Showing 1–50 of 95 results for author: Kohama, Y

Probing intrinsic magnetic phases in low-dimensional nearly twin-free NiPS$_3$ single crystals

Authors: Yeochan An, Heejun Yang, Sung Jin Park, Giung Park, Woonghee Cho, Pyeongjae Park, Seokhwan Yun, Yoshimitsu Kohama, Je-Geun Park

Abstract: We report the intrinsic thermal and magnetic properties of the low-dimensional van der Waals (vdW) antiferromagnet NiPS$_3$ and explore its emergent magnetic phases by controlling crystallographic twinning. Using nearly twin-free crystals, we resolve intrinsic properties that are typically obscured by multidomain effects in bulk samples. Magnetization results reveal a highly anisotropic, sharp spi… ▽ More We report the intrinsic thermal and magnetic properties of the low-dimensional van der Waals (vdW) antiferromagnet NiPS$_3$ and explore its emergent magnetic phases by controlling crystallographic twinning. Using nearly twin-free crystals, we resolve intrinsic properties that are typically obscured by multidomain effects in bulk samples. Magnetization results reveal a highly anisotropic, sharp spin-flop transition, confirming the high domain purity of our crystals. Furthermore, high-precision thermodynamic and transport data reveal a broad fluctuation regime around the Néel temperature ($T_{\mathrm{N}}$ = 157.5 K), with a heat capacity anomaly and a concurrent suppression of thermal conductivity. Field-dependent thermal transport shows a small but distinct contribution from spin-lattice coupling, as evidenced by the dip at the spin-flop transition. We develop a theoretical model to explain these properties reported in this paper, with good agreement between experiment and theory. Our work establishes a definitive baseline for bulk properties of NiPS$_3$ and demonstrates the feasibility of resolving intrinsic anisotropies by addressing crystallographic twinning in vdW magnets. △ Less

Submitted 14 August, 2026; originally announced August 2026.

Comments: Accepted by Advanced Functional Materials; 27 pages, 6 main figures, 8 supporting figures

Observation of an emergent energy scale close to dimensional reduction in a quasi-two-dimensional quantum magnet

Authors: Anneke Reinold, Laur Peedu, Kirill Amelin, Urmas Nagel, Toomas Rõõm, Sven Luther, Hannes Kühne, Dirk Wulferding, Kingshuk Mukhuti, Maarten W. de Dreu, Peter C. M. Christianen, Dennis Kudlacik, Dmitri Yakovlev, Zhiying Zhao, Taro Nakajima, Yoshimitsu Kohama, Thomas Lorenz, Franco Lisandrini, Corinna Kollath, Marcin Raczkowski, Fakher F. Assaad, Zhe Wang

Abstract: By appropriately perturbing a critical transverse-field Ising chain away from its critical point, the system can develop a finite correlation length with a characteristic purely massive spectrum, whose ratios and correlations are precisely described by an integrable field theory and an infinite set of integrals of motion corresponding to the $E_8$ Lie algebra. In this work, we report on experiment… ▽ More By appropriately perturbing a critical transverse-field Ising chain away from its critical point, the system can develop a finite correlation length with a characteristic purely massive spectrum, whose ratios and correlations are precisely described by an integrable field theory and an infinite set of integrals of motion corresponding to the $E_8$ Lie algebra. In this work, we report on experimental observation of a characteristic massive spectrum close to transverse field-induced dimensional reduction in a quasi-two-dimensional quantum magnet Cu$_2$(OH)$_3$Br, providing evidence for an emergent $E_8$ symmetry and the corresponding excitations of bound states in the sublattice of its ferromagnetic chains. These results demonstrate the power of integrable field theory in describing emergent many-body quantum critical phenomena in condensed matter systems. △ Less

Submitted 26 July, 2026; originally announced July 2026.

Comments: 6 pages, 4 figures

Circularly Polarized Magneto-Photoluminescence in Two-Dimensional Chiral Perovskites R- and S-(C4H9NH3)2PbI4 under High Magnetic Fields

Authors: D. Y. Park, S. Park, Yongmin Kim, N. Myoung, Z. Yang, Y. Kohama, Y. H. Matsuda

Abstract: We report circularly polarized magneto-photoluminescence (MPL) measurements on the enantiomeric pair of two-dimensional chiral perovskites R- and S-(C4H9NH3)2PbI4 in pulsed magnetic fields up to 50 T at 4.2 K. The R-form exhibits strong preferential emission into the RC channel (I_RC/I_LC = 10:1), with the S-form showing the opposite sense, robust against the applied field. Three key observations… ▽ More We report circularly polarized magneto-photoluminescence (MPL) measurements on the enantiomeric pair of two-dimensional chiral perovskites R- and S-(C4H9NH3)2PbI4 in pulsed magnetic fields up to 50 T at 4.2 K. The R-form exhibits strong preferential emission into the RC channel (I_RC/I_LC = 10:1), with the S-form showing the opposite sense, robust against the applied field. Three key observations are reported: (i) an anomalous redshift of all exciton transition energies with increasing field-contrasting with the normal diamagnetic blueshift of achiral perovskites-with a non-monotonic initial blueshift to 7.6 T in the dominant RC channel of the R-form; (ii) complete invariance of PL peak positions upon reversal of the field direction, consistent with Rashba-induced mixing of the bright exciton with a nearby m_x = 0 dark state; and (iii) field-induced increase in PL intensity and narrowing of the linewidth, attributed to suppression of disorder scattering as the cyclotron orbit contracts. These results are interpreted in the framework of Rashba spin-splitting and polaron formation in the chiral two-dimensional perovskite lattice. △ Less

Submitted 23 July, 2026; v1 submitted 25 June, 2026; originally announced June 2026.

BCS-BEC crossover driven by small Fermi pockets of a high-Tc cuprate superconductor

Authors: Junhyeok Jeong, Yamato Enomoto, Yoshimitsu Kohama, Tomotaka Nakayama, Kotaro Ando, Kifu Kurokawa, Soonsang Huh, Zhuo Yang, Toshihiro Nomura, Matthew D. Watson, Timur K. Kim, Cephise Cacho, Chun Lin, Makoto Hashimoto, Donghui Lu, Shiro Sakai, Takami Tohyama, Kazuyasu Tokiwa, Takeshi Kondo

Abstract: Fermi arcs observed in underdoped cuprates have sparked debate over whether they represent segments of a large Fermi surface or small Fermi pockets. This ambiguity has long hindered their classification as either the conventional Bardeen-Cooper-Schrieffer (BCS) regime or the strongly coupled Bose-Einstein condensation (BEC) crossover limit. Here, using angle-resolved photoemission spectroscopy and… ▽ More Fermi arcs observed in underdoped cuprates have sparked debate over whether they represent segments of a large Fermi surface or small Fermi pockets. This ambiguity has long hindered their classification as either the conventional Bardeen-Cooper-Schrieffer (BCS) regime or the strongly coupled Bose-Einstein condensation (BEC) crossover limit. Here, using angle-resolved photoemission spectroscopy and quantum oscillations, we demonstrate the coexistence of a small Fermi pocket and a large superconducting gap in the clean inner CuO2 layers of the four-layer cuprate Ba2Ca3Cu4O8(F,O)2. This coexistence constitutes a hallmark of the BCS-BEC crossover and has remained elusive for decades. Despite the presence of antiferromagnetic (AF) order, the superconducting gap in the small pocket is remarkably large, yielding a gap-to-Fermi-energy ratio (Delta_pocket/e_F ~ 0.6) and a critical-to-Fermi-temperature ratio (Tc/TF ~ 1.3) that reach the theoretical upper bound for two-dimensional superconductivity. Unexpectedly, this BCS-BEC crossover emerges not as the carrier density decreases but as it increases, abruptly within a narrow doping range of less than 1%. These results provide a long-sought microscopic foundation for the d-wave pairing mechanism in doped AF-Mott insulators. △ Less

Submitted 3 June, 2026; originally announced June 2026.

Journal ref: Nature Communications 17, 4810 (2026)

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

Authors: Masaki Gen, Shun Okumura, Shusaku Imajo, Taro Nakajima, Karel Prokes, Shunsuke Kitou, Yusuke Tokunaga, Yoichi Nii, Koichi Kindo, Yoshimitsu Kohama, Shintaro Ishiwata, Taka-hisa Arima

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

Submitted 13 June, 2026; v1 submitted 21 May, 2026; originally announced May 2026.

Comments: 11 pages, 5 figures, SM: 7 pages, 6 figures

Magnetocaloric effect measurements in ultrahigh magnetic fields up to 120 T

Authors: Reon Ogawa, Masaki Gen, Kazuyuki Matsuhira, Yoshimitsu Kohama

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

Submitted 8 March, 2026; v1 submitted 4 December, 2025; originally announced December 2025.

Comments: 6 pages, 3 figures. Conference Proceedings

Journal ref: JJAP Conf. Proc. 12, 011009 (2026)

High-Field Torque Magnetometry on the Kagome Antiferromagnet Karpenkoite

Authors: Hibiki Kunisawa, Ryuya Watanabe, Jun-ichi Yamaura, Yoshimitsu Kohama, Toshihiro Nomura

Abstract: We report torque magnetometry results on single crystals of karpenkoite Co3(V2O7)(OH)2 2H2O, a model candidate for the kagome antiferromagnet. No field-induced phase transition is detected up to 45 T for B||c and B||a. Instead, the torque reveals a continuous spin reorientation toward saturation, most likely governed by a dominant Dzyaloshinskii-Moriya interaction. We report torque magnetometry results on single crystals of karpenkoite Co3(V2O7)(OH)2 2H2O, a model candidate for the kagome antiferromagnet. No field-induced phase transition is detected up to 45 T for B||c and B||a. Instead, the torque reveals a continuous spin reorientation toward saturation, most likely governed by a dominant Dzyaloshinskii-Moriya interaction. △ Less

Submitted 19 October, 2025; originally announced October 2025.

