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Field-induced anomaly in the anisotropic non-Fermi-liquid normal state of UBe$_{13}$
Authors:
Yusei Shimizu,
Shunichiro Kittaka,
Yohei Kono,
Shota Nakamura,
Yoshinori Haga,
Etsuji Yamamoto,
Kazushige Machida,
Hiroshi Amitsuka,
Toshiro Sakakibara
Abstract:
We report the results of high-resolution dc magnetization and specific-heat measurements at very low temperatures for
a single crystal \color{black} of UBe$_{13}$ in magnetic fields applied along the [001] and [111] directions, in both the normal and superconducting states. In the normal state, magnetic susceptibility $χ(T) = M/H$ exhibits a logarithmic temperature dependence over a wide tempera…
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We report the results of high-resolution dc magnetization and specific-heat measurements at very low temperatures for
a single crystal \color{black} of UBe$_{13}$ in magnetic fields applied along the [001] and [111] directions, in both the normal and superconducting states. In the normal state, magnetic susceptibility $χ(T) = M/H$ exhibits a logarithmic temperature dependence over a wide temperature range (1-20 K). However, with increasing field, this non-Fermi-liquid (NFL) behavior of $χ(T) $ at low temperatures is suppressed. Moreover, a susceptibility maximum occurs below 4 T, whereas Fermi-liquid coherence is recovered above 8 T. In addition, thermodynamic anomalies ($T_{\rm A}$ and $H_{\rm A}$) occur in both magnetic susceptibility and specific heat at intermediate fields (6--10 T) along the [111] direction. Furthermore, a nontrivial fifth-order nonlinear susceptibility is observed in the normal-state magnetization of UBe$_{13}$. These results suggest a close relationship between the field-induced multipolar correlations of $5f$-electron degrees of freedom and the Fermi-surface reconstruction accompanying the crossover from the NFL state to the Fermi-liquid state in UBe$_{13}$.
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Submitted 22 December, 2025;
originally announced December 2025.
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Probing magnetic-field-induced multipolar ordering through field-angle-resolved magnetostriction and thermal expansion in PrIr$_2$Zn$_{20}$
Authors:
Naoki Okamoto,
Yohei Kono,
Takahiro Onimaru,
Keisuke T. Matsumoto,
Kazumasa Hattori,
Shunichiro Kittaka
Abstract:
We performed field-angle-resolved magnetostriction and thermal-expansion measurements on PrIr$_2$Zn$_{20}$, a cubic non-Kramers compound exhibiting antiferroquadrupolar order below $T_{\rm Q}=0.125$ K. Thermal expansion exhibits two qualitatively different anomalies under magnetic fields applied along the $[001]$ direction, providing experimental support for the existence of an intermediate A phas…
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We performed field-angle-resolved magnetostriction and thermal-expansion measurements on PrIr$_2$Zn$_{20}$, a cubic non-Kramers compound exhibiting antiferroquadrupolar order below $T_{\rm Q}=0.125$ K. Thermal expansion exhibits two qualitatively different anomalies under magnetic fields applied along the $[001]$ direction, providing experimental support for the existence of an intermediate A phase previously reported. Furthermore, comparison between the experimental results and theoretical modeling indicates a strong anisotropic coupling of the $O_{20}$ quadrupolar moment, which plays a key role in stabilizing the A phase. These findings demonstrate that multipolar states in non-Kramers systems can be effectively tuned by magnetic-field orientation, providing insights into the anisotropic nature of quadrupolar interactions.
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Submitted 22 December, 2025; v1 submitted 25 November, 2025;
originally announced November 2025.
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High-resolution magnetostriction measurements of the Pauli-limited superconductor Sr2RuO4
Authors:
Shunichiro Kittaka,
Yohei Kono,
Toshiro Sakakibara,
Naoki Kikugawa,
Shinya Uji,
Dmitry A. Sokolov,
Kazushige Machida
Abstract:
We performed high-resolution magnetostriction measurements on the Pauli-limited superconductor Sr$_2$RuO$_4$ using high-quality single crystals. A first-order superconducting transition, accompanied by pronounced hysteresis, was observed under in-plane magnetic fields, where the relative length change of the sample, $ΔL/L$, was on the order of $10^{-8}$. To ensure the reliability of the measuremen…
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We performed high-resolution magnetostriction measurements on the Pauli-limited superconductor Sr$_2$RuO$_4$ using high-quality single crystals. A first-order superconducting transition, accompanied by pronounced hysteresis, was observed under in-plane magnetic fields, where the relative length change of the sample, $ΔL/L$, was on the order of $10^{-8}$. To ensure the reliability of the measurements, particular attention was paid to minimizing the influence of magnetic torque, which can significantly affect data under in-plane field configurations, via field-angle-resolved magnetostriction. Within the hysteresis regime, slightly below the Pauli-limited upper critical field, a hump-like anomaly in the magnetostriction coefficient was identified. Furthermore, a characteristic double-peak structure in the field-angle derivative of the magnetostriction provides additional support for this anomaly. Although these findings may reflect a lattice response associated with the emergence of the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase in Sr$_2$RuO$_4$, the possibility of a broadened first-order transition cannot be excluded. Notably, this magnetostriction anomaly qualitatively deviates from the FFLO phase boundary suggested by previous NMR measurements, highlighting the necessity for further experimental and theoretical investigations to elucidate the nature of the FFLO state in this material.
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Submitted 14 November, 2025; v1 submitted 10 November, 2025;
originally announced November 2025.
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From Continuous to First-Order-Like: Amorphous-to-Amorphous Transition in Phase-Change Materials
Authors:
Tomoki Fujita,
Yoshio Kono,
Yuhan Chen,
Jens Moesgaard,
Seiya Takahashi,
Arune Makareviciute,
Sho Kakizawa,
Davide Campi,
Marco Bernasconi,
Koji Ohara,
Ichiro Inoue,
Yujiro Hayashi,
Makina Yabashi,
Eiji Nishibori,
Riccardo Mazzarello,
Shuai Wei
Abstract:
Polymorphism is ubiquitous in crystalline solids. Amorphous solids, such as glassy water and silicon, may undergo amorphous-to-amorphous transitions (AATs). The nature of AATs remains ambiguous, due to diverse system-dependent behaviors and experimental challenges to characterize disordered structures. Here, we identify two ordered motifs in amorphous phase-change materials and monitor their inter…
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Polymorphism is ubiquitous in crystalline solids. Amorphous solids, such as glassy water and silicon, may undergo amorphous-to-amorphous transitions (AATs). The nature of AATs remains ambiguous, due to diverse system-dependent behaviors and experimental challenges to characterize disordered structures. Here, we identify two ordered motifs in amorphous phase-change materials and monitor their interplay upon pressure-induced AATs. Tuning temperature, we find a crossover from continuous to first-order-like AATs. The crossover emerges at a special pressure-temperature combination, where the AAT encounters a maximum in crystallization rate. Analyzing the two ordered motifs in a two-state model, we draw a phenomenological parallel to the phase transition behavior of supercooled water near its second critical point. This analogy raises an intriguing question regarding the existence of a critical-like point within amorphous solids.
