and further transitions to a CsCl-type structure at high pressures. When the superconductivity of the CsCl-type PbTe is observed, it is found that its superconducting transition temperature (Tc) decreases with pressure. However, in the HEA-type AgInSnPbBiTe5, Tc is almost independent of pressure, for pressures ranging from 13.0 to 35.1 GPa. This trend is quite similar to that observed in an HEA superconductor (TaNb)0.67(HfZrTi)0.33, which shows that the robustness of superconductivity to external pressure is a universal feature in HEA-type superconductors. To clarify the effects of the modification of the configurational entropy of mixing on the crystal structure, superconducting states, and electronic structure of MTe, electrical resistance measurements, synchrotron X-ray diffraction, and synchrotron X-ray absorption spectroscopy with partial fluorescence mode (PFY-XAS) for three MTe polycrystalline samples of PbTe, AgPbBiTe3, and AgInSnPbBiTe5 with different configurational entropies of mixing at the M site were performed. △ Less

Submitted 13 December, 2021; originally announced December 2021.

Comments: 22 pages, 4 figures, supporting information

Journal ref: Sci. Rep. 12, 7789 (2022)

XERUS: An open-source tool for quick XRD phase identification and refinement automation

Authors: Pedro Baptista de Castro, Kensei Terashima, Miren Garbiñe Esparza Echevarría, Hiroyuki Takeya, Yoshihiko Takano

Abstract: Analysis of XRD diffraction patterns is one of the keystones of materials science and materials research. With the advancement of data-driven methods for materials design, candidate materials can be quickly screened for the study of a desired physical property. Efficient methods to automatically analyze and identify phases present in a given pattern, are paramount for the success of this new parad… ▽ More Analysis of XRD diffraction patterns is one of the keystones of materials science and materials research. With the advancement of data-driven methods for materials design, candidate materials can be quickly screened for the study of a desired physical property. Efficient methods to automatically analyze and identify phases present in a given pattern, are paramount for the success of this new paradigm. To aid this process, the open source python package Xray Estimation and Refinement Using Similarity (XERUS) for semi-automatic/automatic phase identification is presented. XERUS takes advantages of open crystal structure databases, not relying on proprietary databases, to obtain crystal structures on the fly, being then chemical space agnostic. By wrapping around GSASII, it can automatically simulate patterns and calculate similarity measures used for phase identification. Our approach is simple and quick but also applicable to multiphase identification, by coupling the similarity calculations with quick refinements followed by an iterative peak removal process. XERUS is shown in action in four different experimental datasets and also it is benchmarked against a recently proposed deep learning method for a mixture dataset covering the Li-Mn-O-F chemical space. XERUS will be freely available on https://www.github.com/pedrobcst/Xerus/ △ Less

Submitted 9 December, 2021; originally announced December 2021.

High-pressure Mg-Sc-H phase diagram and its superconductivity from first-principles calculations

Authors: Peng Song, Zhufeng Hou, Pedro Baptista de Castro, Kousuke Nakano, Kenta Hongo, Yoshihiko Takano, Ryo Maezono

Abstract: In this work, global search for crystal structures of ternary Mg-Sc-H hydrides (Mg$_x$Sc$_y$H$_z$) under high pressure ($100 \le P \le 200$ GPa) were performed using the evolutionary algorithm and first-principles calculations. Based on them, we computed the thermodynamic convex hull and pressure-dependent phase diagram of Mg$_x$Sc$_y$H$_z$ for $z/(x+y) < 4$. We have identified the stable crystal… ▽ More In this work, global search for crystal structures of ternary Mg-Sc-H hydrides (Mg$_x$Sc$_y$H$_z$) under high pressure ($100 \le P \le 200$ GPa) were performed using the evolutionary algorithm and first-principles calculations. Based on them, we computed the thermodynamic convex hull and pressure-dependent phase diagram of Mg$_x$Sc$_y$H$_z$ for $z/(x+y) < 4$. We have identified the stable crystal structures of four thermodynamically stable compounds with the higher hydrogen content, i.e., $R\bar{3}m$-MgScH$_{6}$, $C2/m$-Mg$_{2}$ScH$_{10}$, $Immm$-MgSc$_{2}$H$_{9}$ and $Pm\bar{3}m$-Mg(ScH$_{4}$)$_{3}$. Their superconducting transition temperatures were computationally predicted by the McMillan-Allen-Dynes formula combined with first-principles phonon calculations. They were found to exhibit superconductivity; among them, $R\bar{3}m$-MgScH$_{6}$ was predicted to have the highest $T_{c}$ (i.e. 23.34 K) at 200 GPa. △ Less