Comments: 6 pages, 1 figure

Journal ref: JJAP Conf. Proc. 12, 011017 (2026)

Spin-supersolidity induced quantum criticality and magnetocaloric effect in the triangular-lattice antiferromagnet Rb$_2$Co(SeO$_3$)$_2$

Authors: Yi Cui, Zhanlong Wu, Zhongcen Sun, Kefan Du, Jun Luo, Shuo Li, Jie Yang, Jinchen Wang, Rui Zhou, Qian Chen, Yoshimitsu Kohama, Atsuhiko Miyata, Zhuo Yang, Rong Yu, Weiqiang Yu

Abstract: We performed high-field magnetization, magnetocaloric effect (MCE), and NMR measurements on the Ising triangular-lattice antiferromagnet Rb$_2$Co(SeO$_3$)$_2$. The observations of the 1/3-magnetization plateau, the split NMR lines, and the thermal activation behaviors of the spin-lattice relaxation rate $1/T_1$ between 2 T and 15.8 T provide unambiguous evidence of a gapped up-up-down (UUD) magnet… ▽ More We performed high-field magnetization, magnetocaloric effect (MCE), and NMR measurements on the Ising triangular-lattice antiferromagnet Rb$_2$Co(SeO$_3$)$_2$. The observations of the 1/3-magnetization plateau, the split NMR lines, and the thermal activation behaviors of the spin-lattice relaxation rate $1/T_1$ between 2 T and 15.8 T provide unambiguous evidence of a gapped up-up-down (UUD) magnetic ordered phase. For fields between 15.8 T and 18.5 T, the anomaly in the magnetic susceptibility, the slow saturation of the NMR line spectral ratio with temperature, and the power-law temperature dependence of $1/T_1$ suggest the ground state to be a spin supersolid with gapless spin excitations. With further increasing the field, the Grüneisen ratio, extracted from the MCE data, reveals a continuous quantum phase transition at $H_{\rm C}\approx$ 19.5 T and a universal quantum critical scaling with the exponents $νz~\approx~$1. Near $H_{\rm C}$, the large high-temperature MCE signal and the broad peaks in the NMR Knight shift and $1/T_1$, manifest the strong spin fluctuations driven by both magnetic frustration and quantum criticality. These results establish Rb$_2$Co(SeO$_3$)$_2$ as a candidate platform for cryogenic magnetocaloric cooling. △ Less

Submitted 30 September, 2025; originally announced September 2025.

Comments: 7 pages, 5 figures

Journal ref: npjQM 11, 52 (2026)

Quintuplet condensation in the skyrmionic insulator Cu2OSeO3 at ultrahigh magnetic fields

Authors: T. Nomura, I. Rousochatzakis, O. Janson, M. Gen, X. -G. Zhou, Y. Ishii, S. Seki, Y. Kohama, Y. H. Matsuda

Abstract: We report ultrahigh magnetic field Faraday rotation results on the chiral helimagnet Cu2OSeO3, the first Mott insulator showing skyrmion lattice phases and a linear magnetoelectric effect. Between 180 and 300 T, we find signatures of a Bose-Einstein condensation (BEC) of magnons, which can be described as a canted XY ferrimagnet. Due to the magnetoelectric coupling, the transverse magnetic order o… ▽ More We report ultrahigh magnetic field Faraday rotation results on the chiral helimagnet Cu2OSeO3, the first Mott insulator showing skyrmion lattice phases and a linear magnetoelectric effect. Between 180 and 300 T, we find signatures of a Bose-Einstein condensation (BEC) of magnons, which can be described as a canted XY ferrimagnet. Due to the magnetoelectric coupling, the transverse magnetic order of the indivual Cu2+ spins is accompanied by a characteristic dome-like electric polarization which is crucial for the observation of the condensate via the Faraday rotation effect. △ Less

Submitted 19 February, 2026; v1 submitted 16 September, 2025; originally announced September 2025.

Comments: 15 pages

Journal ref: Phys. Rev. Lett. 136, 076703 (2026)

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

Authors: Masaki Gen, Hidemaro Suwa, Shusaku Imajo, Chao Dong, Hiroaki Ueda, Makoto Tachibana, Akihiko Ikeda, Koichi Kindo, Yoshimitsu Kohama

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

Submitted 7 March, 2026; v1 submitted 19 August, 2025; originally announced August 2025.

Comments: 7 pages, 4 figures, SM: 8 pages, 8 figures. To be published in Physical Review Letters

High-field NMR study of field-induced states in Pb(TiO)Cu$_4$(PO$_4$)$_4$

Authors: Y. Ihara, T. Kanda, Y. Kato, Y. Motome, K. Matsui, K. Kindo, Y. Kohama, T. Kimura, K. Kimura

Abstract: The square cupola antiferromagnet Pb(TiO)Cu$_4$(PO$_4$)$_4$ exhibits the intriguing magnetoelectric responses arising from the consecutive change in the magnetic quadrupolar-type configuration of magnetic moments under external magnetic fields higher than 15 T. To clarify the high-field magnetic structures in Pb(TiO)Cu$_4$(PO$_4$)$_4$, an NMR measurement was performed in pulsed fields up to 32.2 T… ▽ More The square cupola antiferromagnet Pb(TiO)Cu$_4$(PO$_4$)$_4$ exhibits the intriguing magnetoelectric responses arising from the consecutive change in the magnetic quadrupolar-type configuration of magnetic moments under external magnetic fields higher than 15 T. To clarify the high-field magnetic structures in Pb(TiO)Cu$_4$(PO$_4$)$_4$, an NMR measurement was performed in pulsed fields up to 32.2 T significantly extending the field range accessible by superconducting magnets. The double-peak structure of NMR spectra emerging above 29 T applied along the [001] direction evidences the successive magnetic transitions. The field dependence of NMR spectra was analyzed on the basis of cluster mean-field theory, which allows us to propose possible magnetic structures for the high-field magnetic states. △ Less

Submitted 18 August, 2025; originally announced August 2025.

Comments: 9 pages, 6 figures

Misfit layered superconductor (PbSe)1.14(NbSe2)3 with possible layer-selective FFLO state

Authors: Yuki M. Itahashi, Yamato Nohara, Michiya Chazono, Hideki Matsuoka, Koichiro Arioka, Tetsuya Nomoto, Yoshimitsu Kohama, Youichi Yanase, Yoshihiro Iwasa, Kaya Kobayashi

Abstract: Two-dimensional (2D) superconductors are known for their novel emergent phenomena, however, lack of experimental probes beyond resistivity has hindered further exploration of diverse superconducting states. Bulk 2D superconductors, with superconducting layers separated by non-superconducting layers, offer a unique opportunity to break this limit. Here, we synthesized a single crystal of misfit lay… ▽ More Two-dimensional (2D) superconductors are known for their novel emergent phenomena, however, lack of experimental probes beyond resistivity has hindered further exploration of diverse superconducting states. Bulk 2D superconductors, with superconducting layers separated by non-superconducting layers, offer a unique opportunity to break this limit. Here, we synthesized a single crystal of misfit layered compound (PbSe)1.14(NbSe2)3, composed of alternately stacked tri-layer NbSe2 and non-superconducting block layers with incompatible unit cells. Due to its unique structure, 2D Ising superconductivity is maintained even in a bulk form. Resistivity and tunnel diode oscillator measurements reveal two distinct superconducting phases in magnetic field vs. temperature phase diagram. Combined with the theoretical analysis, the high-magnetic-field phase is identified as a layer-selective Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase, where Ising and finite-q superconductivity are mixed due to the tri-layer structure. Bulk 2D superconductors with misfit structure offer a novel opportunity for understanding of 2D superconductivity through bulk measurements and interlayer engineering. △ Less

Submitted 16 June, 2025; originally announced June 2025.

Comments: 23 pages, 5 figures

Triplon Bose-Einstein condensation and proximate magnetism in dimerized antiferromagnets

Authors: Z. Y. Zhao, F. Y. Li, C. Dong, R. Chen, M. Y. Cui, Z. W. Ouyang, J. F. Wang, Y. Kohama, Z. Z. He, Gang v. Chen

Abstract: Dimerized quantum magnets provide a useful arena for novel quantum states and phases transitions with the singlet-triplet type of triplon excitations. Here we study the triplon physics and the Bose-Einstein condensation in two isostructural dimerized antiferromagnets $A$Cu(SeO$_3$)$_2$ ($A$ = Hg, Cd). With the systematic measurements, we demonstrate a dimer singlet ground state in HgCu(SeO$_3$)… ▽ More Dimerized quantum magnets provide a useful arena for novel quantum states and phases transitions with the singlet-triplet type of triplon excitations. Here we study the triplon physics and the Bose-Einstein condensation in two isostructural dimerized antiferromagnets $A$Cu(SeO$_3$)$_2$ ($A$ = Hg, Cd). With the systematic measurements, we demonstrate a dimer singlet ground state in HgCu(SeO$_3$)$_2$ with a triplon gap $\sim$ 7.9 K and a triplon Bose-Einstein condensation with an antiferromagnetic order in CdCu(SeO$_3$)$_2$ below 4.4 K. We further adopt the bond-operator technique and show that the elemental replacement preserves the Hamiltonian and allows the study in a unified theoretical framework with tunable interdimer and intradimer interactions on the opposite sides of the quantum critical point. With the peculiar Cu$_2$O$_8$ dimer configuration and effective ferromagnetic interdimer interaction, $A$Cu(SeO$_3$)$_2$ is distinguished from other $S$ = 1/2 dimerized antiferromagnets. Our results represent a global understanding of the magnetic ground states as well as the magnetic transitions in the dimerized magnets of this unusual crystal structure. △ Less

Submitted 26 May, 2025; originally announced May 2025.