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Submitted 9 April, 2025;
originally announced April 2025.
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Multiple magnetic orders discovered in the superconducting state of EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$
Authors:
Nan Zhou,
Yue Sun,
Ivan S. Veshchunov,
S. Kittaka,
X. L. Shen,
H. M. Ma,
W. Wei,
Y. Q. Pan,
M. Cheng,
Y. F. Zhang,
Y. Kono,
Yuping Sun,
T. Tamegai,
Xuan Luo,
Zhixiang Shi,
Toshiro Sakakibara
Abstract:
The interplay between superconductivity and magnetism is an important subject in condensed matter physics. EuFe$_{2}$As$_{2}$-based iron pnictides could offer an interesting plateau to study their relationship that has attracted considerable attention. So far, two magnetic phase transitions were observed in EuFe$_{2}$As$_{2}$-based crystal, which were deemed to originate from the itinerant Fe mome…
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The interplay between superconductivity and magnetism is an important subject in condensed matter physics. EuFe$_{2}$As$_{2}$-based iron pnictides could offer an interesting plateau to study their relationship that has attracted considerable attention. So far, two magnetic phase transitions were observed in EuFe$_{2}$As$_{2}$-based crystal, which were deemed to originate from the itinerant Fe moments ($\sim$ 190 K) and the localized Eu$^{2+}$ moments ($\sim$ 19 K), respectively. Here, we systematically studied the heat capacity for the EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ crystals with \textit{x} = 0.21 (optimally doped) and \textit{x} = 0.29 (overdoped). We have found two new magnetic orders in the superconducting state (ranging from 0.4 to 1.2 K) in the optimally doped crystal. As more P was introduced into the As site, one of the magnetic orders becomes absent in the overdoped crystal. Additionally, we observed strong field and orientation dependence in heat capacity. The present findings in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ have detected the new low-temperature magnetic orders, which may originate from the localized Eu$^{2+}$ spins order or the spin reorientation.
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Submitted 6 December, 2024;
originally announced December 2024.
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Rotational Grüneisen ratio: a probe for quantum criticality in anisotropic systems
Authors:
Shohei Yuasa,
Yohei Kono,
Yuta Ozaki,
Minoru Yamashita,
Yasuyuki Shimura,
Toshiro Takabatake,
Shunichiro Kittaka
Abstract:
The Grüneisen ratio $Γ$ and its magnetic analog, the magnetic Grüneisen ratio $Γ_H$, are powerful probes to study the nature of quantum phase transitions. Here, we propose a Grüneisen parameter, the rotational Grüneisen ratio $Γ_φ$, by introducing the orientation of the external field as a control parameter. We investigate $Γ_φ$ of the highly anisotropic paramagnets CeRhSn and CeIrSn by measuring…
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The Grüneisen ratio $Γ$ and its magnetic analog, the magnetic Grüneisen ratio $Γ_H$, are powerful probes to study the nature of quantum phase transitions. Here, we propose a Grüneisen parameter, the rotational Grüneisen ratio $Γ_φ$, by introducing the orientation of the external field as a control parameter. We investigate $Γ_φ$ of the highly anisotropic paramagnets CeRhSn and CeIrSn by measuring the rotational magnetocaloric effect in a wide range of temperatures and magnetic fields. We find that the $Γ_φ$ data of both compounds are scaled by using the same critical exponents and the field-invariant critical field angle. Remarkably, the scaling function for the $Γ_φ$ data reveals the presence of highly anisotropic quantum criticality that develops as a function of the easy-axis component of the magnetic field from the quantum critical line. This paper provides a thermodynamic approach to detect and identify magnetic quantum criticality in highly anisotropic systems.
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Submitted 10 January, 2025; v1 submitted 12 December, 2024;
originally announced December 2024.
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Modulation vector of the Fulde-Ferrell-Larkin-Ovchinnikov state in CeCoIn5 revealed by high-resolution magnetostriction measurements
Authors:
Shunichiro Kittaka,
Yohei Kono,
Kaito Tsunashima,
Daisuke Kimoto,
Makoto Yokoyama,
Yusei Shimizu,
Toshiro Sakakibara,
Minoru Yamashita,
Kazushige Machida
Abstract:
The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state is an exotic superconducting phase formed by Cooper pairs with finite center-of-mass momentum $q$. On theoretical grounds, the superconducting order parameter in the FFLO state is spatially modulated along the $q$ vector, and the emergence of an associated anisotropy is expected at the phase transition from the Abrikosov state to the FFLO state. He…
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The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state is an exotic superconducting phase formed by Cooper pairs with finite center-of-mass momentum $q$. On theoretical grounds, the superconducting order parameter in the FFLO state is spatially modulated along the $q$ vector, and the emergence of an associated anisotropy is expected at the phase transition from the Abrikosov state to the FFLO state. Here, we report the results of high-resolution magnetostriction measurements for a single crystal of CeCoIn$_5$ around $B \parallel c$. We find two anomalies in the magnetostriction along the $c$ axis, parallel to the magnetic-field orientation. In sharp contrast, this $B_{\rm K}$ anomaly disappears in the magnetostriction along the $a$-axis direction, perpendicular to the magnetic-field orientation. To explain this uniaxial expansion, we suggest a possibility that the FFLO transition occurs slightly below the upper critical field, and the FFLO modulation vector parallel to the applied magnetic field gives rise to the anisotropic response.
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Submitted 30 June, 2023; v1 submitted 21 June, 2023;
originally announced June 2023.