Submitted 14 September, 2021; originally announced September 2021.

Comments: 7 pages, 5 figures, 1 Supplemental Material

The systematic study on the stability and superconductivity of Y-Mg-H compounds under high pressure

Authors: Peng Song, Zhufeng Hou, Pedro Baptista de Castro, Kousuke Nakano, Kenta Hongo, Yoshihiko Takano, Ryo Maezono

Abstract: Motivated by recent discovery of yttrium-based high-temperature ternary superconducting hydrides (e.g., CaYH$_{12}$, LaYH$_{12}$, and ScYH$_{6}$), we have employed evolutionary algorithm and first-principles calculations to comprehensively examine the structural stability and superconductivity of the YMgH$_{x}$ system at high pressure. The hydrogen content $x$ and the pressure are both important f… ▽ More Motivated by recent discovery of yttrium-based high-temperature ternary superconducting hydrides (e.g., CaYH$_{12}$, LaYH$_{12}$, and ScYH$_{6}$), we have employed evolutionary algorithm and first-principles calculations to comprehensively examine the structural stability and superconductivity of the YMgH$_{x}$ system at high pressure. The hydrogen content $x$ and the pressure are both important factors in the stability of these candidate structures. We find that the stability of hydrogen-rich materials frequently necessitates higher pressure. For instance, the pressures to stabilize $P4/mmm$-YMgH$_{8}$ and $Cmmm$-YMgH$_{12}$ are both more than 250 GPa. Hydrogen-less materials, such as $I4_{1}/amd$-YMgH$_{2}$ and $P6_{3}/mmc$-YMgH$_{3}$, can be stable at pressures as low as 100 GPa. In addition, we find a metastable structure for YMgH$_{6}$ with the same space group as the $P4/mmm$-YMgH$_{8}$. A metastable sodalite-like face-centered cubic (FCC) structure is also found in YMgH$_{12}$. These four clathrate structures of $P4/mmm$-YMgH$_{6}$, $P4/mmm$-YMgH$_{8}$, $Cmmm$-YMgH$_{12}$, and $Fd\bar{3}m$-YMgH$_{12}$ is made up of H14, H18, H24, and H24 cages, respectively, in which the H-H pair exhibits weak covalent bonding. According to phonon calculations, $P4/mmm$-YMgH$_{6}$ and $P4/mmm$-YMgH$_{8}$ require a pressure of 300 GPa to maintain dynamic stability, however $Cmmm$-YMgH$_{12}$ and $Fd\bar{3}m$-YMgH$_{12}$ can maintain dynamic stability at pressures of 200 GPa and 250 GPa, respectively. Electron-phonon coupling calculations indicate that they might be potential high-temperature superconductors, with superconductivity intimately linked to the H cage structure. The sodalite structure $Fd\bar{3}m$-YMgH$_{12}$ has a $T_\mathrm{c}$ value of 190 K and a strong electron-phonon coupling constant of 2.18. △ Less

Submitted 17 July, 2021; v1 submitted 12 July, 2021; originally announced July 2021.

