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Tokiwa, Yoshifumi; Opletal, P.; Sakai, Hironori; Kambe, Shinsaku; Yamamoto, Etsuji; Kimata, Motoi*; Awaji, Satoshi*; Sasaki, Takahiko*; Aoki, Dai*; Haga, Yoshinori; et al.
Physical Review B, 109(14), p.L140502_1 - L140502_6, 2024/04
Times Cited Count：5 Percentile：75.63(Materials Science, Multidisciplinary)The normal-conducting state of the superconductor UTe is studied by entropy analysis for magnetic fields along the 
-axis, obtained from magnetization using the relation 
. We observe a strong increase in entropy with magnetic field due to metamagnetic fluctuations (spatially uniform, 
). The field dependence is well described by the Hertz-Millis-Moriya theory for quantum criticality of itinerant metamagnetism. Notably, the lower bound of the quantum-critical region coincides well with the position of the minimum in the superconducting transition temperature 
. Hence, our results suggest that fluctuations reinforce the superconductivity.
Zhao, K.*; Tokiwa, Yoshifumi; Chen, H.*; Gegenwart, P.*
Nature Physics, 20(3), p.442 - 449, 2024/03
Times Cited Count：10 Percentile：94.39(Physics, Multidisciplinary)In magnetic crystals, despite the explicit breaking of time-reversal symmetry, two equilibrium states related by time reversal are always energetically degenerate. In ferromagnets, this time-reversal degeneracy is reflected in the hysteresis of the magnetic field dependence of the magnetization and, if metallic, in that of the anomalous Hall effect (AHE). Under time-reversal, both these quantities change signs but not their magnitude. Here we show that a time-reversal-like degeneracy appears in the metallic kagome spin ice HoAgGe when magnetic fields are applied parallel to the kagome plane. We find vanishing hysteresis in the field dependence of the magnetization at low temperature, but finite hysteresis in the field-dependent AHE. This suggests the emergence of states with nearly the same energy and net magnetization but different sizes of the AHE and of the longitudinal magnetoresistance. By analysing the experimental data and a minimal tight-binding model, we identify a time-reversal-like operation connecting these near-degenerate states, which is related to the non-trivial distortion of the kagome lattice in HoAgGe. Our work demonstrates the diagnostic power of transport phenomena for identifying hidden symmetries in frustrated spin systems.
Suetsugu, Shota*; Sakai, Hironori; Opletal, P.; Tokiwa, Yoshifumi; Haga, Yoshinori; 12 of others*
Science Advances (Internet), 10(6), p.eadk3772_1 - eadk3772_6, 2024/02
Times Cited Count：10 Percentile：96.78(Multidisciplinary Sciences)Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Opletal, P.; Tokiwa, Yoshifumi; Haga, Yoshinori; Kitagawa, Shunsaku*; Ishida, Kenji*; Aoki, Dai*; Knebel, G.*; et al.
Physical Review Letters, 131(22), p.226503_1 - 226503_7, 2023/12
Times Cited Count：10 Percentile：81.90(Physics, Multidisciplinary)Tokiwa, Yoshifumi; Sakai, Hironori; Kambe, Shinsaku; Opletal, P.; Yamamoto, Etsuji; Kimata, Motoi*; Awaji, Satoshi*; Sasaki, Takahiko*; Yanase, Yoichi*; Haga, Yoshinori; et al.
Physical Review B, 108(14), p.144502_1 - 144502_5, 2023/10
Times Cited Count：6 Percentile：60.56(Materials Science, Multidisciplinary)The vortex dynamics in the spin-triplet superconductor, UTe, are studied by measuring the DC electrical resistivity with currents along the 
-axis under magnetic fields along the -axis. Surprisingly, we have discovered an island region of low critical current deep inside the superconducting (SC) state, well below the SC upper critical field, attributed to a weakening of vortex pinning. Notably, this region coincides with the recently proposed intermediate-field SC state. We discuss the possibility of nonsingular vortices in the intermediate state, where SC order parameter does not vanish entirely in the vortex cores due to the mixing of multiple SC components.
probed by anisotropic low-energy excitationsIshihara, Kota*; Roppongi, Masaki*; Kobayashi, Masayuki*; Imamura, Kumpei*; Mizukami, Yuta*; Sakai, Hironori; Opletal, P.; Tokiwa, Yoshifumi; Haga, Yoshinori; Hashimoto, Kenichiro*; et al.