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Magnetic structures of electron systems on the extended spatially completely anisotropic triangular lattice near quantum critical points
Authors:
Yuki Kono,
Hiroshi Shimahara
Abstract:
We examine magnetic structures of electron systems on an extended triangular lattice that consists of two types of bond triangles with electron transfer energies t_l and t'_l (l = 1, 2, and 3), respectively. We examine the ground state in the mean-field theory when t_1 = t'_1, focusing on collinear states with two sublattices. It is shown that when the imbalance of the spatial anisotropies of the…
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We examine magnetic structures of electron systems on an extended triangular lattice that consists of two types of bond triangles with electron transfer energies t_l and t'_l (l = 1, 2, and 3), respectively. We examine the ground state in the mean-field theory when t_1 = t'_1, focusing on collinear states with two sublattices. It is shown that when the imbalance of the spatial anisotropies of the two triangles is large, up-up-down-down (uudd) phases are stable, and the most likely ground states of the lambda-(BETS)_2FeCl_4 system are the Neel state with the modulation vector (π/c,π/a) and a uudd state, where c = a_1 = a'_1 and a = (a_2+a'_2)/2, with a_1, a_1', a_2, and a_2' being the lattice constants of the bonds with t_1, t'_1, t_2, and t'_2, respectively. These results are consistent with those from the classical spin system. In addition, this study reveals behaviors near the quantum critical point, which cannot be reproduced in the localized spin model. As the imbalance of the spatial anisotropies increases, the U_c of the Neel state increases, and that of the uudd state decreases. In the phase diagrams containing areas of the paramagnetic state, the Neel state with (π/c,π/a), and a uudd state, their boundaries terminate at a triple point, near which all the transitions are of the first order. The phase boundary between the antiferromagnetic phases does not depend on U, and the transition is of the first order everywhere on the boundary. By contrast, the transitions from the two antiferromagnetic phases to the paramagnetic phase are of the second order, unless the system is close to the triple point.
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Submitted 4 November, 2021;
originally announced November 2021.
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Gapped ground state in a spin-1/2 frustrated square lattice
Authors:
H. Yamaguchi,
N. Uemoto,
T. Okubo,
Y. Kono,
S. Kittaka,
T. Sakakibara,
T. Yajima,
S. Shimono,
Y. Iwasaki,
Y. Hosokoshi
Abstract:
We present a model compound with a spin-1/2 frustrated square lattice, in which three ferromagnetic (F) interactions and one antiferromagnetic (AF) compet. Considering the effective spin-1 formed by the dominant F dimer, this square lattice can be mapped to a spin-1 spatially anisotropic triangular lattice. The magnetization curve exhibits gapped behavior indicative of a dominant one-dimensional (…
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We present a model compound with a spin-1/2 frustrated square lattice, in which three ferromagnetic (F) interactions and one antiferromagnetic (AF) compet. Considering the effective spin-1 formed by the dominant F dimer, this square lattice can be mapped to a spin-1 spatially anisotropic triangular lattice. The magnetization curve exhibits gapped behavior indicative of a dominant one-dimensional (1D) AF correlation. In the field-induced gapless phase, the specific heat and magnetic susceptibility show a phase transition to an ordered state with 2D characteristics. These results indicate that the spin-1 Haldane state is extended to the 2D system. We demonstrate that the gapped ground state observed in the present spin-1/2 frustrated square lattice originates from the one-dimensionalization caused by frustration.
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Submitted 29 August, 2021;
originally announced August 2021.
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Quantum critical phenomena in a spin-1/2 frustrated square lattice with spatial anisotropy
Authors:
H. Yamaguchi,
Y. Iwasaki,
Y. Kono,
T. Okubo,
S. Miyamoto,
Y. Hosokoshi,
A. Matsuo,
T. Sakakibara,
T. Kida,
M. Hagiwara
Abstract:
We present a model compound with a spin-1/2 spatially anisotropic frustrated square lattice, in which three antiferromagnetic interactions and one ferromagnetic interaction are competing. We observe an unconventional gradual increase in the low-temperature magnetization curve reminiscent of the quantum critical behavior between gapped and gapless phases. In addition, the specific heat and electron…
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We present a model compound with a spin-1/2 spatially anisotropic frustrated square lattice, in which three antiferromagnetic interactions and one ferromagnetic interaction are competing. We observe an unconventional gradual increase in the low-temperature magnetization curve reminiscent of the quantum critical behavior between gapped and gapless phases. In addition, the specific heat and electron spin resonance signals indicate one-dimensional characteristics. These results demonstrate quantum critical behavior associated with one dimensionalization caused by frustrated interactions in the spin-1/2 spatially anisotropic square lattice.
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Submitted 22 June, 2021;
originally announced June 2021.
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Experimental realization of Lieb-Mattis plateau in a quantum spin chain
Authors:
H. Yamaguchi,
T. Okita,
Y. Iwasaki,
Y. Kono,
N. Uemoto,
Y. Hosokoshi,
T. Kida,
T. Kawakami,
A. Matsuo,
M. Hagiwara
Abstract:
We present a mixed spin-(1/2, 5/2) chain composed of a charge-transfer salt (4-Br-$o$-MePy-V)FeCl$_4$. We observe the entire magnetization curve up to saturation, which exhibits a clear Lieb-Mattis magnetization plateau and subsequent quantum phase transition towards the gapless Luttinger-liquid phase. The observed magnetic behavior is quantitatively explained by a mixed spin-(1/2, 5/2) chain mode…
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We present a mixed spin-(1/2, 5/2) chain composed of a charge-transfer salt (4-Br-$o$-MePy-V)FeCl$_4$. We observe the entire magnetization curve up to saturation, which exhibits a clear Lieb-Mattis magnetization plateau and subsequent quantum phase transition towards the gapless Luttinger-liquid phase. The observed magnetic behavior is quantitatively explained by a mixed spin-(1/2, 5/2) chain model. The present results demonstrate a quantum many-body effect based on quantum topology and provide a new stage in the search for topological properties in condensed matter physics.
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Submitted 22 April, 2020;
originally announced April 2020.
