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Journal Articles

Ferromagnetic crossover within the ferromagnetic order of U$$_{7}$$Te$$_{12}$$

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

We investigate the physical properties of a single crystal of uranium telluride U$$_{7}$$Te$$_{12}$$. We have confirmed that U$$_{7}$$Te$$_{12}$$ crystallizes in the hexagonal structure with three nonequivalent crystallographic uranium sites. The paramagnetic moments are estimated to be approximately 1 $$mu_{B}$$ per the uranium site, assuming a uniform moment on all the sites. A ferromagnetic phase transition occurs at $$T_{rm C}$$= 48 K, where the in-plane magnetization increases sharply, whereas the out of-plane component does not increase significantly. With decreasing temperature further below $$T_{rm C}$$ under field-cooling conditions, the out-of-plane component increases rapidly around T$$^{star}$$= 26 K. In contrast, the in-plane component hardly changes at T$$^{star}$$. Specific heat measurement indicates no $$lambda$$-type anomaly around T$$^{star}$$, 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.

Journal Articles

Nested antiferromagnetic spin fluctuations and non-Fermi-liquid behavior in electron-doped CeCo$$_{1-x}$$Ni$$_{x}$$In$$_5$$

Sakai, Hironori; Tokunaga, Yo; Kambe, Shinsaku; Zhu, J.-X.*; Ronning, F.*; Thompson, J. D.*; Kotegawa, Hisashi*; To, Hideki*; Suzuki, Kohei*; Oshima, Yoshiki*; et al.

Physical Review B, 106(23), p.235152_1 - 235152_8, 2022/12

 Times Cited Count:0 Percentile:0(Materials Science, Multidisciplinary)

We investigate the electronic state of Ni-substituted CeCo$$_{1-x}$$Ni$$_x$$In$$_5$$ by nuclear quadrupole and magnetic resonance (NQR/NMR) techniques. The heavy fermion superconductivity below $$T_{rm c} = 2.3$$ K for $$x = 0$$ is suppressed by Ni substitutions, and $$T_{rm c}$$ reaches zero for $$x = 0.25$$. The $$^{115}$$In NQR spectra for $$x = 0.125$$ and 0.25 can be explained by simulating the electrical field gradient that is calculated for a virtual supercell with density functional theory. The spin-lattice relaxation rate $$1/T_1$$ indicates that Ni substitution weakens antiferromagnetic correlations that are not localized near the substituent but instead are uniform in space. The temperature ($$T$$) dependence of $$(T_1T)^{-1}$$ for $$x = 0.25$$ shows a maximum around $$T_{rm g} = 2$$ K and $$(T_1T)^{-1}$$ decreases toward almost zero when temperature is further reduced as if a gap might be opening in the magnetic excitation spectrum; however, the magnetic specific heat and the static magnetic susceptibility evolve smoothly through $$T_{rm g}$$ with a $$-ln T$$ dependence. The peculiar T dependence of $$(T_1T)^{-1}$$ and non-Fermi-liquid specific heat and susceptibility can be interpreted in a unified way by assuming nested antiferromagnetic spin fluctuations in a quasi-two-dimensional electronic system.

Journal Articles

Structural 130 K phase transition and emergence of a two-ion Kondo state in Ce$$_2$$Rh$$_2$$Ga explored by $$^{69,71}$$Ga nuclear quadrupole resonance

Yamamoto, Shingo*; Fujii, Takuto*; Luther, S.*; Yasuoka, Hiroshi*; Sakai, Hironori; B$"a$rtl, F.*; Ranjith, K. M.*; Rosner, H.*; Wosnitza, J.*; Strydom, A. M.*; et al.