Comments: 7 pages, 4 figures, with supplementary materials

Fermi-liquid transport beyond the upper critical field in superconducting La$_2$PrNi$_2$O$_7$ thin films

Authors: Yu-Te Hsu, Yidi Liu, Yoshimitsu Kohama, Tommy Kotte, Vikash Sharma, Yaoju Tarn, Bai Yang Wang, Zhi-Xun Shen, Yijun Yu, Harold Y. Hwang

Abstract: Unconventional superconductivity typically emerges out of a strongly correlated normal state, manifesting as a highly renormalized Fermi liquid or a strange metal with $T$-linear resistivity. In Ruddlesden-Popper bilayer nickelates, superconductivity with a critical temperature $T_{\rm c}$ exceeding 80 and 40~K has been respectively realised in pressurized bulk crystals and epitaxially strained th… ▽ More Unconventional superconductivity typically emerges out of a strongly correlated normal state, manifesting as a highly renormalized Fermi liquid or a strange metal with $T$-linear resistivity. In Ruddlesden-Popper bilayer nickelates, superconductivity with a critical temperature $T_{\rm c}$ exceeding 80 and 40~K has been respectively realised in pressurized bulk crystals and epitaxially strained thin films. These advancements call for the characterisation of fundamental normal-state and superconducting parameters in these new materials platforms of high-$T_{\rm c}$ superconductivity. Here we report detailed magnetotransport experiments on superconducting La$_2$PrNi$_2$O$_7$ (LPNO) thin films under pulsed magnetic fields up to 64~T and access the normal-state behaviour over a wide temperature range between 1.5 and 300~K. We find that the normal state of thin-film LPNO exhibits the hallmarks of Fermi-liquid transport, including $T^2$ temperature dependence of resistivity and Hall angle, and $H^2$ magnetoresistance obeying Kohler scaling. Using the empirical Kadowaki-Woods ratio, we estimate a quasiparticle effective mass $m^*/m_e \simeq 10$, thereby revealing the highly renormalized Fermi liquid state therein. Our results demonstrate that thin-film LPNO follows the same $T_{\rm c}/T_{\rm F}$ scaling observed across a myriad of strongly correlated superconductors and establish key normal-state characteristics of strained bilayer superconducting nickelates. △ Less

Submitted 8 February, 2026; v1 submitted 25 May, 2025; originally announced May 2025.

XRD study of the magnetization plateau above 40 T in the frustrated helimagnet CuGaCr$_{4}$S$_{8}$

Authors: M. Gen, K. Noda, K. Shimbori, T. Tanaka, D. Bhoi, K. Seki, H. Kobayashi, K. Gautam, M. Akaki, Y. Ishii, Y. H. Matsuda, Y. Kubota, Y. Inubushi, M. Yabashi, Y. Kohama, T. Arima, A. Ikeda

Abstract: CuGaCr$_{4}$S$_{8}$, which contains a chromium breathing pyrochlore network, exhibits diverse magnetic phases, including an incommensurate helical state below 31 K and a 1/2-magnetization plateau above 40 T, owing to the interplay between magnetic frustration and spin-lattice coupling. Here, we perform a single-shot powder x-ray diffraction experiment on CuGaCr$_{4}$S$_{8}$ in a pulsed high magnet… ▽ More CuGaCr$_{4}$S$_{8}$, which contains a chromium breathing pyrochlore network, exhibits diverse magnetic phases, including an incommensurate helical state below 31 K and a 1/2-magnetization plateau above 40 T, owing to the interplay between magnetic frustration and spin-lattice coupling. Here, we perform a single-shot powder x-ray diffraction experiment on CuGaCr$_{4}$S$_{8}$ in a pulsed high magnetic field of 55 T, revealing an orthorhombic-to-cubic (or pseudocubic) structural transition upon entering the 1/2-magnetization plateau phase at low temperatures. This observation suggests the emergence of a commensurate ferrimagnetic order, where a 3-up-1-down spin configuration is realized in each small tetrahedron, and the all-up or all-down in each large tetrahedron. We propose two types of 16-sublattice magnetic structures, which are degenerate within exchange interactions between the first, second, and third nearest neighbors. △ Less

Submitted 14 April, 2025; originally announced April 2025.

Comments: 8 pages, 7 figures, 2 tables

Ultrasound measurement technique for the single-turn-coil magnets

Authors: T. Nomura, A. Hauspurg, D. I. Gorbunov, A. Miyata, E. Schulze, S. A. Zvyagin, V. Tsurkan, Y. H. Matsuda, Y. Kohama, S. Zherlitsyn

Abstract: Ultrasound is a powerful means to study numerous phenomena of condensed-matter physics as acoustic waves couple strongly to structural, magnetic, orbital, and charge degrees of freedom. In this paper, we present such technique combined with single-turn coils (STC) which generate magnetic fields beyond 100 T with the typical pulse duration of 6 us. As a benchmark of this technique, the ultrasound r… ▽ More Ultrasound is a powerful means to study numerous phenomena of condensed-matter physics as acoustic waves couple strongly to structural, magnetic, orbital, and charge degrees of freedom. In this paper, we present such technique combined with single-turn coils (STC) which generate magnetic fields beyond 100 T with the typical pulse duration of 6 us. As a benchmark of this technique, the ultrasound results for MnCr2S4, Cu6[Si6O18]6H2O, and liquid oxygen are shown. The resolution for the relative sound-velocity change in the STC is estimated as Delta v/v~10^-3, which is sufficient to study various field-induced phase transitions and critical phenomena. △ Less

Submitted 17 February, 2025; originally announced February 2025.

Comments: 8 pages, 6 figures

Journal ref: Rev. Sci. Instrum. 92, 063902 (2021)

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

Authors: Anneke Reinold, Lucas Berger, Marcin Raczkowski, Zhiying Zhao, Yoshimitsu Kohama, Masaki Gen, Denis I. Gorbunov, Yurii Skourski, Sergei Zherlitsyn, Fakher F. Assaad, Thomas Lorenz, Zhe Wang

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

Submitted 14 November, 2024; originally announced November 2024.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. B 111, L100405 (2025)

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

Authors: Nan Tang, Masaki Gen, Martin Rotter, Huiyuan Man, Kazuyuki Matsuhira, Akira Matsuo, Koichi Kindo, Akihiko Ikeda, Yasuhiro H. Matsuda, Philipp Gegenwart, Satoru Nakatsuji, Yoshimitsu Kohama

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

Submitted 11 January, 2025; v1 submitted 5 September, 2024; originally announced September 2024.

Comments: 10 pages, 8 figures, published in Phys. Rev. B

Dominant Kitaev Interaction and Field-induced Quantum Disordered Phase in the Cobaltate Na$_2$Co$_2$TeO$_6$

Authors: Xu-Guang Zhou, Han Li, Chaebin Kim, Akira Matsuo, Kavita Mehlawat, Kazuki Matsui, Zhuo Yang, Atsuhiko Miyata, Gang Su, Koichi Kindo, Je-Geun Park, Yoshimitsu Kohama, Wei Li, Yasuhiro H. Matsuda

Abstract: The identification of quantum spin liquid phases in Kitaev candidate materials remains a major experimental challenge. Since most Kitaev candidates develop antiferromagnetic (AFM) order at low temperatures, currently there are great interest on the field-induced magnetic disordered phase in these compounds, that are distinct from (partially) polarized states. Recently, a cobaltate Na$_2$Co$_2$TeO… ▽ More The identification of quantum spin liquid phases in Kitaev candidate materials remains a major experimental challenge. Since most Kitaev candidates develop antiferromagnetic (AFM) order at low temperatures, currently there are great interest on the field-induced magnetic disordered phase in these compounds, that are distinct from (partially) polarized states. Recently, a cobaltate Na$_2$Co$_2$TeO$_6$ has emerged as a promising Kitaev candidate with high-spin $t^{5}_{2g}e^2_g$ configuration and spin-orbit entangled $J_{\rm eff} = 1/2$ honeycomb lattice system. There are intensive studies on field-induced magnetic states and phase transitions under in-plane magnetic fields. In this study, we propose an intermediate disordered phase induced by an out-of-plane field along the $c$-axis, through high-field magnetization and magnetocaloric effect measurements. To explain the high-field behavior of Na$_2$Co$_2$TeO$_6$, we develop an effective $K$-$J$-$Γ$-$Γ^{\prime}$ spin model featuring a dominant AFM Kitaev interaction. This framework uncovers an intermediate quantum spin liquid phase, establishing the material as a unique platform for exploring Kitaev physics and field-induced quantum-disordered states. △ Less

Submitted 7 January, 2026; v1 submitted 4 August, 2024; originally announced August 2024.