Nature Communications (Internet), 14, p.2966_1 - 2966_7, 2023/05
Times Cited Count：31 Percentile：97.96(Multidisciplinary Sciences)The superconducting symmetry of the heavy fermion uranium-based superconductor UTe is investigated using low temperature penetration depth measurements. The anisotropic low-energy quasiparticle excitations indicates multiple superconducting components in a chiral complex form. The most consistent is a chiral non-unitary state.
along hard magnetic axisSakai, Hironori; Tokiwa, Yoshifumi; Opletal, P.; Kimata, Motoi*; Awaji, Satoshi*; Sasaki, Takahiko*; Aoki, Dai*; Kambe, Shinsaku; Tokunaga, Yo; Haga, Yoshinori
Physical Review Letters, 130(19), p.196002_1 - 196002_6, 2023/05
Times Cited Count：24 Percentile：95.69(Physics, Multidisciplinary)The superconducting (SC) phase diagram in uranium ditelluride is explored under magnetic fields (
) along the hard magnetic -axis using a high-quality single crystal with 
= 2.1 K. Simultaneous electrical resistivity and AC magnetic susceptibility measurements discern low- and high-field SC (LFSC and HFSC, respectively) phases with contrasting field-angular dependence. Crystal quality increases the upper critical field of the LFSC phase, but the 
of 
T, at which the HFSC phase appears, is always the same through the various crystals. A phase boundary signature is also observed inside the LFSC phase near , indicating an intermediate SC phase characterized by small flux pinning forces.
Ishihara, Kota*; Kobayashi, Masayuki*; Imamura, Kumpei*; Konczykowski, M.*; Sakai, Hironori; Opletal, P.; Tokiwa, Yoshifumi; Haga, Yoshinori; Hashimoto, Kenichiro*; Shibauchi, Takasada*
Physical Review Research (Internet), 5(2), p.L022002_1 - L022002_6, 2023/04
Lower superconducting critical fields 
of UTe have been determined. Orthorhombic UTe has magnetic easy axis along the -axis. We found perpendicular to showed anomalous enhancement. By comparing with anisotropy of upper critical fields, effect of magnetic fluctuations on superconductivity is suggested.
Te
Opletal, P.; Sakai, Hironori; Haga, Yoshinori; Tokiwa, Yoshifumi; Yamamoto, Etsuji; Kambe, Shinsaku; Tokunaga, Yo
Journal of the Physical Society of Japan, 92(3), p.034704_1 - 034704_5, 2023/03
Times Cited Count：2 Percentile：24.57(Physics, Multidisciplinary)We investigate the physical properties of a single crystal of uranium telluride UTe. We have confirmed that UTe crystallizes in the hexagonal structure with three nonequivalent crystallographic uranium sites. The paramagnetic moments are estimated to be approximately 1 
per the uranium site, assuming a uniform moment on all the sites. A ferromagnetic phase transition occurs at 
= 48 K, where the in-plane magnetization increases sharply, whereas the out of-plane component does not increase significantly. With decreasing temperature further below under field-cooling conditions, the out-of-plane component increases rapidly around T
= 26 K. In contrast, the in-plane component hardly changes at T. Specific heat measurement indicates no 
-type anomaly around T, so this is a cross-over suggesting a reorientation of the ordering moments or successive magnetic ordering on the part of the multiple uranium sites.
)Jesche, A.*; Winterhalter-Stocker, N.*; Hirschberger, F.*; Bellon, A.*; Bachus, S.*; Tokiwa, Yoshifumi; Tsirlin, A. A.*; Gegenwart, P.*
Physical Review B, 107(10), p.104402_1 - 104402_8, 2023/03
Times Cited Count：20 Percentile：92.24(Materials Science, Multidisciplinary)Crystal structure, thermodynamic properties, and adiabatic demagnetization refrigeration (ADR) effect in the spin-1/2 triangular antiferromagnet KBaGd(BO) are reported. With the average nearest-neighbor exchange coupling of 44 mK, this compound shows magnetic order below 
= 263 mK in zero field. The ADR tests reach the temperature of 
= 122 mK, more than twice lower than , along with the entropy storage capacity of 192 mJ K
cm
and the hold time of more than 8 h in the PPMS setup, both significantly improved compared to the spin-
Yb
analog. We argue that KBaGd(BO) shows a balanced interplay of exchange and dipolar couplings that together with structural randomness and geometrical frustration shift to well below the ordering temperature , therefore facilitating the cooling.
Aoki, Dai*; Sakai, Hironori; Opletal, P.; Tokiwa, Yoshifumi; Ishizuka, Jun*; Yanase, Yoichi*; Harima, Hisatomo*; Nakamura, Ai*; Li, D.*; Homma, Yoshiya*; et al.