Physical Review B, 106(11), p.115125_1 - 115125_5, 2022/09

 Times Cited Count:0 Percentile:0(Materials Science, Multidisciplinary)

We have studied the microscopic magnetic properties, the nature of the 130 K phase transition, and the ground state in the recently synthesized compound Ce$$_2$$Rh$$_2$$Ga by use of $$^{69,71}$$Ga nuclear quadrupole resonance (NQR). The NQR spectra clearly show an unusual phase transition at $$T_tsim130$$ K, yielding a splitting of the high-temperature single NQR line into two well-resolved NQR lines, providing evidence for two crystallographically inequivalent Ga sites. The NQR frequencies are in good agreement with fully relativistic calculations of the band structure. Our NQR results indicate the absence of magnetic or charge order down to 0.3 K. The temperature dependence of the spin-lattice relaxation rate $$1/T_1$$ shows three distinct regimes, with onset temperatures at $$T_t$$ and 2 K. The temperature-independent $$1/T_1$$, observed between $$T_t$$ and 2 K, crosses over to a Korringa process, $$1/T_1propto T$$, below $$sim$$2 K, which evidences a rare two-ion Kondo scenario: The system evolves into a dense Kondo coherent state below 2.0 and 0.8 K probed by the two different Ga sites.

Journal Articles

First observation of the de Haas-van Alphen effect and Fermi surfaces in the unconventional superconductor UTe$$_2$$

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:6 Percentile:94.33(Physics, Multidisciplinary)

Journal Articles

Single crystal growth of superconducting UTe$$_2$$ by molten salt flux method

Sakai, 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:2 Percentile:75.4(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$$_2$$. The single crystals under an optimized growth condition with excess uranium exhibit a superconducting transition at $$T_{rm c}=2.1$$ K, which is the highest $$T_{rm c}$$ 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 $$T_{rm c}$$. These results indicate that the increase of $$T_{rm c}$$ in UTe$$_2$$ 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.

Journal Articles

Homogeneity of (U, $$M$$)O$$_2$$ ($$M$$ = Th, Np) prepared by supercritical hydrothermal synthesis

Shirasaki, Kenji*; Tabata, Chihiro*; Sunaga, Ayaki*; Sakai, Hironori; Li, D.*; Konaka, Mariko*; Yamamura, Tomoo*

Journal of Nuclear Materials, 563, p.153608_1 - 153608_11, 2022/05

 Times Cited Count:2 Percentile:71.47(Materials Science, Multidisciplinary)

We focused on the direct synthesis of (U, $$M$$)O$$_2$$ solid solution ($$M$$=Th, Np) by extending our recent progress in hydrothermal synthesis with additives. The homogeneity of the (U, $$M$$)O$$_2$$ ($$M$$ = Th, Np) systems prepared by supercritical hydrothermal reactions was investigated through crystallographic analysis based on Vegard's law, and the $$^{23}$$Na nuclear magnetic resonance (NMR) measurement of (U, Np, Na)O$$_2$$ solid solutions. Our experimental and analytical results revealed that (i) an optimal additive is ammonium carbonate and starting uranium valence is IV in the case of (U, Th)O$$_{2+x}$$, and (ii) an optimal additive is ethanol and starting uranium valence is VI in the case of (U, Np)O$$_{2+x}$$, for producing the homogeneous solid solutions by hydrothermal synthesis.

Journal Articles

Effect of uranium deficiency on normal and superconducting properties in unconventional superconductor UTe$$_2$$

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:5 Percentile:92.43(Physics, Condensed Matter)

Journal Articles

Drastic change in magnetic anisotropy of UTe$$_2$$ under pressure revealed by $$^{125}$$Te-NMR

Kinjo, Katsuki*; Fujibayashi, Hiroki*; Nakamine, Genki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Nakamura, Ai*; Shimizu, Yusei*; et al.

Physical Review B, 105(14), p.L140502_1 - L140502_5, 2022/04

 Times Cited Count:2 Percentile:78.71(Materials Science, Multidisciplinary)

Journal Articles

Slow electronic dynamics in the paramagnetic state of UTe$$_2$$

Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Haga, Yoshinori; Tokiwa, Yoshifumi; Opletal, P.; Fujibayashi, Hiroyuki*; 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:6 Percentile:95.83(Physics, Multidisciplinary)

$$^{125}$$Te NMR experiments in field ($$H$$) applied along the easy magnetization axis (the $$a$$-axis) revealed slow electronic dynamics developing in the paramagnetic state of UTe$$_2$$. 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 $$b$$-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 $$H|a$$. We suggest that UTe$$_2$$ 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.