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Superconductivity in PtSbS with a Noncentrosymmetric Cubic Crystal Structure
Authors:
Ryosuke Mizutani,
Yoshihiko Okamoto,
Hayate Nagaso,
Youichi Yamakawa,
Hiroshi Takatsu,
Hiroshi Kageyama,
Shunichiro Kittaka,
Yohei Kono,
Toshiro Sakakibara,
Koshi Takenaka
Abstract:
We report the synthesis, electronic properties, and electronic structure of ullmannite-type PtSbS, which has a cubic crystal structure without space inversion symmetry. Electrical resistivity and magnetization measured at low temperatures suggested that this compound is a bulk superconductor with a superconducting transition temperature of Tc = 0.15 K. First principles calculations indicated that…
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We report the synthesis, electronic properties, and electronic structure of ullmannite-type PtSbS, which has a cubic crystal structure without space inversion symmetry. Electrical resistivity and magnetization measured at low temperatures suggested that this compound is a bulk superconductor with a superconducting transition temperature of Tc = 0.15 K. First principles calculations indicated that Fermi surfaces of PtSbS include strongly nested hole pockets, which can make this compound interesting if they contribute to the emergence of superconductivity.
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Submitted 29 August, 2019;
originally announced August 2019.
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Emergent critical phenomenon in spin-1/2 ferromagnetic-leg ladders: Quasi-one-dimensional Bose--Einstein condensate
Authors:
Y. Kono,
S. Kittaka,
H. Yamaguchi,
Y. Hosokoshi,
T. Sakakibara
Abstract:
We examine the magnetic-field-induced criticality of phase boundary near saturation field $H_{\mathrm{c}}$ in the spin-1/2 ferromagnetic (FM)-leg ladder 3-Cl-4-F-V [=3-(3-chloro-4-fluorophenyl)-1,5-diphenylverdazyl], the predominant interactions of which arise from FM chains (strong-leg type). Critical temperatures were precisely determined through dc magnetization, specific heat, and magnetocalor…
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We examine the magnetic-field-induced criticality of phase boundary near saturation field $H_{\mathrm{c}}$ in the spin-1/2 ferromagnetic (FM)-leg ladder 3-Cl-4-F-V [=3-(3-chloro-4-fluorophenyl)-1,5-diphenylverdazyl], the predominant interactions of which arise from FM chains (strong-leg type). Critical temperatures were precisely determined through dc magnetization, specific heat, and magnetocaloric effect measurements. The criticality of 3-Cl-4-F-V is characterized by a linear phase boundary with respect to $H_{\mathrm{c}}-H$ near $H\,=\,H_{\mathrm{c}}$. This behavior is similar to that of another strong-leg-type FM-leg ladder. The universal critical behavior in these strong-leg-type FM-leg ladders is expected to demonstrate the theoretically predicted quasi-one-dimensional Bose--Einstein condensation.
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Submitted 23 August, 2019;
originally announced August 2019.
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Field-angle-resolved landscape of non-Fermi-liquid behavior in the quasi-kagome Kondo Lattice CeRhSn
Authors:
Shunichiro Kittaka,
Yohei Kono,
Suguru Tsuda,
Toshiro Takabatake,
Toshiro Sakakibara
Abstract:
We have employed a magnetic field angle as a tuning parameter in a comprehensive measurement of the specific heat, magnetocaloric effect, and magnetization for the quasi-kagome Kondo lattice CeRhSn, which is considered to exhibit zero-field quantum criticality driven by geometrical frustration. By constructing the field-angle-resolved landscape of the entropy, we unexpectedly revealed that the non…
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We have employed a magnetic field angle as a tuning parameter in a comprehensive measurement of the specific heat, magnetocaloric effect, and magnetization for the quasi-kagome Kondo lattice CeRhSn, which is considered to exhibit zero-field quantum criticality driven by geometrical frustration. By constructing the field-angle-resolved landscape of the entropy, we unexpectedly revealed that the non-Fermi-liquid nature survives up to a metamagnetic crossover field of roughly 3 T in the very narrow field-orientation range, close to the direction parallel to the quasi-kagome plane. We propose that spin fluctuations along the hexagonal $c$ axis are the dominant driving force for the non-Fermi-liquid behavior because it is strongly suppressed by a magnetic-field component along the $c$ axis. The multidimensional entropy landscape, which directly reflects the degeneracy of ground states, opens a new route for uncovering the nature of exotic phases in anisotropic systems.
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Submitted 10 May, 2021; v1 submitted 18 April, 2019;
originally announced April 2019.
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Quantum critical behaviour and Lifshitz transition in intermediate valence $α$-YbAlB$_4$
Authors:
Mihael S. Grbić,
Eoin C. T. O'Farrell,
Yosuke Matsumoto,
Kentaro Kuga,
Manuel Brando,
Robert Küchler,
Andriy H. Nevidomskyy,
Makoto Yoshida,
Toshiro Sakakibara,
Yohei Kono,
Yasuyuki Shimura,
Michael L. Sutherland,
Masashi Takigawa,
Satoru Nakatsuji
Abstract:
Intermetallic compounds containing $f$-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic $f$-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass ($m^{*}$) and a corresponding decrease of…
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Intermetallic compounds containing $f$-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic $f$-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass ($m^{*}$) and a corresponding decrease of the Fermi temperature. However, the presence of $f$-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with quasiparticles of moderate $m^{*}$. Such systems are typically isotropic, with a characteristic energy scale $T_0$ of the order of hundreds of kelvins that require large magnetic fields or pressures to promote a valence or magnetic instability. Here we show that the intermediate valence compound $α$-YbAlB$_4$ surprisingly exhibits both quantum critical behaviour and a Lifshitz transition under low magnetic field, which is attributed to the anisotropy of the hybridization between the conduction and localized $f$-electrons. These findings suggest a new route to bypass the large valence energy scale in developing the QC.
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Submitted 24 March, 2019;
originally announced March 2019.
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$S$ =1/2 ferromagnetic Heisenberg chain in a verdazyl-based complex
Authors:
N. Uemoto,
Y. Kono,
S. Kittaka,
T. Sakakibara,
T. Yajima,
Y. Iwasaki,
S. Miyamoto,
Y. Hosokoshi,
H. Yamaguchi
Abstract:
We present a model compound for the $S$=1/2 ferromagnetic Heisenberg chain composed of the verdazyl-based complex $[$Zn(hfac)$_2]$$[$4-Cl-$o$-Py-V-(4-F)$_2]$. $Ab$ $initio$ MO calculations indicate a predominant ferromagnetic interaction forming an $S$=1/2 ferromagnetic chain. The magnetic susceptibility and specific heat indicate a phase transition to an AF order owing to the finite interchain co…
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We present a model compound for the $S$=1/2 ferromagnetic Heisenberg chain composed of the verdazyl-based complex $[$Zn(hfac)$_2]$$[$4-Cl-$o$-Py-V-(4-F)$_2]$. $Ab$ $initio$ MO calculations indicate a predominant ferromagnetic interaction forming an $S$=1/2 ferromagnetic chain. The magnetic susceptibility and specific heat indicate a phase transition to an AF order owing to the finite interchain couplings. We explain the magnetic susceptibility and magnetization curve above the phase transition temperature based on the $S$=1/2 ferromagnetic Heisenberg chain. The magnetization curve in the ordered phase is described by a conventional AF two-sublattice model. Furthermore, the obtained magnetic specific heat reproduces the almost temperature-independent behavior of the $S$=1/2 ferromagnetic Heisenberg chain. In the low-temperature region, the magnetic specific heat exhibits $\sqrt{T}$ dependence, which is attributed to the energy dispersion in the ferromagnetic chain.