Comments: 8 pages, 4 figures

Journal ref: Phys. Rev. B 112, L241108 (2025)

Gapless spin excitations in a quantum spin liquid state of S=1/2 perfect kagome antiferromagnet

Authors: S. Suetsugu, T. Asaba, S. Ikemori, Y. Sekino, Y. Kasahara, K. Totsuka, B. Li, Y. Zhao, Y. Li, Y. Kohama, Y. Matsuda

Abstract: Quantum spin liquids (QSLs) represent an exotic quantum many-body state characterized by the suppression of long-range magnetic order due to strong quantum fluctuations. The kagome spin-1/2 antiferromagnet (AFM) is a prime candidate for realizing QSLs, but its ground state remains an unresolved conundrum. Here we investigate the recently discovered perfect kagome AFM YCu$_3$(OH)$_{6.5}$Br$_{2.5}$… ▽ More Quantum spin liquids (QSLs) represent an exotic quantum many-body state characterized by the suppression of long-range magnetic order due to strong quantum fluctuations. The kagome spin-1/2 antiferromagnet (AFM) is a prime candidate for realizing QSLs, but its ground state remains an unresolved conundrum. Here we investigate the recently discovered perfect kagome AFM YCu$_3$(OH)$_{6.5}$Br$_{2.5}$ to elucidate two central enigmas surrounding the kagome AFM. Ultra-sensitive torque magnetometry experiments reveal that the intrinsic magnetic susceptibility arising from the kagome layer remains nearly temperature-independent down to exceedingly low temperatures. This observation seemingly implies the emergence of gapless fermionic spin excitations akin to Pauli paramagnetism in metals. However, most strikingly, these results stand in stark contrast to the conspicuous absence of a temperature-linear contribution to the specific heat. These findings appear irreconcilable with the widely-discussed theoretical frameworks assuming fermionic quasiparticles (QPs), instead suggesting a transition of bosonic QPs into a superfluid state with a gapless Goldstone mode. Furthermore, magnetocaloric measurements evince an entropy anomaly, constituting thermodynamic evidence that magnetic fields instigate the opening of a spin gap, driving a quantum phase transition into a 1/9 magnetization plateau state. These results shed light on the nature of the low-energy excitations in zero and strong magnetic fields, providing crucial insights into the long-standing unresolved issues of the ground state of the kagome AFM. △ Less

Submitted 23 July, 2024; originally announced July 2024.

Comments: 23 pages, 9 figures

Giant Linear Dichroism Controlled by Magnetic Field in FePS$_3$

Authors: Xu-Guang Zhou, Zhuo Yang, Youjin Lee, Jaena Park, Yoshimitsu Kohama, Koichi Kindo, Yasuhiro H. Matsuda, Je-Geun Park, Oleg Janson, Atsuhiko Miyata

Abstract: Magnetic-field control of fundamental optical properties is a crucial challenge in the engineering of multifunctional microdevices. Van der Waals (vdW) magnets retaining a magnetic order even in atomically thin layers, offer a promising platform for hosting exotic magneto-optical functionalities owing to their strong spin-charge coupling. Here, we demonstrate that a giant optical anisotropy can be… ▽ More Magnetic-field control of fundamental optical properties is a crucial challenge in the engineering of multifunctional microdevices. Van der Waals (vdW) magnets retaining a magnetic order even in atomically thin layers, offer a promising platform for hosting exotic magneto-optical functionalities owing to their strong spin-charge coupling. Here, we demonstrate that a giant optical anisotropy can be controlled by magnetic fields in the vdW magnet FePS$_3$. The giant linear dichroism ($\sim$11%), observed below $T_{\text{N}}\!\sim\!120$ K, is nearly fully suppressed in a wide energy range from 1.6 to 2.0 eV, following the collapse of the zigzag magnetic order above 40 T. This remarkable phenomenon can be explained as a result of symmetry changes due to the spin order, enabling minority electrons of Fe$^{2+}$ to hop in a honeycomb lattice. The modification of spin-order symmetry by external fields provides a novel route for controllable anisotropic optical micro-devices. △ Less

Submitted 1 May, 2024; originally announced May 2024.

Comments: 5 pages, 4 figures

Rhenium oxyhalides: a showcase for anisotropic-triangular-lattice quantum antiferromagnets

Authors: M. Gen, D. Hirai, K. Morita, S. Kogane, N. Matsuyama, T. Yajima, M. Kawamura, K. Deguchi, A. Matsuo, K. Kindo, Y. Kohama, Z. Hiroi

Abstract: The spin-1/2 Heisenberg antiferromagnet on an anisotropic triangular lattice (ATL) is an archetypal spin system hosting exotic quantum magnetism and dimensional crossover. However, the progress in experimental research on this field has been limited due to the scarcity of ideal model materials. Here, we show that rhenium oxyhalides $A_{3}$ReO$_{5}X_{2}$, where spin-1/2 Re$^{6+}$ ions form a layere… ▽ More The spin-1/2 Heisenberg antiferromagnet on an anisotropic triangular lattice (ATL) is an archetypal spin system hosting exotic quantum magnetism and dimensional crossover. However, the progress in experimental research on this field has been limited due to the scarcity of ideal model materials. Here, we show that rhenium oxyhalides $A_{3}$ReO$_{5}X_{2}$, where spin-1/2 Re$^{6+}$ ions form a layered structure of ATLs, allow for flexible chemical substitution in both cation $A^{2+}$ ($A$ = Ca, Sr, Ba, Pb) and anion $X^{-}$ ($X$ = Cl, Br) sites, leading to seven synthesizable compounds. By combining magnetic susceptibility and high-field magnetization measurements with theoretical calculations using the orthogonalized finite-temperature Lanczos method, we find that the anisotropy $J'/J$ ranges from 0.25 to 0.45 depending on the chemical composition. Our findings demonstrate that $A_{3}$ReO$_{5}X_{2}$ is an excellent platform for realizing diverse effective spin Hamiltonians that differ in the strength of the anisotropy $J'/J$ as well as the relevance of perturbation terms such as the Dzyaloshinskii-Moriya interaction and interlayer exchange coupling. △ Less

Submitted 10 November, 2023; originally announced November 2023.

Comments: 11 pages, 5 figures, SM: 4 pages, 2 figures

Distinctive Doping Dependence of Upper Critical Field in Iron-Based Superconductor LaFeAsO$_{1-x}$H$_{x}$

Authors: Shiro Kawachi, Jun-ichi Yamaura, Yoshio Kuramoto, Soshi Iimura, Toshihiro Nomura, Yoshimitsu Kohama, Takashi Sasaki, Masashi Tokunaga, Youichi Murakami, Hideo Hosono

Abstract: High magnetic fields up to 105 T have been utilized in deriving the upper critical field $B_{\rm c2}$ of LaFeAsO$_{1-x}$H$_x$ throughout whole temperatures below $T_{\rm c}$. Resistivity measurements demonstrate that $B_{\rm c2}$ behaves differently in samples with $x = 0.12$ (SC1) from those with 0.32 (SC2). In SC1, the two-band model assuming the $s$-wave pairing gives a good fitting with repuls… ▽ More High magnetic fields up to 105 T have been utilized in deriving the upper critical field $B_{\rm c2}$ of LaFeAsO$_{1-x}$H$_x$ throughout whole temperatures below $T_{\rm c}$. Resistivity measurements demonstrate that $B_{\rm c2}$ behaves differently in samples with $x = 0.12$ (SC1) from those with 0.32 (SC2). In SC1, the two-band model assuming the $s$-wave pairing gives a good fitting with repulsive intraband interaction and dominant interband coupling. In SC2, we have to assume attractive intraband interaction with weak interband coupling, which in fact suggests a non-$s$-wave pairing in view of the strong Coulomb repulsion. These results support the possibility that SC1 and SC2 have different pairing symmetries. △ Less

Submitted 24 August, 2023; originally announced August 2023.

Stroboscopic Time-of-Flight Neutron Diffraction in Long Pulsed Magnetic Fields

Authors: Taro Nakajima, Masao Watanabe, Yasuhiro Inamura, Kazuki Matsui, Tomoki Kanda, Tetsuya Nomoto, Kazuki Ohishi, Yukihiko Kawamura, Hiraku Saito, Hiromu Tamatsukuri, Noriki Terada, Yoshimitsu Kohama

Abstract: We present proof-of-principle experiments of stroboscopic time-of-flight (TOF) neutron diffraction in long pulsed magnetic fields. By utilizing electric double-layer capacitors, we developed a long pulsed magnet for neutron diffraction measurements, which generates pulsed magnetic fields with the full widths at the half maximum of more than $10^2$ ms. The field variation is slow enough to be appro… ▽ More We present proof-of-principle experiments of stroboscopic time-of-flight (TOF) neutron diffraction in long pulsed magnetic fields. By utilizing electric double-layer capacitors, we developed a long pulsed magnet for neutron diffraction measurements, which generates pulsed magnetic fields with the full widths at the half maximum of more than $10^2$ ms. The field variation is slow enough to be approximated as a steady field within the time scale of a polychromatic neutron pulse passing through a sample placed in a distance of the order of $10^1$ m from the neutron source. This enables us to efficiently explore the reciprocal space using a wide range of neutron wavelength in high magnetic fields. We applied this technique to investigate field-induced magnetic phases in the triangular lattice antiferromagnets CuFe$_{1-x}$Ga$_x$O$_2$ ($x=0, 0.035$). △ Less

Submitted 21 August, 2023; originally announced August 2023.