Journal Articles

Supercritical hydrothermal synthesis of UO$$_{2+x}$$; Stoichiometry, crystal shape and size, and homogeneity observed using $$^{23}$$Na-NMR spectroscopy of (U, Na)O$$_{2+x}$$

Tabata, Chihiro*; Shirasaki, Kenji*; Sunaga, Ayaki*; Sakai, Hironori; Li, D.*; Konaka, Mariko*; Yamamura, Tomoo*

CrystEngComm (Internet), 23(48), p.8660 - 8672, 2021/12

 Times Cited Count:4 Percentile:51.64(Chemistry, Multidisciplinary)

The hydrothermal synthesis of pure uranium dioxide under supercritical water (SCW) conditions was investigated. The nonstoichiometry, crystallite size and morphology of the UO$$_{2+x}$$ particles were investigated. The SCW hydrothermal synthesis may be a promising method for producing homogeneous UO$$_{2+x}$$ and its solid solutions with well-defined nonstoichiometries ($$x$$), shapes, and sizes.

Journal Articles

Nanoscale heterogeneity induced by nonmagnetic Zn dopants in the quantum critical metal CeCoIn$$_5$$; $$^{115}$$In NQR/NMR and $$^{59}$$Co NMR study

Sakai, Hironori; Tokunaga, Yo; Kambe, Shinsaku; Zhu, J.-X.*; Ronning, F.*; Thompson, J. D.*; Ramakrishna, S. K.*; Reyes, A. P.*; Suzuki, Kohei*; Oshima, Yoshiki*; et al.

Physical Review B, 104(8), p.085106_1 - 085106_12, 2021/08

 Times Cited Count:2 Percentile:34.91(Materials Science, Multidisciplinary)

Antiferromagnetism in a prototypical quantum critical metal CeCoIn$$_5$$ is known to be induced by slight substitutions of non-magnetic Zn atoms for In. In nominally 7% Zn substituted CeCoIn$$_5$$, an antiferromagnetic (AFM) state coexists with heavy fermion superconductivity. Heterogeneity of the electronic states is investigated in Zn doped CeCoIn$$_5$$ by means of nuclear quadrupole and magnetic resonances (NQR and NMR). Site-dependent NQR relaxation rates $$1/T_1$$ indicate that the AFM state is locally nucleated around Zn substituents in the matrix of a heavy fermion state, and percolates through the bulk at the AFM transition temperature $$T_{rm N}$$. At lower temperatures, an anisotropic superconducting (SC) gap below the SC transition temperature $$T_{rm c}$$, and the SC state permeates through the AFM regions via a SC proximity effect. Applying an external magnetic field induces a spin-flop transition near 5 T, reducing the volume of the AFM regions. Consequently, a short ranged inhomogeneous AFM state survives and coexists with a paramagnetic Fermi liquid state at high fields.

Journal Articles

Critical slowing-down and field-dependent paramagnetic fluctuations in the skyrmion host EuPtSi; $$mu$$SR and NMR studies

Higa, Nonoka*; Ito, Takashi; Yogi, Mamoru*; Hattori, Taisuke; Sakai, Hironori; Kambe, Shinsaku; Guguchia, Z.*; Higemoto, Wataru; Nakashima, Miho*; Homma, Yoshiya*; et al.

Physical Review B, 104(4), p.045145_1 - 045145_7, 2021/07

 Times Cited Count:0 Percentile:0(Materials Science, Multidisciplinary)

Journal Articles

Inhomogeneous superconducting state probed by $$^{125}$$Te NMR on UTe$$_2$$

Nakamine, Genki*; Kinjo, Katsuki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Nakamura, Ai*; Shimizu, Yusei*; Homma, Yoshiya*; et al.