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Submitted 16 March, 2019;
originally announced March 2019.
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Anisotropic magnetic-field response of quantum critical fluctuations in Ni-doped CeCoIn5
Authors:
M. Yokoyama,
K. Suzuki,
K. Tenya,
S. Nakamura,
Y. Kono,
S. Kittaka,
T. Sakakibara
Abstract:
This paper demonstrates the anisotropic response of quantum critical fluctuations with respect to the direction of the magnetic field $B$ in Ni-doped CeCoIn$_5$ by measuring the magnetization $M$ and specific heat $C$. The results show that $M/B$ at $B=0.1\ {\rm T}$ for both the tetragonal $c$ and $a$ directions exhibits $T^{-η}$ dependencies, and that $C/T$ at $B=0$ follows a $-\ln T$ function, w…
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This paper demonstrates the anisotropic response of quantum critical fluctuations with respect to the direction of the magnetic field $B$ in Ni-doped CeCoIn$_5$ by measuring the magnetization $M$ and specific heat $C$. The results show that $M/B$ at $B=0.1\ {\rm T}$ for both the tetragonal $c$ and $a$ directions exhibits $T^{-η}$ dependencies, and that $C/T$ at $B=0$ follows a $-\ln T$ function, which are the characteristics of non-Fermi-liquid (NFL) behaviors. For $B\,||\,c$, both the $M/B\propto T^{-η}$ and $C/T \propto -\ln T$ dependencies change into nearly temperature-constant behaviors by increasing $B$, indicating a crossover from the NFL state to the Fermi-liquid state. For $B\,||\,a$, however, the NFL behavior in $C/T$ persists up to $B=7\ {\rm T}$, whereas $M/B$ exhibits temperature-independent behavior for $B\ge 1\ {\rm T}$. These contrasting characteristics in $M/B$ and $C/T$ reflect the anisotropic nature of quantum critical fluctuations; the $c$-axis spin component significantly contributes to the quantum critical fluctuations. We compare this anisotropic behavior of the spin fluctuations to superconducting properties in pure CeCoIn$_5$, especially to the anisotropy in the upper critical field and the Ising-like characteristics in the spin resonance excitation, and suggest a close relationship between them.
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Submitted 12 February, 2019;
originally announced February 2019.
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Field-induced quantum magnetism in the verdazyl-based charge-transfer salt $[$$o$-MePy-V-($p$-Br)$_2]$FeCl$_4$
Authors:
Y. Iwasaki,
T. Kida,
M. Hagiwara,
T. Kawakami,
Y. Kono,
S. Kittaka,
T. Sakakibara,
Y. Hosokoshi,
H. Yamaguchi
Abstract:
We successfully synthesized a verdazyl-based charge-transfer salt $[$$o$-MePy-V-($p$-Br)$_2]$FeCl$_4$, which has an $S_{\rm{V}}$=1/2 on the radical $o$-MePy-V-($p$-Br)$_2$ and an $S_{\rm{Fe}}$=5/2 on the FeCl$_4$ anion. $Ab$ $initio$ molecular orbital calculations indicate the formation of an $S_{\rm{V}}$=1/2 honeycomb lattice composed of three types of exchange interaction with two types of inequ…
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We successfully synthesized a verdazyl-based charge-transfer salt $[$$o$-MePy-V-($p$-Br)$_2]$FeCl$_4$, which has an $S_{\rm{V}}$=1/2 on the radical $o$-MePy-V-($p$-Br)$_2$ and an $S_{\rm{Fe}}$=5/2 on the FeCl$_4$ anion. $Ab$ $initio$ molecular orbital calculations indicate the formation of an $S_{\rm{V}}$=1/2 honeycomb lattice composed of three types of exchange interaction with two types of inequivalent site. Further, the $S_{\rm{V}}$=1/2 at one site is sandwiched by $S_{\rm{Fe}}$=5/2 spins through antiferromagnetic (AF) interactions. The magnetic properties indicate that the dominant AF interactions between the $S_{\rm{V}}$ = 1/2 spins form a gapped singlet state, and the remaining $S_{\rm{Fe}}$ = 5/2 spins cause an AF order. The magnetization curve exhibits a linear increase up to approximately 7 T, and an unconventional 5/6 magnetization plateau appears between 7 T and 40 T. We discuss the differences between the effective interactions associated with the magnetic properties of the present compound and ($o$-MePy-V)FeCl$_4$. We explain the low-field linear magnetization curve through a mean-field approximation of an $S_{\rm{Fe}}$ = 5/2 spin model. At higher field regions, the 5/6 magnetization plateau and subsequent nonlinear increase are reproduced by the $S_{\rm{V}}$ = 1/2 AF dimer, in which a particular internal field is applied to one of the spin sites. The ESR resonance signals in the low-temperature and low-field regime are explained by conventional two-sublattice AF resonance modes with easy-axis anisotropy. These results demonstrate that exchange interactions between $S_{\rm{V}}$ = 1/2 and $S_{\rm{Fe}}$ = 5/2 spins in $[$$o$-MePy-V-($p$-Br)$_2]$FeCl$_4$ realize unconventional magnetic properties with low-field classical behavior and field-induced quantum behavior.
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Submitted 19 December, 2018;
originally announced December 2018.