Comments: 9 pages, 7 figures

Unveiling phase diagram of the lightly doped high-Tc cuprate superconductors with disorder removed

Authors: Kifu Kurokawa, Shunsuke Isono, Yoshimitsu Kohama, So Kunisada, Shiro Sakai, Ryotaro Sekine, Makoto Okubo, Matthew D. Watson, Timur K. Kim, Cephise Cacho, Shik Shin, Takami Tohyama, Kazuyasu Tokiwa, Takeshi Kondo

Abstract: The currently established electronic phase diagram of cuprates is based on a study of single- and double-layered compounds. These CuO$_2$ planes, however, are directly contacted with dopant layers, thus inevitably disordered with an inhomogeneous electronic state. Here, we solve this issue by investigating a 6-layered Ba$_2$Ca$_5$Cu$_6$O$_{12}$(F,O)$_2$ with inner CuO$_2$ layers, which are clean w… ▽ More The currently established electronic phase diagram of cuprates is based on a study of single- and double-layered compounds. These CuO$_2$ planes, however, are directly contacted with dopant layers, thus inevitably disordered with an inhomogeneous electronic state. Here, we solve this issue by investigating a 6-layered Ba$_2$Ca$_5$Cu$_6$O$_{12}$(F,O)$_2$ with inner CuO$_2$ layers, which are clean with the extremely low disorder, by angle-resolved photoemission spectroscopy (ARPES) and quantum oscillation measurements. We find a tiny Fermi pocket with a doping level less than 1% to exhibit well-defined quasiparticle peaks which surprisingly lack the polaronic feature. This provides the first evidence that the slightest amount of carriers is enough to turn a Mott insulating state into a metallic state with long-lived quasiparticles. By tuning hole carriers, we also find an unexpected phase transition from the superconducting to metallic states at 4%. Our results are distinct from the nodal liquid state with polaronic features proposed as an anomaly of the heavily underdoped cuprates. △ Less

Submitted 14 July, 2023; originally announced July 2023.

Journal ref: Nature Communications 14, 4064 (2023)

High-field phase diagram of the chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4

Authors: Toshihiro Nomura, Yasuyuki Kato, Yukitoshi Motome, Atsushi Miyake, Masashi Tokunaga, Yoshimitsu Kohama, Sergei Zherlitsyn, Joachim Wosnitza, Shojiro Kimura, Tsukasa Katsuyoshi, Tsuyoshi Kimura, Kenta Kimura

Abstract: High-field phase diagram of a chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4 is studied by means of the ultrasound, dielectric, and magnetocaloric-effect measurements. These experimental techniques reveal two new phase transitions at high fields, which have not been resolved by the previous magnetization experiments. Specifically, the c66 acoustic mode shows drastic changes with hysteresis with a… ▽ More High-field phase diagram of a chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4 is studied by means of the ultrasound, dielectric, and magnetocaloric-effect measurements. These experimental techniques reveal two new phase transitions at high fields, which have not been resolved by the previous magnetization experiments. Specifically, the c66 acoustic mode shows drastic changes with hysteresis with applied fields along the c axis, indicating a strong magneto-elastic coupling. Combined with the cluster mean-field theory, we discuss the origins of these phase transitions. By considering the chiral-twist effect of Cu4O12 cupola units, which is inherent to the chiral crystal structure, the phase diagram is reasonably reproduced. The agreement between the experiment and theory suggests that this material is a unique quasi two-dimensional spin system with competing exchange interactions and chirality, leading to the rich phase diagram. △ Less

Submitted 1 December, 2023; v1 submitted 4 June, 2023; originally announced June 2023.

Comments: 12 pages, 11 figures, 1 table

Journal ref: Phys. Rev. B 108, 054434 (2023)

Breathing pyrochlore magnet CuGaCr$_{4}$S$_{8}$: Magnetic, thermodynamic, and dielectric properties

Authors: M. Gen, H. Ishikawa, A. Miyake, T. Yajima, H. O. Jeschke, H. Sagayama, A. Ikeda, Y. H. Matsuda, K. Kindo, M. Tokunaga, Y. Kohama, T. Kurumaji, Y. Tokunaga, T. Arima

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

Submitted 16 October, 2023; v1 submitted 19 March, 2023; originally announced March 2023.

Comments: 12 pages, 13 figures

Journal ref: Phys. Rev. Mater. 7, 104404 (2023)

Simultaneous measurement of specific heat and thermal conductivity in pulsed magnetic fields

Authors: Tetsuya Nomoto, Chengchao Zhong, Hiroshi Kageyama, Yoko Suzuki, Marcelo Jaime, Yoshiaki Hashimoto, Shingo Katsumoto, Naofumi Matsuyama, Chao Dong, Akira Matsuo, Koichi Kindo, Koichi Izawa, Yoshimitsu Kohama

Abstract: We report an experimental setup for simultaneously measuring specific heat and thermal conductivity in feedback-controlled pulsed magnetic fields of 50 msec duration at cryogenic temperatures. A stabilized magnetic field pulse obtained by the feedback control, which dramatically improves the thermal stability of the setup and sample, is used in combination with the flash method to obtain absolute… ▽ More We report an experimental setup for simultaneously measuring specific heat and thermal conductivity in feedback-controlled pulsed magnetic fields of 50 msec duration at cryogenic temperatures. A stabilized magnetic field pulse obtained by the feedback control, which dramatically improves the thermal stability of the setup and sample, is used in combination with the flash method to obtain absolute values of thermal properties up to 37.2 T in the 2 K to 16 K temperature range. We describe the experimental setup and demonstrate the performance of the present method with measurements on single crystal samples of the geometrically frustrated quantum spin-dimer system SrCu$_2$(BO$_3$)$_2$. Our proof-of-principle results show excellent agreement with data taken using a standard steady-state method, confirming the validity and convenience of the present approach. △ Less

Submitted 3 February, 2023; originally announced February 2023.

Comments: 9 pages, 7 figures

Signatures of a magnetic superstructure phase induced by ultrahigh magnetic fields in a breathing pyrochlore antiferromagnet

Authors: M. Gen, A. Ikeda, K. Aoyama, H. O. Jeschke, Y. Ishii, H. Ishikawa, T. Yajima, Y. Okamoto, X. -G. Zhou, D. Nakamura, S. Takeyama, K. Kindo, Y. H. Matsuda, Y. Kohama

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

Submitted 9 August, 2023; v1 submitted 23 January, 2023; originally announced January 2023.

Comments: 10 pages, 5 figures, SI: 15 pages, 14 figures

Journal ref: Proc. Natl. Acad. Sci. U.S.A. 120, e2302756120 (2023)

Quantum oscillations in a centrosymmetric skyrmion-hosting magnet GdRu2Si2

Authors: N. Matsuyama, T. Nomura, S. Imajo, T. Nomoto, R. Arita, K. Sudo, M. Kimata, N. D. Khanh, R. Takagi, Y. Tokura, S. Seki, K. Kindo, Y. Kohama

Abstract: We have performed magnetic torque and resistivity measurements on a centrosymmetric skyrmion-host GdRu2Si2, in which the dominant magnetic interaction leading to skyrmion formation is under debate. We observe both the de Haas-van Alphen and Shubnikov-de Haas oscillations in the forced ferromagnetic phase. The angular dependence of the quantum oscillation frequencies can be reproduced by the ab-ini… ▽ More We have performed magnetic torque and resistivity measurements on a centrosymmetric skyrmion-host GdRu2Si2, in which the dominant magnetic interaction leading to skyrmion formation is under debate. We observe both the de Haas-van Alphen and Shubnikov-de Haas oscillations in the forced ferromagnetic phase. The angular dependence of the quantum oscillation frequencies can be reproduced by the ab-initio calculation. The de Haas-van Alphen oscillation is also observed in the double-Q phase with a different frequency to that in the forced ferromagnetic phase, indicating a Fermi surface reconstruction due to the coupling between localized spins and conduction electrons. Based on these experimental findings, the magnetic interactions in this system are discussed. △ Less

Submitted 10 April, 2023; v1 submitted 23 December, 2022; originally announced December 2022.

Comments: 11 pages, 8 figures

Nonreciprocal Phonon Propagation in a Metallic Chiral Magnet

Authors: T. Nomura, X. -X. Zhang, R. Takagi, K. Karube, A. Kikkawa, Y. Taguchi, Y. Tokura, S. Zherlitsyn, Y. Kohama, S. Seki

Abstract: The phonon magnetochiral effect (MChE) is the nonreciprocal acoustic and thermal transports of phonons caused by the simultaneous breaking of the mirror and time-reversal symmetries. So far, the phonon MChE has been observed only in a ferrimagnetic insulator Cu2OSeO3, where the nonreciprocal response disappears above the Curie temperature of 58 K. Here, we study the nonreciprocal acoustic properti… ▽ More The phonon magnetochiral effect (MChE) is the nonreciprocal acoustic and thermal transports of phonons caused by the simultaneous breaking of the mirror and time-reversal symmetries. So far, the phonon MChE has been observed only in a ferrimagnetic insulator Cu2OSeO3, where the nonreciprocal response disappears above the Curie temperature of 58 K. Here, we study the nonreciprocal acoustic properties of a room-temperature ferromagnet Co9Zn9Mn2 for unveiling the phonon MChE close to the room temperature. Surprisingly, the nonreciprocity in this metallic compound is enhanced at higher temperatures and observed up to 250 K. This clear contrast between insulating Cu2OSeO3 and metallic Co9Zn9Mn2 suggests that metallic magnets have a mechanism to enhance the nonreciprocity at higher temperatures. From the ultrasound and microwave-spectroscopy experiments, we conclude that the magnitude of the phonon MChE of Co9Zn9Mn2 mostly depends on the magnon bandwidth, which increases at low temperatures and hinders the magnon-phonon hybridization. Our results suggest that the phonon nonreciprocity could be further enhanced by engineering the magnon band of materials. △ Less

Submitted 8 April, 2023; v1 submitted 30 November, 2022; originally announced December 2022.