Comments: 7 pages, 5 figures, 1 Supplemental Material

Diamond anvil cell with boron-doped diamond heater for high-pressure synthesis and in-situ transport measurements

Authors: Ryo Matsumoto, Sayaka Yamamoto, Shintaro Adachi, Takeshi Sakai, Tetsuo Irifune, Yoshihiko Takano

Abstract: Temperature and pressure are essential parameters in the synthesis, evaluation, and application of functional materials. This study proposes the addition of a heating function to a high-pressure diamond anvil cell (DAC) with in-situ measurement probes. The proposed DAC allows for simultaneous control of temperature and pressure within the sample space and can be used to synthesize functional mater… ▽ More Temperature and pressure are essential parameters in the synthesis, evaluation, and application of functional materials. This study proposes the addition of a heating function to a high-pressure diamond anvil cell (DAC) with in-situ measurement probes. The proposed DAC allows for simultaneous control of temperature and pressure within the sample space and can be used to synthesize functional materials under extreme conditions. The various components, namely the heater, thermometer, and measurement probes, were fabricated with a boron-doped diamond epitaxial film and could be used repeatedly. The developed DAC was used to successfully conduct the high-pressure annealing of La(O,F)BiS$_{2}$ single crystal and the high-pressure synthesis of EuFBiS$_{2}$ superconductors. The proposed technique shows promise for further exploration of superconductors to broaden the research field. △ Less

Submitted 16 June, 2021; originally announced June 2021.

Pressure-induced superconductivity in TiGeTe$_{6}$

Authors: Sayaka Yamamoto, Ryo Matsumoto, Shintaro Adachi, Kensei Terashima, Hiromi Tanaka, Tetsuo Irifune, Hiroyuki Takeya, Yoshihiko Takano

Abstract: Layered ternary transition-metal chalcogenides have been focused as a vein of exploration for superconductors. In this study, TiGeTe$_{6}$ single crystals were synthesized and characterized by structural and valence state analyses and electrical transport measurements. The transport properties were measured under various pressures up to 71 GPa. The activation energy gets smaller as the applied pre… ▽ More Layered ternary transition-metal chalcogenides have been focused as a vein of exploration for superconductors. In this study, TiGeTe$_{6}$ single crystals were synthesized and characterized by structural and valence state analyses and electrical transport measurements. The transport properties were measured under various pressures up to 71 GPa. The activation energy gets smaller as the applied pressure increases, and a signature of a pressure-induced metallization was observed under around 8.4 GPa. Under 13 GPa, pressure-induced superconductivity was discovered in this compound for the first time, with successive drops at 3 K and 6 K in the resistance, indicating the presence of multiple superconducting transitions. The superconducting transition temperature kept increasing as we further applied the pressure to the TiGeTe$_{6}$ single crystal in the performed pressure range, reaching as high as 8.1 K under 71 GPa. △ Less

Submitted 11 May, 2021; originally announced May 2021.

Crystal Growth and High-Pressure Effects of Bi-Based Superconducting Whiskers

Authors: Ryo Matsumoto, Sayaka Yamamoto, Yoshihiko Takano, Hiromi Tanaka

Abstract: Three growth methods were tested for producing high-transition temperature superconducting Bi$_2$Sr$_2$Ca$_{n-1}$Cu$_n$O$_{2n+4+δ}$ whiskers, employing different ways to focus a compressive stress and size effect of the precursors. First, thermographic imaging was used to investigate thermal stress from temperature distribution in the precursors during growth annealing. To enhance thermal stress i… ▽ More Three growth methods were tested for producing high-transition temperature superconducting Bi$_2$Sr$_2$Ca$_{n-1}$Cu$_n$O$_{2n+4+δ}$ whiskers, employing different ways to focus a compressive stress and size effect of the precursors. First, thermographic imaging was used to investigate thermal stress from temperature distribution in the precursors during growth annealing. To enhance thermal stress in the precursors, a thermal cycling method and an Ag-paste coating method were proposed and found to significantly accelerate the whisker growth. The use of pulverized precursors also promoted whisker growth, possibly due to contribution from the vapor-liquid-solid growth mechanism. The obtained whiskers revealed the typical composition, diffraction patterns, and superconducting properties of the Bi-2212 phase. The proposed methods were able to stably produce longer whiskers compared to the conventional method. Using the obtained whiskers, electrical transport measurements under high pressure were successfully performed at up to around 50 GPa. △ Less

Submitted 4 April, 2021; originally announced April 2021.