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Field-enhanced quantum fuctuation in S=1/2 frustrated square lattice
Authors:
H. Yamaguchi,
Y. Sasaki,
T. Okubo,
M. Yoshida,
T. Kida,
M. Hagiwara,
Y. Kono,
S. Kittaka,
T. Sakakibara,
M. Takigawa,
Y. Iwasaki,
Y. Hosokoshi
Abstract:
We present a new model compound with the S = 1/2 frustrated square lattice composed of the charge-transfer salt (o-MePy-V)PF6. Ab initio calculations indicate the formation of an S = 1/2 square lattice, in which six types of nearest-neighbor ferromagnetic- and antiferromagnetic interactions cause frustration. By applying a magnetic field, we observe an unusually gradual increase of magnetization a…
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We present a new model compound with the S = 1/2 frustrated square lattice composed of the charge-transfer salt (o-MePy-V)PF6. Ab initio calculations indicate the formation of an S = 1/2 square lattice, in which six types of nearest-neighbor ferromagnetic- and antiferromagnetic interactions cause frustration. By applying a magnetic field, we observe an unusually gradual increase of magnetization and a subsequent 1/2-plateau-like behavior. A numerical analysis using the tensor network method qualitatively demonstrates such behaviors and suggests a collinear ordered state and a field-enhanced quantum fluctuation. Furthermore, the local magnetization and T1^-1 probed by nuclear magnetic resonance measurements support these findings.
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Submitted 21 August, 2018;
originally announced August 2018.
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Quasi-one-dimensional Bose-Einstein Condensation in the Spin-1/2 Ferromagnetic-leg Ladder 3-I-V
Authors:
Y. Kono,
S. Kittaka,
H. Yamaguchi,
Y. Hosokoshi,
T. Sakakibara
Abstract:
Quantum criticality of the spin-1/2 ferromagnetic-leg ladder 3-I-V [=3-(3-iodophenyl)-1,5-diphenylverdazyl] has been examined with respect to the antiferromagnetic to paramagnetic phase transition near the saturation field $H_{c}$. The phase boundary $T_{c}(H)$ follows the power-law $T_{c}(H)\propto H_{c}-H$ for a wide temperature range. This characteristic behavior is discussed as a quasi-one-dim…
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Quantum criticality of the spin-1/2 ferromagnetic-leg ladder 3-I-V [=3-(3-iodophenyl)-1,5-diphenylverdazyl] has been examined with respect to the antiferromagnetic to paramagnetic phase transition near the saturation field $H_{c}$. The phase boundary $T_{c}(H)$ follows the power-law $T_{c}(H)\propto H_{c}-H$ for a wide temperature range. This characteristic behavior is discussed as a quasi-one-dimensional (quasi-1D) Bose-Einstein condensation, which is predicted theoretically for weakly coupled quasi-1D ferromagnets. Thus, 3-I-V provides the first promising candidate for this attractive prediction.
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Submitted 27 March, 2018;
originally announced March 2018.
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Three-dimensional Bose-Einstein Condensation in the Spin-1/2 Ferromagnetic-leg Ladder 3-Br-4-F-V
Authors:
Y. Kono,
H. Yamaguchi,
Y. Hosokoshi,
T. Sakakibara
Abstract:
The critical exponent of the phase boundary has been examined on the three-dimensional incommensurate ordering phase in the spin-1/2 ferromagnetic-leg ladder 3-Br-4-F-V [=3-(3-bromo-4-fluorophenyl)-1,5-diphenylverdazyl]. Using the temperature-window fitting technique, we obtained the critical exponents which agreed with the three-dimensional (3D) Bose-Einstein condensation (BEC) universality class…
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The critical exponent of the phase boundary has been examined on the three-dimensional incommensurate ordering phase in the spin-1/2 ferromagnetic-leg ladder 3-Br-4-F-V [=3-(3-bromo-4-fluorophenyl)-1,5-diphenylverdazyl]. Using the temperature-window fitting technique, we obtained the critical exponents which agreed with the three-dimensional (3D) Bose-Einstein condensation (BEC) universality class at both sides of the lower critical field and the saturation field. 3-Br-4-F-V thus becomes a new member of the quantum magnets which prove the universality of the 3D BEC exponent.
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Submitted 26 September, 2017;
originally announced September 2017.
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Randomness-induced quantum spin liquid on honeycomb lattice
Authors:
H. Yamaguchi,
M. Okada,
Y. Kono,
S. Kittaka,
T. Sakakibara,
T. Okabe,
Y. Iwasaki,
Y. Hosokoshi
Abstract:
We present a quantu spin liquid state in a spin-1/2 honeycomb lattice with randomness in the exchange interaction. That is, we successfully introduce randomness into the organic radial-based complex and realize a random-singlet (RS) state. All magnetic and thermodynamic experimental results indicate the liquid-like behaviors, which are consistent with those expected in the RS state. These results…
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We present a quantu spin liquid state in a spin-1/2 honeycomb lattice with randomness in the exchange interaction. That is, we successfully introduce randomness into the organic radial-based complex and realize a random-singlet (RS) state. All magnetic and thermodynamic experimental results indicate the liquid-like behaviors, which are consistent with those expected in the RS state. These results demonstrate that the randomness or inhomogeneity in the actual systems stabilize the RS state and yield liquid-like behavior.
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Submitted 24 September, 2017;
originally announced September 2017.
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Wing structure in the phase diagram of the Ising Ferromagnet URhGe close to its tricritical point investigated by angle-resolved magnetization measurements
Authors:
Shota Nakamura,
Toshiro Sakakibara,
Yusei Shimizu,
Shunichiro Kittaka,
Yohei Kono,
Yoshinori Haga,
Jiří Pospíšil,
Etsuji Yamamoto
Abstract:
High-precision angle-resolved dc magnetization and magnetic torque studies were performed on a single-crystalline sample of URhGe, an orthorhombic Ising ferromagnet with the $c$ axis being the magnetization easy axis, in order to investigate the phase diagram around the ferromagnetic (FM) reorientation transition in a magnetic field near the $b$ axis. We have clearly detected first-order transitio…
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High-precision angle-resolved dc magnetization and magnetic torque studies were performed on a single-crystalline sample of URhGe, an orthorhombic Ising ferromagnet with the $c$ axis being the magnetization easy axis, in order to investigate the phase diagram around the ferromagnetic (FM) reorientation transition in a magnetic field near the $b$ axis. We have clearly detected first-order transition in both the magnetization and the magnetic torque at low temperatures, and determined detailed profiles of the wing structure of the three-dimensional $T$-$H_{b}$-$H_{c}$ phase diagram, where $H_{c}$ and $H_{b}$ denotes the field components along the $c$ and the $b$ axes, respectively. The quantum wing critical points are located at $μ_0H_c\sim\pm$1.1 T and $μ_0H_b\sim$13.5 T. Two second-order transition lines at the boundaries of the wing planes rapidly tend to approach with each other with increasing temperature up to $\sim 3$ K. Just at the zero conjugate field ($H_c=0$), however, a signature of the first-order transition can still be seen in the field derivative of the magnetization at $\sim 4$ K, indicating that the tricritical point exists in a rather high temperature region above 4 K. This feature of the wing plane structure is consistent with the theoretical expectation that three second-order transition lines merge tangentially at the triciritical point.