Journal of the Physical Society of Japan, 91(8), p.083704_1 - 083704_5, 2022/08
Times Cited Count：54 Percentile：98.03(Physics, Multidisciplinary) by molten salt flux methodSakai, Hironori; Opletal, P.; Tokiwa, Yoshifumi; Yamamoto, Etsuji; Tokunaga, Yo; Kambe, Shinsaku; Haga, Yoshinori
Physical Review Materials (Internet), 6(7), p.073401_1 - 073401_10, 2022/07
Times Cited Count：47 Percentile：94.54(Materials Science, Multidisciplinary)The molten salt flux method is applied as a new synthetic route for the single crystals of the spin-triplet superconductor UTe. The single crystals under an optimized growth condition with excess uranium exhibit a superconducting transition at 
K, which is the highest reported for this compound. The obtained crystals show a remarkably large residual resistivity ratio with respect to the room temperature value and a small residual electronic contribution in specific heat well below . These results indicate that the increase of in UTe can be achieved by reducing the disorder associated with uranium vacancies. The excess uranium in the molten salt acts as a reducing agent, preventing tetravalent uranium from becoming pentavalent and suppressing creation of uranium vacancies. At the same time, the relatively low growth temperature can suppress Te volatilization.
Haga, Yoshinori; Opletal, P.; Tokiwa, Yoshifumi; Yamamoto, Etsuji; Tokunaga, Yo; Kambe, Shinsaku; Sakai, Hironori
Journal of Physics; Condensed Matter, 34(17), p.175601_1 - 175601_7, 2022/04
Times Cited Count：27 Percentile：85.25(Physics, Condensed Matter)Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Haga, Yoshinori; Tokiwa, Yoshifumi; Opletal, P.; Fujibayashi, Hiroki*; Kinjo, Katsuki*; Kitagawa, Shunsaku*; Ishida, Kenji*; et al.
Journal of the Physical Society of Japan, 91(2), p.023707_1 - 023707_5, 2022/02
Times Cited Count：25 Percentile：91.32(Physics, Multidisciplinary)
Te NMR experiments in field () applied along the easy magnetization axis (the -axis) revealed slow electronic dynamics developing in the paramagnetic state of UTe. The observed slow fluctuations are concerned with a successive growth of long-range electronic correlations below 30
40 K, where the spin susceptibility along the hard magnetization axis (the -axis) shows a broad maximum. The experiments also imply that tiny amounts of disorder or defects locally disturb the long-range electronic correlations and develop an inhomogeneous electronic state at low temperatures, leading to a low temperature upturn observed in the bulk-susceptibility in 
. We suggest that UTe would be located on the paramagnetic side near an electronic phase boundary, where either the magnetic or Fermi-surface instability would be the origin of the characteristic fluctuations.
Tokiwa, Yoshifumi; Bachus, S.*; Kavita, K.*; Jesche, A.*; Tsirlin, A. A.*; Gegenwart, P.*
Communications Materials (Internet), 2(1), p.42_1 - 42_6, 2021/04
Generation of very low temperatures has been crucially important for applications and fundamental research, as low-temperature quantum coherence enables operation of quantum computers and formation of exotic quantum states, such as superfluidity/superconductivity. One of the major techniques to reach milli-Kelvin temperatures is adiabatic demagnetization refrigeration. This method uses almost non-interacting magnetic moments of paramagnetic salts where large distances suppress interactions between the moments. The large spatial separations are facilitated by water molecules, with a drawback of reduced stability of the material. Here, we show that the water-free frustrated magnet KBaYb(BO
)
can be ideal for refrigeration, achieving at least 22 mK. Compared to conventional refrigerants, KBaYb(BO) does not degrade even under high temperatures and ultra-high vacuum. Further, its magnetic frustration and structural randomness enable cooling to temperatures several times lower than the energy scale of magnetic interactions, which is the main limiting factor for the base temperature of conventional refrigerants.
Fujimori, Shinichi; Okochi, Takuo*; Kawasaki, Ikuto; Yasui, Akira; Takeda, Yukiharu; Okane, Tetsuo; Saito, Yuji; Fujimori, Atsushi; Yamagami, Hiroshi; Haga, Yoshinori; et al.