Fermi surfaces of the topological semimetal CaSn$_{3}$ probed through de Haas van Alphen oscillations

Authors: K A M Hasan Siddiquee, Riffat Munir, Charuni Dissanayake, Xinzhe Hu, Swapnil Yadav, Yasumasa Takano, Eun Sang Choi, Duy Le, Talat S Rahman, Yasuyuki Nakajima

Abstract: In the search of topological superconductors, nailing down the Fermiology of the normal state is as crucial a prerequisite as unraveling the superconducting pairing symmetry. In particular, the number of time-reversal-invariant momenta in the Brillouin zone enclosed by Fermi surfaces is closely linked to the topological class of time-reversal-invariant systems, and can experimentally be investigat… ▽ More In the search of topological superconductors, nailing down the Fermiology of the normal state is as crucial a prerequisite as unraveling the superconducting pairing symmetry. In particular, the number of time-reversal-invariant momenta in the Brillouin zone enclosed by Fermi surfaces is closely linked to the topological class of time-reversal-invariant systems, and can experimentally be investigated. We report here a detailed study of de Haas van Alphen quantum oscillations in single crystals of the topological semimetal CaSn$_{3}$ with torque magnetometry in high magnetic fields up to 35 T. In conjunction with density functional theory based calculations, the observed quantum oscillations frequencies indicate that the Fermi surfaces of CaSn$_{3}$ enclose an odd number of time-reversal-invariant momenta, satisfying one of the proposed criteria to realize topological superconductivity. Nonzero Berry phases extracted from the magnetic oscillations also support the nontrivial topological nature of CaSn$_{3}$. △ Less

Submitted 14 March, 2021; originally announced March 2021.

Comments: 7 pages, 7 figures, accepted for publication in Journal of Physics: Condensed Matter

Unusual upper critical fields of the topological nodal-line semimetal candidate Sn$_{x}$NbSe$_{2-δ}$

Authors: Riffat Munir, K A M Hasan Siddiquee, Charuni Dissanayake, Xinzhe Hu, Yasumasa Takano, Eun Sang Choi, Yasuyuki Nakajima

Abstract: We report superconductivity in Sn$_{x}$NbSe$_{2-δ}$, a topological nodal-line semimetal candidate with a noncentrosymmetric crystal structure. The superconducting transition temperature $T_{c}$ of this compound is extremely sensitive to Sn concentration $x$ and Se deficiency $δ$, 5.0 K for Sn$_{0.13}$NbSe$_{1.70}$ and 8.6 K for Sn$_{0.14}$NbSe$_{1.71}$ and Sn$_{0.15}$NbSe$_{1.69}$. In all samples,… ▽ More We report superconductivity in Sn$_{x}$NbSe$_{2-δ}$, a topological nodal-line semimetal candidate with a noncentrosymmetric crystal structure. The superconducting transition temperature $T_{c}$ of this compound is extremely sensitive to Sn concentration $x$ and Se deficiency $δ$, 5.0 K for Sn$_{0.13}$NbSe$_{1.70}$ and 8.6 K for Sn$_{0.14}$NbSe$_{1.71}$ and Sn$_{0.15}$NbSe$_{1.69}$. In all samples, the temperature dependence of the upper critical field $H_{c2}(T)$ differs from the prediction of the Werthamer-Helfand-Hohenberg theory. While the zero-temperature value of the in-plane upper critical field of Sn$_{x}$NbSe$_{2-δ}$ with the higher $T_{c}$ is lower than the Pauli paramagnetic limit $H_{P}$, that of the lower $T_{c}$ sample exceeds $H_{P}$ by a factor of $\sim$2. Our observations suggest that odd-parity contribution dominates the superconducting gap function of Sn$_{x}$NbSe$_{2-δ}$, and it can be fine-tuned by the Sn concentration and Se deficiency. △ Less

Submitted 14 March, 2021; originally announced March 2021.

Comments: 6 pages, 6 figures