Comments: 6 pages, 4 figures, 1 table

Journal ref: Phys. Rev. Lett. 130, 176301 (2023)

High upper critical field (120 T) with small anisotropy of highly hydrogen-substituted SmFeAsO epitaxial film

Authors: Kota Hanzawa, Jumpei Matsumoto, Soshi Iimura, Yoshimitsu Kohama, Hidenori Hiramatsu, Hideo Hosono

Abstract: The electronic transport properties of a highly hydrogen-substituted 1111-type SmFeAsO epitaxial film with high critical-temperature (Tc = 45 K) were investigated under high magnetic fields. By using a single-turn magnet generating up to 130 T, we clarified that the upper critical field (μ0Hc2) of SmFeAsO0.65H0.35 is 120 T at the nearly low-temperature limit of 2.2 K for μ0H || ab. The angular dep… ▽ More The electronic transport properties of a highly hydrogen-substituted 1111-type SmFeAsO epitaxial film with high critical-temperature (Tc = 45 K) were investigated under high magnetic fields. By using a single-turn magnet generating up to 130 T, we clarified that the upper critical field (μ0Hc2) of SmFeAsO0.65H0.35 is 120 T at the nearly low-temperature limit of 2.2 K for μ0H || ab. The angular dependence of μ0Hc2 revealed that the anisotropic parameter (γ) around Tc is ~2, which is comparable with that of a practical candidate 122-type BaFe2As2 with lower Tc and much smaller than that of F-substituted SmFeAsO. The small γ mainly originates from the high hydrogen incorporation. The extremely high μ0Hc2 and small γ, together with the high Tc and high critical current density, suggest that SmFeAsO1-xHx has high potential for the superconducting electromagnets and cables. △ Less

Submitted 18 November, 2022; originally announced November 2022.

Journal ref: Phys. Rev. Materials 6, L111801 (2022)

Dimensional reduction and incommensurate dynamic correlations in the $S=\frac{1}{2}$ triangular-lattice antiferromagnet Ca$_3$ReO$_5$Cl$_2$

Authors: S. A. Zvyagin, A. N. Ponomaryov, J. Wosnitza, D. Hirai, Z. Hiroi, M. Gen, Y. Kohama, A. Matsuo, Y. H. Matsuda, K. Kindo

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

Submitted 26 October, 2022; originally announced October 2022.

Journal ref: Nature Communications 13, 6310 (2022)

Rhombic skyrmion lattice coupled with orthorhombic structural distortion in EuAl$_{4}$

Authors: Masaki Gen, Rina Takagi, Yoshito Watanabe, Shunsuke Kitou, Hajime Sagayama, Naofumi Matsuyama, Yoshimitsu Kohama, Akihiko Ikeda, Yoshichika Ōnuki, Takashi Kurumaji, Taka-hisa Arima, Shinichiro Seki

Abstract: The centrosymmetric tetragonal itinerant magnet EuAl$_{4}$ exhibits an intricate magnetic phase diagram including rhombic and square skyrmion-lattice (SkL) phases in the external magnetic field. Here, we report a multi-axis dilatometric investigation of EuAl$_{4}$ by means of a newly designed fiber-Bragg-grating technique complemented by a resonant x-ray scattering experiment, revealing anisotropi… ▽ More The centrosymmetric tetragonal itinerant magnet EuAl$_{4}$ exhibits an intricate magnetic phase diagram including rhombic and square skyrmion-lattice (SkL) phases in the external magnetic field. Here, we report a multi-axis dilatometric investigation of EuAl$_{4}$ by means of a newly designed fiber-Bragg-grating technique complemented by a resonant x-ray scattering experiment, revealing anisotropic magnetostriction and magnetovolume effect associated with successive phase transitions. The rhombic and square SkL phases are found to possess $\sim$0.10% and $\sim$0.03% orthorhombic structural distortion within the $ab$ plane, respectively. We propose that the coupling between the spin system and the lattice deformation should be essential for the structural instability in EuAl$_{4}$, yielding a rich variety of topological spin textures with spontaneous rotational-symmetry breaking as well as a potential controllability of the SkL phases by uniaxial stress or pressure. △ Less

Submitted 23 January, 2023; v1 submitted 26 September, 2022; originally announced September 2022.

Comments: 8 pages, 5 figures, SM: 4 pages, 3 figures. To be published in Physical Review B as a Letter

Unveiling new quantum phases in the Shastry-Sutherland compound SrCu2(BO3)2up to the saturation magnetic field

Authors: T. Nomura, P. Corboz, A. Miyata, S. Zherlitsyn, Y. Ishii, Y. Kohama, Y. H. Matsuda, A. Ikeda, C. Zhong, H. Kageyama, F. Mila

Abstract: Under magnetic fields, quantum magnets often undergo exotic phase transitions with various kinds of order. The discovery of a sequence of fractional magnetization plateaus in the Shastry-Sutherland compound SrCu2(BO3)2 has played a central role in the high-field research on quantum materials, but so far this system could only be probed up to half the saturation value of the magnetization. Here, we… ▽ More Under magnetic fields, quantum magnets often undergo exotic phase transitions with various kinds of order. The discovery of a sequence of fractional magnetization plateaus in the Shastry-Sutherland compound SrCu2(BO3)2 has played a central role in the high-field research on quantum materials, but so far this system could only be probed up to half the saturation value of the magnetization. Here, we report the first experimental and theoretical investigation of this compound up to the saturation magnetic field of 140 T and beyond. Using ultrasound and magnetostriction techniques combined with extensive tensor-network calculations (iPEPS), several spin-supersolid phases are revealed between the 1/2 plateau and saturation (1/1 plateau). Quite remarkably, the sound velocity of the 1/2 plateau exhibits a drastic decrease of -50%, related to the tetragonal-to-orthorhombic instability of the checkerboard-type magnon crystal. The unveiled nature of this paradigmatic quantum system is a new milestone for exploring exotic quantum states of matter emerging in extreme conditions. △ Less

Submitted 24 June, 2023; v1 submitted 15 September, 2022; originally announced September 2022.

Comments: 8 pages, 4 figures, 2 tables

Journal ref: Nat. Commun. 14, 3769 (2023)

Correlation-driven organic 3D topological insulator with relativistic fermions

Authors: Tetsuya Nomoto, Shusaku Imajo, Hiroki Akutsu, Yasuhiro Nakazawa, Yoshimitsu Kohama

Abstract: Exploring new topological phenomena and functionalities induced by strong electron correlation has been a central issue in modern condensed-matter physics. One example is a topological insulator (TI) state and its functionality driven by the Coulomb repulsion rather than a spin-orbit coupling. Here, we report a "correlation-driven" TI state realized in an organic zero-gap system $α$-(BETS)$_2$I… ▽ More Exploring new topological phenomena and functionalities induced by strong electron correlation has been a central issue in modern condensed-matter physics. One example is a topological insulator (TI) state and its functionality driven by the Coulomb repulsion rather than a spin-orbit coupling. Here, we report a "correlation-driven" TI state realized in an organic zero-gap system $α$-(BETS)$_2$I$_3$. The surface metallic state that emerges at low temperatures exhibits characteristic transport properties of a gapless Dirac semimetal, evidencing the presence of a topological surface state in this compound. Moreover, we observe a topological phase switching between the TI state and non-equilibrium Dirac semimetal state by a dc current, which is a unique functionality of a correlation-driven TI state. Our findings demonstrate that correlation-driven TIs are promising candidates not only for practical electronic devices but also as a field for discovering new topological phenomena and phases. △ Less

Submitted 1 August, 2022; originally announced August 2022.

Comments: 36 pages including 10 figures

Journal ref: Nat Commun 14, 2130 (2023)

Novel quantum phase of the chromium spinel oxide HgCr$_{\rm 2}$O$_{\rm 4}$ in high magnetic fields

Authors: Shojiro Kimura, Shusaku Imajo, Masaki Gen, Tsutomu Momoi, Masayuki Hagiwara, Hiroaki Ueda, Yoshimitsu Kohama

Abstract: In this study, we have performed the magnetocaloric effect and the specific heat measurements of chromium spinel oxide HgCr$_2$O$_4$, wherein the magnetic Cr$^{3+}$ ions form a highly frustrated pyrochlore lattice with significant spin-lattice coupling. In addition to the known magnetic-field-induced phases, our thermodynamic measurements detect a novel quantum phase just before the saturation of… ▽ More In this study, we have performed the magnetocaloric effect and the specific heat measurements of chromium spinel oxide HgCr$_2$O$_4$, wherein the magnetic Cr$^{3+}$ ions form a highly frustrated pyrochlore lattice with significant spin-lattice coupling. In addition to the known magnetic-field-induced phases, our thermodynamic measurements detect a novel quantum phase just before the saturation of the magnetization, which has not been expected from the classical theories of the pyrochlore lattice antiferromagnet with spin-lattice coupling. Based on recent theoretical model calculation, we discuss the possibility of a spin nematic state appearing for this quantum phase. △ Less

Submitted 2 May, 2022; originally announced May 2022.

Comments: 14 pages, 4 figures

Ferroelectric transition of a chiral molecular crystal BINOL2DMSO

Authors: Toshihiro Nomura, Takeshi Yajima, Zhuo Yang, Ryosuke Kurihara, Yuto Ishii, Masashi Tokunaga, Yasuhiro H. Matsuda, Yoshimitsu Kohama, Kenta Kimura, Tsuyoshi Kimura

Abstract: We report dielectric, thermodynamical, acoustic, and optical properties of a chiral molecular crystal, 1,1'-bi-2-naphthol 2-dimethylsulfoxide (BINOL2DMSO). We find two successive phase transitions at Tc1=190 K and Tc2=125 K. The first transition at Tc1 is characterized by an order-disorder transition of the guest molecules DMSO along with ferroelectricity. At the second transition of Tc2, the crys… ▽ More We report dielectric, thermodynamical, acoustic, and optical properties of a chiral molecular crystal, 1,1'-bi-2-naphthol 2-dimethylsulfoxide (BINOL2DMSO). We find two successive phase transitions at Tc1=190 K and Tc2=125 K. The first transition at Tc1 is characterized by an order-disorder transition of the guest molecules DMSO along with ferroelectricity. At the second transition of Tc2, the crystal structure deforms from tetragonal to monoclinic, leading to domain formation. Low-temperature x-ray diffraction suggests that the space group changes from P4_12_12 (P4_32_12) to P4_1 (P4_3) at Tc1, and down to P112_1 at Tc2. △ Less

Submitted 1 May, 2022; v1 submitted 4 April, 2022; originally announced April 2022.