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Submitted 31 August, 2017;
originally announced September 2017.
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Thermodynamic Investigation of Metamagnetic Transitions and Partial Disorder in the Quasi-Kagome Kondo Lattice CePdAl
Authors:
Kenji Mochidzuki,
Yusei Shimizu,
Akihiro Kondo,
Shota Nakamura,
Shunichiro Kittaka,
Yohei Kono,
Toshiro Sakakibara,
Yoichi Ikeda,
Yosikazu Isikawa,
Koichi Kindo
Abstract:
Low-temperature ($T$) thermodynamic properties in magnetic fields ($B$) of the quasi-Kagome antiferromagnet CePdAl ($T_{\rm N}\sim$ 2.7 K) were studied by means of magnetization and specific-heat $C(T,B)$ measurements. The unusual magnetic phase diagram, including three thermodynamic phases I-III, and crossover anomalies, has been obtained. In low-field phase I, the existence of the partial Kondo…
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Low-temperature ($T$) thermodynamic properties in magnetic fields ($B$) of the quasi-Kagome antiferromagnet CePdAl ($T_{\rm N}\sim$ 2.7 K) were studied by means of magnetization and specific-heat $C(T,B)$ measurements. The unusual magnetic phase diagram, including three thermodynamic phases I-III, and crossover anomalies, has been obtained. In low-field phase I, the existence of the partial Kondo screening state on the one-third Ce sites is supported from the thermodynamic point of view: (i) an appearance of the paramagnetic moment with one-third of the full moment around 3 T, and (ii) an occurrence of the entropy release $\sim$0.3$R$ln2 around the observed crossover. On the other hand, a strong enhancement of $C/T$ is found around the point, where $T_{\rm N}(B)$ meets the boundary of phase III, indicating the possible presence of a tri-critical point. Furthermore, it is suggested that the three metamagnetic transitions at $B_{{\rm m}i}$ ($i=$1,2,3) come from successive increments of the Ising-type magnetic moment along the $c$-axis. In high-field state above 20 T, the behavior of $f$ electron can be rather described by the crystal-electric-field model.
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Submitted 23 November, 2016;
originally announced November 2016.
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Low-Energy Excitations and Ground State Selection in Quantum Breathing Pyrochlore Antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$
Authors:
T. Haku,
K. Kimura,
Y. Matsumoto,
M. Soda,
M. Sera,
D. Yu,
R. A. Mole,
T. Takeuchi,
S. Nakatsuji,
Y. Kono,
T. Sakakibara,
L. -J. Chang,
T. Masuda
Abstract:
We study low energy excitations in the quantum breathing pyrochlore antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$ by combination of inelastic neutron scattering (INS) and thermodynamical properties measurements. The INS spectra are quantitatively explained by spin-1/2 single-tetrahedron model having $XXZ$ anisotropy and Dzyaloshinskii-Moriya interaction. This model has a two-fold degeneracy of the lo…
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We study low energy excitations in the quantum breathing pyrochlore antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$ by combination of inelastic neutron scattering (INS) and thermodynamical properties measurements. The INS spectra are quantitatively explained by spin-1/2 single-tetrahedron model having $XXZ$ anisotropy and Dzyaloshinskii-Moriya interaction. This model has a two-fold degeneracy of the lowest-energy state per tetrahedron and well reproduces the magnetization curve at 0.5 K and heat capacity above 1.5 K. At lower temperatures, however, we observe a broad maximum in the heat capacity around 63 mK, demonstrating that a unique quantum ground state is selected due to extra perturbations with energy scale smaller than the instrumental resolution of INS.
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Submitted 27 May, 2016;
originally announced May 2016.
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Pauli-limited superconductivity and antiferromagnetism in the heavy-fermion compound CeCo(In1-xZnx)5
Authors:
M. Yokoyama,
H. Mashiko,
R. Otaka,
Y. Sakon,
K. Fujimura,
K. Tenya,
A. Kondo,
K. Kindo,
Y. Ikeda,
H. Yoshizawa,
Y. Shimizu,
Y. Kono,
T. Sakakibara
Abstract:
We report on the anisotropic properties of Pauli-limited superconductivity (SC) and antiferromagnetism (AFM) in the solid solutions CeCo(In_{1-x}Zn_x)_5 (x<=0.07). In CeCo(In_{1-x}Zn_x)_5, the SC transition temperature T_c is continuously reduced from 2.3 K (x=0) to ~1.4 K (x=0.07) by doping Zn, and then the AFM order with the transition temperature of T_N~2.2 K develops for x larger than ~0.05. T…
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We report on the anisotropic properties of Pauli-limited superconductivity (SC) and antiferromagnetism (AFM) in the solid solutions CeCo(In_{1-x}Zn_x)_5 (x<=0.07). In CeCo(In_{1-x}Zn_x)_5, the SC transition temperature T_c is continuously reduced from 2.3 K (x=0) to ~1.4 K (x=0.07) by doping Zn, and then the AFM order with the transition temperature of T_N~2.2 K develops for x larger than ~0.05. The present thermal, transport and magnetic measurements under magnetic field B reveal that the substitution of Zn for In yields little change of low-temperature upper critical field μ_0H_{c2} for both the tetragonal a and c axes, while it monotonically reduces the SC transition temperature T_c. In particular, the magnitudes of μ_0H_{c2} at the nominal Zn concentration of x = 0.05 (measured Zn amount of ~0.019) are 11.8 T for B||a and 4.8 T for B||c, which are as large as those of pure compound though T_c is reduced to 80% of that for x=0. We consider that this feature originates from a combination of both an enhanced AFM correlation and a reduced SC condensation energy in these alloys. It is also clarified that the AFM order differently responds to the magnetic field, depending on the field directions. For B||c, the clear anomaly due to the AFM transition is observed up to the AFM critical field of ~5 T in the thermodynamic quantities, whereas it is rapidly damped with increasing B for B||a. We discuss this anisotropic response on the basis of a rich variety of the AFM modulations involved in the Ce115 compounds.