Journal of the Physical Society of Japan, 90(6), p.064709_1 - 064709_7, 2021/06

 Times Cited Count:9 Percentile:85.59(Physics, Multidisciplinary)

Journal Articles

Anisotropic response of spin susceptibility in the superconducting state of UTe$$_2$$ probed with $$^{125}$$Te-NMR measurement

Nakamine, Genki*; Kinjo, Katsuki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Nakamura, Ai*; Shimizu, Yusei*; Homma, Yoshiya*; et al.

Physical Review B, 103(10), p.L100503_1 - L100503_5, 2021/03

 Times Cited Count:16 Percentile:93.29(Materials Science, Multidisciplinary)

Journal Articles

Universal scaling behavior under pressure in the heavy-fermion antiferromagnet CeRh$$_2$$Si$$_2$$; $$^{29}$$Si NMR study

Sakai, Hironori; Matsumoto, Yuji*; Haga, Yoshinori; Tokunaga, Yo; Kambe, Shinsaku

Physical Review B, 103(8), p.085114_1 - 085114_8, 2021/02

 Times Cited Count:0 Percentile:0(Materials Science, Multidisciplinary)

The microscopic origin of a magnetic phase diagram under pressure in a heavy fermion antiferromagnet CeRh$$_2$$Si$$_2$$ was investigated using the $$^{29}$$Si nuclear magnetic resonance (NMR) technique. We investigated the temperature and pressure dependencies of $$q$$-independent local fluctuations caused by the single-site Kondo effect. A universal scaling behavior observed on the energy scale of the local fluctuations in an entire pressure region demonstrates that a characteristic energy scale $$T_0$$ of Kondo interactions monotonically increases by applying pressure without a critical anomaly around the quantum critical pressure $$P_{rm c}$$ of antiferromagnetism. Our NMR result agrees with the Doniach picture of the heavy-fermion phase diagram, where the progressive delocalization of the $$f$$-electrons occurs across $$P_{rm c}$$, accompanied by the development of antiferromagnetic correlations among the $$f$$-electrons.

Journal Articles

Orbitally defined field-induced electronic state in a Kondo lattice

Lessux, G. G.*; Sakai, Hironori; Hattori, Taisuke*; Tokunaga, Yo; Kambe, Shinsaku; Kuhns, P. L.*; Reyes, A. P.*; Thompson, J. D.*; Pagliuso, P. G.*; Urbano, R. R.*

Physical Review B, 101(16), p.165111_1 - 165111_6, 2020/04

 Times Cited Count:6 Percentile:51.79(Materials Science, Multidisciplinary)

CeRhIn$$_5$$ is a Kondo-lattice prototype in which a magnetic field $$B^{ast}$$ $$simeq$$ 31T induces an abrupt Fermi-surface (FS) reconstruction and pronounced in-plane electrical transport anisotropy all within its antiferromagnetic state. Here we report low-temperature nuclear magnetic resonance (NMR) measurements revealing a pronounced decrease in the $$^{115}$$In formal Knight shift, without changes in crystal or magnetic structures, of CeRhIn$$_5$$ at fields ($$||c$$) spanning $$B^{ast}$$. We discuss the emergent state above $$B^{ast}$$ in terms of a change in Ce's 4$$f$$ orbitals that arises from field-induced evolution of crystal-electric field (CEF) energy levels. This change in orbital character enhances hybridization between the 4$$f$$ and the conduction electrons that leads ultimately to an itinerant quantum-critical point at $$B_{c0}$$ $$simeq$$ 50T.

Journal Articles

$$^{33}$$S nuclear magnetic resonance spectra of uranium disulfide $$beta$$-US$$_2$$

Sakai, Hironori; Tokunaga, Yo; Haga, Yoshinori; Kambe, Shinsaku; Ramakrishna, S. K.*; Reyes, A. P.*; Rosa, P. F. S.*; Ronning, F.*; Thompson, J. D.*; Fisk, Z.*; et al.