Comments: 16 pages, 10 figures

Journal ref: J. Phys. Soc. Jpn. 91, 064702 (2022)

Magnetically hidden state on the ground floor of the magnetic Devil's staircase

Authors: Shusaku Imajo, Naofumi Matsuyama, Toshihiro Nomura, Takumi Kihara, Shintao Nakamura, Christophe Marcenat, Thierry Klein, Gabriel Seyfarth, Chengchao Zhong, Hiroshi Kageyama, Koichi Kindo, Tsutomu Momoi, Yoshimitsu Kohama

Abstract: We investigated the low-temperature and high-field thermodynamic and ultrasonic properties of SrCu2(BO3)2, which exhibits various plateaux in its magnetization curve above 27~T, called a magnetic Devil's staircase. The results of the present study confirm that magnetic crystallization, the first step of the staircase, occurs above 27~T as a 1st-order transition accompanied by a sharp singularity i… ▽ More We investigated the low-temperature and high-field thermodynamic and ultrasonic properties of SrCu2(BO3)2, which exhibits various plateaux in its magnetization curve above 27~T, called a magnetic Devil's staircase. The results of the present study confirm that magnetic crystallization, the first step of the staircase, occurs above 27~T as a 1st-order transition accompanied by a sharp singularity in heat capacity $C_p$ and a kink in the elastic constant. In addition, we observe a thermodynamic anomaly at lower fields around 26~T, which has not been previously detected by any magnetic probes. At low temperatures, this magnetically hidden state has a large entropy and does not exhibit Schottky-type gapped behavior, which suggests the existence of low-energy collective excitations. Based on our observations and theoretical predictions, we propose that magnetic quadrupoles form a spin-nematic state around 26~T as a hidden state on the ground floor of the magnetic Devil's staircase. △ Less

Submitted 3 October, 2022; v1 submitted 14 March, 2022; originally announced March 2022.

Journal ref: Phys. Rev. Lett. 129, 147201 (2022)

Complex magnetic phase diagram with a small phase pocket in a three-dimensional frustrated magnet CuInCr$_{4}$S$_{8}$

Authors: M. Gen, H. Ishikawa, A. Ikeda, A. Miyake, Z. Yang, Y. Okamoto, M. Mori, K. Takenaka, H. Sagayama, T. Kurumaji, Y. Tokunaga, T. Arima, M. Tokunaga, K. Kindo, Y. H. Matsuda, Y. Kohama

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

Submitted 24 January, 2023; v1 submitted 16 December, 2021; originally announced December 2021.

Comments: 13 pages, 12 figures. Published in Phys. Rev. Research

Emergent anisotropy in the Fulde-Ferrell-Larkin-Ovchinnikov state

Authors: Shusaku Imajo, Toshihiro Nomura, Yoshimitsu Kohama, Koichi Kindo

Abstract: Exotic superconductivity is formed by unconventional electron pairing and exhibits various unique properties that cannot be explained by the basic theory. The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state is known as an exotic superconducting state in that the electron pairs have a finite center-of-mass momentum leading to a spatially modulated pattern of superconductivity. The spatial modulation… ▽ More Exotic superconductivity is formed by unconventional electron pairing and exhibits various unique properties that cannot be explained by the basic theory. The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state is known as an exotic superconducting state in that the electron pairs have a finite center-of-mass momentum leading to a spatially modulated pattern of superconductivity. The spatial modulation endows the FFLO state with emergent anisotropy. However, the anisotropy has never been experimentally verified despite numerous efforts over the years. Here, we report detection of anisotropic acoustic responses depending on the sound propagation direction appearing above the Pauli limit. This anisotropy reveals that the two-dimensional FFLO state has a center-of-mass momentum parallel to the nesting vector on the Fermi surface. The present findings will facilitate our understanding of not only superconductivity in solids but also exotic pairings of various particles. △ Less

Submitted 3 October, 2022; v1 submitted 25 October, 2021; originally announced October 2021.

Journal ref: Nature Communications 13, 5590 (2022)

Physical properties of liquid oxygen under ultrahigh magnetic fields

Authors: T. Nomura, A. Ikeda, M. Gen, A. Matsuo, K. Kindo, Y. Kohama, Y. H. Matsuda, S. Zherlitsyn, J. Wosnitza, H. Tsuda, T. C. Kobayashi

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

Submitted 11 September, 2021; originally announced September 2021.

Comments: 10 pages, 10 figures. arXiv admin note: text overlap with arXiv:1906.01207

NMR measurements in dynamically controlled field pulse

Authors: Yoshihiko Ihara, Kaoru Hayashi, Tomoki Kanda, Kazuki Matsui, Koichi Kindo, Yoshimitsu Kohama

Abstract: We present the architecture of the versatile NMR spectrometer with software-defined radio (SDR) technology and its application to the dynamically controlled pulsed magnetic fields. The pulse-field technology is the only solution to access magnetic fields greater than 50 T, but the NMR experiment in the pulsed magnetic field was difficult because of the continuously changing field strength. The dyn… ▽ More We present the architecture of the versatile NMR spectrometer with software-defined radio (SDR) technology and its application to the dynamically controlled pulsed magnetic fields. The pulse-field technology is the only solution to access magnetic fields greater than 50 T, but the NMR experiment in the pulsed magnetic field was difficult because of the continuously changing field strength. The dynamically controlled field pulse allows us to perform NMR experiment in a quasi-steady field condition by creating a constant magnetic field for a short time around the peak of the field pulse. We confirmed the reproducibility of the field pulses using the NMR spectroscopy as a high precision magnetometer. With the highly reproducible field strength we succeeded in measuring the nuclear spin-lattice relaxation rate $1/T_1$, which had never been measured by the pulse-field NMR experiment without dynamic field control. We also implement the NMR spectrum measurement with both the frequency-sweep and field-sweep modes and discuss the appropriate choice of these modes depending on the magnetic properties of sample to be measured. This development, with further improvement at a long-duration field pulse, will innovate the microscopic measurement in extremely high magnetic fields. △ Less

Submitted 20 August, 2021; originally announced August 2021.

Comments: 8 pages, 8 figures

Extraordinary $π$-Electron Superconductivity Emerging from a Quantum Spin Liquid

Authors: Shusaku Imajo, Shiori Sugiura, Hiroki Akutsu, Yoshimitsu Kohama, Takayuki Isono, Taichi Terashima, Koichi Kindo, Shinya Uji, Yasuhiro Nakazawa

Abstract: Quantum spin liquids (QSLs), in which spins are highly entangled, have been considered a groundwork for generating exotic superconductivity.Despite numerous efforts, superconductivity emerging from QSLs has been unrealized in actual materials due to the difficulties in stabilizing QSL states with metallic conductivity.Recently, an organic compound, $κ$-(BEDT-TTF)$_4$Hg$_{2.89}$Br$_8$, with a nearl… ▽ More Quantum spin liquids (QSLs), in which spins are highly entangled, have been considered a groundwork for generating exotic superconductivity.Despite numerous efforts, superconductivity emerging from QSLs has been unrealized in actual materials due to the difficulties in stabilizing QSL states with metallic conductivity.Recently, an organic compound, $κ$-(BEDT-TTF)$_4$Hg$_{2.89}$Br$_8$, with a nearly regular triangular lattice of molecular dimers was recognized as a candidate for doped QSLs. In this study, we report an unusual superconducting phase of $κ$-(BEDT-TTF)$_4$Hg$_{2.89}$Br$_8$: unexpectedly large ratios of the upper critical field to the critical temperature $H_{\rm c2}$/$T_{\rm c}$ in fields not only parallel but also perpendicular to the two-dimensional conducting layers and a very wide region of fluctuating superconductivity above $T_{\rm c}$.Our results reveal that these peculiarities arise from strong electron correlations and possible quantum criticality unique to the doped QSL state, leading to a heavy mass of itinerant carriers and a large superconducting energy gap. △ Less

Submitted 17 June, 2021; originally announced June 2021.

Journal ref: Phys. Rev. Research 3, 033026 (2021)

High-mobility two-dimensional carriers from surface Fermi arcs in magnetic Weyl semimetal films

Authors: Shingo Kaneta-Takada, Yuki K. Wakabayashi, Yoshiharu Krockenberger, Toshihiro Nomura, Yoshimitsu Kohama, Sergey A. Nikolaev, Hena Das, Hiroshi Irie, Kosuke Takiguchi, Shinobu Ohya, Masaaki Tanaka, Yoshitaka Taniyasu, Hideki Yamamoto

Abstract: High-mobility two-dimensional carriers originating from surface Fermi arcs in magnetic Weyl semimetals are highly desired for accessing exotic quantum transport phenomena and for topological electronics applications. Here, we demonstrate high-mobility two-dimensional carriers that show quantum oscillations in magnetic Weyl semimetal SrRuO3 epitaxial films by systematic angle-dependent, high-magnet… ▽ More High-mobility two-dimensional carriers originating from surface Fermi arcs in magnetic Weyl semimetals are highly desired for accessing exotic quantum transport phenomena and for topological electronics applications. Here, we demonstrate high-mobility two-dimensional carriers that show quantum oscillations in magnetic Weyl semimetal SrRuO3 epitaxial films by systematic angle-dependent, high-magnetic field magnetotransport experiments. The exceptionally high-quality SrRuO3 films were grown by state-of-the-art oxide thin film growth technologies driven by machine learning algorithm. The quantum oscillations for the 10-nm SrRuO3 film show a high quantum mobility of 3500 cm2/Vs, a light cyclotron mass, and two-dimensional angular dependence, which can be attributed to the surface Fermi arcs. The linear thickness dependence of the phase shift of the quantum oscillations provides evidence for the non-trivial nature of the quantum oscillations mediated by the surface Fermi arcs. In addition, at low temperatures and under magnetic fields of up to 52 T, the quantum limit of SrRuO3 manifests the chiral anomaly of the Weyl nodes. Emergence of the hitherto hidden two-dimensional Weyl states in a ferromagnetic oxide pave the way to explore novel quantum transport phenomena for topological oxide electronics. △ Less

Submitted 22 December, 2021; v1 submitted 6 June, 2021; originally announced June 2021.