Journal of the Physical Society of Japan, 81(1), p.014703_1 - 014703_9, 2012/01
Times Cited Count：39 Percentile：82.05(Physics, Multidisciplinary)High-energy-resolution core-level and valence-band photoelectron spectroscopic studies were performed for the heavy Fermion uranium compounds UGe, UCoGe, URhGe, URuSi, UNiAl, UPdAl, and UPt as well as typical localized and itinerant uranium compounds to understand the relationship between the uranium valence state and their core-level spectral line shapes. The core-level spectra of UGe, UCoGe, URhGe, URuSi, and UNiAl are rather similar to those of itinerant compounds, suggesting that U 5
electrons in these compounds are well hybridized with ligand states. On the other hand, the core-level spectra of UPdAl and UPt show considerably different spectral line shapes from those of the itinerant compounds, suggesting that U 5 electrons in UPdAl and UPt are less hybridized with ligand states, leading to the correlated nature of U 5 electrons in these compounds.
antiferromagnetism in cubic UIn; 
In-NMR/NQR studySakai, Hironori; Kambe, Shinsaku; Tokunaga, Yo; Chudo, Hiroyuki; Tokiwa, Yoshifumi*; Aoki, Dai*; Haga, Yoshinori; Onuki, Yoshichika; Yasuoka, Hiroshi
Physical Review B, 79(10), p.104426_1 - 104426_7, 2009/03
Times Cited Count：6 Percentile：28.42(Materials Science, Multidisciplinary)In nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements have been performed on an antiferromagnet UIn with the cubic AuCu-type structure. Under zero field, the observation of the NQR spectrum has led to an estimated 
of 11.8 MHz at 90 K. The temperature variation of the NQR relaxation rates (
) far above the N
el temperature 
=88 K approaches a constant value, which indicates a localized nature for the 
-electrons in this system. On the other hand, in the antiferromagnetically ordered state, we propose that the most plausible direction of antiferromagnetic U moments may be 
among the possible orientations of 
, , or 
.
; An Angle-resolved photoemission spectroscopy studyFujimori, Shinichi; Fujimori, Atsushi; Shimada, Kenya*; Narimura, Takamasa*; Kobayashi, Kenichi*; Namatame, Hirofumi*; Taniguchi, Masaki*; Harima, Hisatomo*; Shishido, Hiroaki*; Ikeda, Shugo; et al.
Physical Review B, 73(22), p.224517_1 - 224517_5, 2006/06
Times Cited Count：45 Percentile：82.56(Materials Science, Multidisciplinary)We have performed a high-resolution angle resolved Ce 4
-4 resonant photoemission experiment on the heavy fermion superconductor CeIrIn. We have observed a quasi-particle band which has a energy disepersion of 
30 meV in the Ce 4 on-resonance spectra. The result suggests that although the Ce 4 spectra are dominated by the localized/correlated character being dominant, the small itinerant component is responsible for the superconductivity in this compound.
Fujimori, Shinichi; Terai, Kota; Takeda, Yukiharu; Okane, Tetsuo; Saito, Yuji; Muramatsu, Yasuji; Fujimori, Atsushi; Yamagami, Hiroshi*; Ikeda, Shugo; Matsuda, Tatsuma; et al.
Physica B; Condensed Matter, 378-380, p.995 - 996, 2006/05
Times Cited Count：2 Percentile：11.91(Physics, Condensed Matter)Recently, photoemission experiments in soft X-ray region have attracted much attention due to their high sensitivities for bulk electronic structures of strongly correlated electron system. We have carried out the high-resolution photoemission experiments on some uranium compounds using soft X-ray synchrotron radiation from SPring-8 to understand their electronic structures. Bulk- and U 5-sensitive band structure and Fermi surface were obtained for itinerant U 5 compounds UFeGa and USb, and they are compared with the results of the band structure calculations treating U 5 states as being itinerant. In addition, we show the results of photoemission study on some heavy fermion compounds such as UPdAl and UNiAl. The temperature dependences of the U 5 electronic structure of UPdAl will be also reported.
band states in the layered compound UFeGa observed by soft X-ray angle-resolved photoemission spectroscopyFujimori, Shinichi; Terai, Kota; Takeda, Yukiharu; Okane, Tetsuo; Saito, Yuji; Muramatsu, Yasuji; Fujimori, Atsushi; Yamagami, Hiroshi*; Tokiwa, Yoshifumi*; Ikeda, Shugo; et al.
Physical Review B, 73(12), p.125109_1 - 125109_6, 2006/03
Times Cited Count：22 Percentile：66.04(Materials Science, Multidisciplinary)We have performed angle-resolved photoemission spectroscopy (ARPES) experiments on paramagnetic UFeGa using soft X-ray synchrotron radiation (
=500 eV) and derived the bulk- and U 5-sensitive electronic structure of UFeGa. Although the agreement between the experimental band strucure and the LDA calculation treating U 5 electrons as beeing itinerant is qualitative, the morphology of the Fermi surface is well explained by the calculation. This result claims that the importance of the electron correlation effect even for the itinerant U 5 compound.