JPS Conference Proceedings (Internet), 30, p.011169_1 - 011169_6, 2020/03

Uranium disulfide $$beta$$-US$$_2$$ showing a semimetal-to-semiconductor crossover has been investigated by the nuclear magnetic resonance (NMR) technique for $$^{33}$$S nuclei with the nuclear spin of $$I=3/2$$. Since the natural concentration 0.76% of NMR active $$^{33}$$S nuclei is too dilute, the isotopic enrichment to $$sim$$50% has been carried out for the single crystal growth. The $$^{33}$$S NMR spectra have been successfully obtained using a single crystal of $$beta$$-US$$_2$$ with external fields along the crystallographic $$c$$ axis. The S sites assignments have been made based on these NMR spectra.

Journal Articles

Superconducting properties of heavy fermion UTe$$_2$$ revealed by $$^{125}$$Te-nuclear magnetic resonance

Nakamine, Genki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Nakamura, Ai*; Shimizu, Yusei*; Homma, Yoshiya*; Li, D.*; et al.

Journal of the Physical Society of Japan, 88(11), p.113703_1 - 113703_4, 2019/11

 Times Cited Count:44 Percentile:94.58(Physics, Multidisciplinary)

Journal Articles

Novel universality class for the ferromagnetic transition in the low carrier concentration systems UTeS and USeS exhibiting large negative magnetoresistance

Tateiwa, Naoyuki; Haga, Yoshinori; Sakai, Hironori; Yamamoto, Etsuji

Physical Review B, 100(6), p.064413_1 - 064413_7, 2019/08

 Times Cited Count:1 Percentile:6.16(Materials Science, Multidisciplinary)

We report the novel critical behavior of magnetization in low carrier concentration systems UTeS and USeS that exhibit the large negative magnetoresistance around the ferromagnetic transition temperatures $$T_{rm C}$$ $$sim$$ 85 and 23 K, respectively. We determine the critical exponents, $$beta$$ for the spontaneous magnetization $$M_{rm s}$$, $$gamma$$ for the magnetic susceptibility $$chi$$, and $$delta$$ for the magnetization isotherm at $$T_{rm C}$$ with several analytical methods. The ferromagnetic states in UTeS and USeS have strong uniaxial magnetic anisotropy. However, the critical exponents in the two compounds are different from those in the three-dimensional Ising system. Similar exponents have been reported for the uranium ferromagnetic superconductors UGe$$_2$$ and URhGe. An important finding is that the novel critical phenomenon appears regardless of the charge carrier density or the degree of the itinerancy of the $$5f$$ electrons.

Journal Articles

$$^{125}$$Te-NMR study on a single crystal of heavy fermion superconductor UTe$$_2$$

Tokunaga, Yo; Sakai, Hironori; Kambe, Shinsaku; Hattori, Taisuke; Higa, Nonoka; Nakamine, Genki*; Kitagawa, Shunsaku*; Ishida, Kenji*; Nakamura, Ai*; Shimizu, Yusei*; et al.

Journal of the Physical Society of Japan, 88(7), p.073701_1 - 073701_4, 2019/07

 Times Cited Count:47 Percentile:95.05(Physics, Multidisciplinary)

We report $$^{125}$$Te-NMR studies on a newly discovered heavy fermion superconductor UTe$$_2$$. Using a single crystal, we have measured the $$^{125}$$Te-NMR Knight shift $$K$$ and spin-lattice relaxation rate $$1/T_1$$ for fields along the three orthorhombic crystal axes. The data confirm a moderate Ising anisotropy for both the static ($$K$$) and dynamical susceptibilities ($$1/T_1$$) in the paramagnetic state above about 20 K. Around 20 K, however, we have observed a sudden loss of NMR spin-echo signal due to sudden enhancement of the NMR spin-spin relaxation rate $$1/T_2$$, when the field is applied along the easy axis of magnetization (=$$a$$ axis). This behavior suggests the development of longitudinal magnetic fluctuations along the $$a$$ axis at very low frequencies below 20 K.

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