Revealing three-dimensional quantum criticality by Sr-substitution in Han Purple

Authors: Stephan Allenspach, Pascal Puphal, Joosep Link, Ivo Heinmaa, Ekaterina Pomjakushina, Cornelius Krellner, Jakob Lass, Gregory S. Tucker, Christof Niedermayer, Shusaku Imajo, Yoshimitsu Kohama, Koichi Kindo, Steffen Krämer, Mladen Horvatić, Marcelo Jaime, Alexander Madsen, Antonietta Mira, Nicolas Laflorencie, Frédéric Mila, Bruce Normand, Christian Rüegg, Raivo Stern, Franziska Weickert

Abstract: Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous "quasi-one-dimensional" coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3… ▽ More Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous "quasi-one-dimensional" coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3D), quasi-2D systems are special for several physical reasons. Motivated by the ancient pigment Han Purple (BaCuSi$_{2}$O$_{6}$), a quasi-2D material displaying anomalous critical properties, we present a complete analysis of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$. We measure the zero-field magnetic excitations by neutron spectroscopy and deduce the magnetic Hamiltonian. We probe the field-induced transition by combining magnetization, specific-heat, torque and magnetocalorimetric measurements with low-temperature nuclear magnetic resonance studies near the QPT. By a Bayesian statistical analysis and large-scale Quantum Monte Carlo simulations, we demonstrate unambiguously that observable 3D quantum critical scaling is restored by the structural simplification arising from light Sr-substitution in Han Purple. △ Less

Submitted 9 June, 2021; v1 submitted 11 March, 2021; originally announced March 2021.

Comments: 19 pages, 5 figures

Journal ref: Phys. Rev. Research 3, 023177 (2021)

Higher magnetic-field generation by a mass-loaded single-turn coil

Authors: M. Gen, A. Ikeda, S. Kawachi, T. Shitaokoshi, Y. H. Matsuda, Y. Kohama, T. Nomura

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

Submitted 19 February, 2021; originally announced February 2021.

Comments: 6 pages, 5 figures, Accepted in Review of Scientific Instruments

Normal state specific heat in the cuprates La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+δ}$ near the critical point of the pseudogap phase

Authors: C. Girod, D. LeBoeuf, A. Demuer, G. Seyfarth, S. Imajo, K. Kindo, Y. Kohama, M. Lizaire, A. Legros, A. Gourgout, H. Takagi, T. Kurosawa, M. Oda, N. Momono, J. Chang, S. Ono, G. -q. Zheng, C. Marcenat, L. Taillefer, T. Klein

Abstract: The specific heat $C$ of the cuprate superconductors La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+δ}$ was measured at low temperature (down to $0.5~{\rm K}$), for dopings $p$ close to $p^\star$, the critical doping for the onset of the pseudogap phase. A magnetic field up to $35~{\rm T}$ was applied to suppress superconductivity, giving direct access to the normal state at low t… ▽ More The specific heat $C$ of the cuprate superconductors La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+δ}$ was measured at low temperature (down to $0.5~{\rm K}$), for dopings $p$ close to $p^\star$, the critical doping for the onset of the pseudogap phase. A magnetic field up to $35~{\rm T}$ was applied to suppress superconductivity, giving direct access to the normal state at low temperature, and enabling a determination of $C_e$, the electronic contribution to the normal-state specific heat, at $T \to 0$. In La$_{2-x}$Sr$_x$CuO$_4$ at $x=p = 0.22$, $0.24$ and $0.25$, $C_e / T = 15-16~{\rm mJmol}^{-1}{\rm K}^{-2}$ at $T = 2~{\rm K}$, values that are twice as large as those measured at higher doping ($p > 0.3$) and lower doping ($p < 0.15$). This confirms the presence of a broad peak in the doping dependence of $C_e$ at $p^\star\simeq 0.19$, as previously reported for samples in which superconductivity was destroyed by Zn impurities. Moreover, at those three dopings, we find a logarithmic growth as $T \to 0$, such that $C_e / T \sim {\rm B}\ln(T_0/T)$. The peak vs $p$ and the logarithmic dependence vs $T$ are the two typical thermodynamic signatures of quantum criticality. In the very different cuprate Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+δ}$, we again find that $C_e / T \sim {\rm B}\ln(T_0/T$) at $p \simeq p^\star$, strong evidence that this $\ln(1/T)$ dependence - first discovered in the cuprates La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ and La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ - is a universal property of the pseudogap critical point. All four materials display similar values of the $\rm B$ coefficient, indicating that they all belong to the same universality class. △ Less

Submitted 22 January, 2021; originally announced January 2021.

Comments: 8 pages, 6 figures

Journal ref: Phys. Rev. B 103, 214506 (2021)

Combination of Optical Transitions of Polarons with Rashba Effect in Methylammonium Lead Tri-halide Perovskites under High Magnetic Fields

Authors: Halim Choi, Yong Ho Shin, Chang Soo Park, Yongmin Kim, Daeyoung Park, Moon Seok Jeong, Hiroyuki Nojiri, Zhuo Yang, Yoshimitsu Kohama

Abstract: We investigate photoluminescence (PL) transitions of MAPbX$_{3}$ (X = I, Br and Cl) organic-inorganic hybrid perovskite single crystals under magnetic fields of up to 60 T. In these materials, sharp free-exciton transition peaks emerge at a low temperature (4.2 K). Under strong magnetic fields, the free-exciton PL transitions of three different halogens show dramatic differences. The free-exciton… ▽ More We investigate photoluminescence (PL) transitions of MAPbX$_{3}$ (X = I, Br and Cl) organic-inorganic hybrid perovskite single crystals under magnetic fields of up to 60 T. In these materials, sharp free-exciton transition peaks emerge at a low temperature (4.2 K). Under strong magnetic fields, the free-exciton PL transitions of three different halogens show dramatic differences. The free-exciton transitions of the MAPbCl$_{3}$ crystal undergo negative energy shifts, while those of the MAPbBr$_{3}$ crystal show normal diamagnetic shifts. To obtain the variation from Cl to Br, we attempt to measure PL transitions of MAPbCl$_{x}$Br$_{3-x}$. For MAPbI$_{3}$, the transition-energy shifts for both $σ^{+}$ and $σ^{-}$ transitions at 4.2 K exhibit a power-law dependence on the magnetic field. Such inconsistent magnetic-field effects on different halogens make it difficult to understand the transition-energy behavior through a unified model. We propose a possible mechanism for the field effects that is based on a combination of the Rashba effect induced by strong spin-orbit coupling and the polaron effect caused by the polar nature of the inorganic elements. △ Less

Submitted 28 April, 2021; v1 submitted 18 January, 2021; originally announced January 2021.

Comments: 31 pages, 12 figures

Journal ref: Phys. Rev. B 104, 035205 (2021)

Emergence of Frustrated Short-Range Order above Long-Range Order in the $S=1/2$ Kagome Antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O

Authors: Yoshihiko Ihara, Kazuki Matsui, Yoshimitsu Kohama, Sven Luther, Daryna Opherden, Jochen Wosnitza, Hannes Kühne, Hiroyuki K. Yoshida

Abstract: We report on the low-energy dynamics in the kagome antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O (Ca-kapellasite) as studied by use of $^2$D-NMR measurements. Previous $^{35}$Cl-NMR measurements revealed that the nuclear spin-lattice relaxation rate ($1/T_1$) shows two peaks at temperatures, $T^{\ast} = 7.2$ K and $T_s \simeq 25$ K. While the low-temperature peak at $T^{\ast}$ is ascribed t… ▽ More We report on the low-energy dynamics in the kagome antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O (Ca-kapellasite) as studied by use of $^2$D-NMR measurements. Previous $^{35}$Cl-NMR measurements revealed that the nuclear spin-lattice relaxation rate ($1/T_1$) shows two peaks at temperatures, $T^{\ast} = 7.2$ K and $T_s \simeq 25$ K. While the low-temperature peak at $T^{\ast}$ is ascribed to the critical fluctuations near the long-range magnetic ordering, the origin of the high-temperature peak has not been fully understood. From the $1/T_1$ measurements on the D sites at the OD groups (D$_{\rm OD}$), we find no peak at $T_s$, evidencing that the high-temperature peak is not related to the molecular dynamics of the OD groups. We discuss the possibility of a frustration-induced short-range ordered state below $T_s$ before the long-range order is stabilized by the Dzyaloshinskii-Moriya interaction. We also observed static internal fields at the D$_{\rm OD}$ site in the long-range ordered state below $T^{\ast}$, and confirm the previously proposed negative-chirality $q=0$ magnetic structure. △ Less

Submitted 6 January, 2021; originally announced January 2021.

Comments: 5 pages, 4 figures