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Submitted 16 November, 2015;
originally announced November 2015.
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Quadrupole Order in the Frustrated Pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$
Authors:
H. Takatsu,
S. Onoda,
S. Kittaka,
A. Kasahara,
Y. Kono,
T. Sakakibara,
Y. Kato,
B. Fåk,
J. Ollivier,
J. W. Lynn,
T. Taniguchi,
M. Wakita,
H. Kadowaki
Abstract:
A hidden order that emerges in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ with $T_{\text{c}}=0.53$ K is studied using specific heat, magnetization, and neutron scattering experiments on a high-quality single crystal. Semi-quantitative analyses based on a pseudospin-1/2 Hamiltonian for ionic non-Kramers magnetic doublets demonstrate that it is an ordered state of electric quadrupole mo…
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A hidden order that emerges in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ with $T_{\text{c}}=0.53$ K is studied using specific heat, magnetization, and neutron scattering experiments on a high-quality single crystal. Semi-quantitative analyses based on a pseudospin-1/2 Hamiltonian for ionic non-Kramers magnetic doublets demonstrate that it is an ordered state of electric quadrupole moments. The elusive spin liquid state of the nominal Tb$_2$Ti$_2$O$_7$ is most likely a U(1) quantum spin-liquid state.
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Submitted 17 April, 2016; v1 submitted 15 June, 2015;
originally announced June 2015.
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Anomalous magnetization of $S$=2 ferromagnetic-antiferromagnetic alternating chain with Ising anisotropy
Authors:
H. Yamaguchi,
Y. Shinpuku,
Y. Kono,
S. Kittaka,
T. Sakakibara,
M. Hagiwara,
T. Kawakami,
K. Iwase,
T. Ono,
Y. Hosokoshi
Abstract:
We present the first experimental realization of an $S=2$ ferromagnetic-antiferromagnetic (F-AF) alternating chain in a new Mn-verdazyl complex [Mn(hfac)$_2$]$\cdot$($o$-Py-V) [hfac=1,1,1,5,5,5-hexafluoroacetylacetonate; $o$-Py-V=3-(2-pyridyl)-1,5-diphenylverdazyl]. Through the $ab$ $initio$ molecular orbital calculation, magnetization, and ESR measurements, this compound is confirmed to form an…
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We present the first experimental realization of an $S=2$ ferromagnetic-antiferromagnetic (F-AF) alternating chain in a new Mn-verdazyl complex [Mn(hfac)$_2$]$\cdot$($o$-Py-V) [hfac=1,1,1,5,5,5-hexafluoroacetylacetonate; $o$-Py-V=3-(2-pyridyl)-1,5-diphenylverdazyl]. Through the $ab$ $initio$ molecular orbital calculation, magnetization, and ESR measurements, this compound is confirmed to form an $S=2$ F-AF alternating chain with Ising anisotropy below about 100 K. Furthermore, we find an anomalous change in magnetization at 1/4 of the saturation value, which is probably a manifestation of the quantum nature of the system.
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Submitted 18 March, 2015;
originally announced March 2015.
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$S$ = 1/2 ferromagnetic-antiferromagnetic alternating Heisenberg chain in a zinc-verdazyl complex
Authors:
Hironori Yamaguchi,
Yasuhiro Shinpuku,
Tokuro Shimokawa,
Kenji Iwase,
Toshio Ono,
Yohei Kono,
Shunichiro Kittaka,
Toshiro Sakakibara,
Yuko Hosokoshi
Abstract:
We successfully synthesized the zinc-verdazyl complex [Zn(hfac)$_2$]$\cdot$($o$-Py-V) [hfac = 1,1,1,5,5,5-hexafluoroacetylacetonate; $o$-Py-V = 3-(2-pyridyl)-1,5-diphenylverdazyl], which is an ideal model compound with an $S$ = 1/2 ferromagnetic-antiferromagnetic alternating Heisenberg chain (F-AF AHC). $Ab$ $initio$ molecular orbital (MO) calculations indicate that two dominant interactions…
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We successfully synthesized the zinc-verdazyl complex [Zn(hfac)$_2$]$\cdot$($o$-Py-V) [hfac = 1,1,1,5,5,5-hexafluoroacetylacetonate; $o$-Py-V = 3-(2-pyridyl)-1,5-diphenylverdazyl], which is an ideal model compound with an $S$ = 1/2 ferromagnetic-antiferromagnetic alternating Heisenberg chain (F-AF AHC). $Ab$ $initio$ molecular orbital (MO) calculations indicate that two dominant interactions $J_{\rm{F}}$ and $J_{\rm{AF}}$ form the $S=1/2$ F-AF AHC in this compound. The magnetic susceptibility and magnetic specific heat of the compound exhibit thermally activated behavior below approximately 1 K. Furthermore, its magnetization curve is observed up to the saturation field and directly indicates a zero-field excitation gap of 0.5 T. These experimental results provide evidence for the existence of a Haldane gap. We successfully explain the results in terms of the $S=1/2$ F-AF AHC through quantum Monte Carlo calculations with $|J_{\rm{AF}}/J_{\rm{F}}|$ = 0.22. The $ab$ $initio$ MO calculations also indicate a weak AF interchain interaction $J'$ and that the coupled F-AF AHCs form a honeycomb lattice. The $J'$ dependence of the Haldane gap is calculated, and the actual value of $J'$ is determined to be less than 0.01$|J_{\rm{F}}|$.
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Submitted 24 February, 2015;
originally announced February 2015.
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Fine-Tuning of Magnetic Interactions in Organic Spin Ladders
Authors:
Hironori Yamaguchi,
Hirotsugu Miyagai,
Tokuro Shimokawa,
Kenji Iwase,
Toshio Ono,
Yohei Kono,
Naoki Kase,
Koji Araki,
Shunichiro Kittaka,
Toshiro Sakakibara,
Takashi Kawakami,
Kouichi Okunishi,
Yuko Hosokoshi
Abstract:
We have succeeded in synthesizing two types of new organic radical crystals 3-I-V [= 3- (3-iodophenyl)-1,5-diphenylverdazyl] and 3-Br-4-F-V [= 3-(3-bromo-4-fluorophenyl)-1,5- diphenylverdazyl]. Their crystal strucutures are found to be isomorphous to that of previously reported spin ladder 3-Cl-4-F-V. Through the quantitative analysis of their molecular arrangements and magnetic properties, we con…
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We have succeeded in synthesizing two types of new organic radical crystals 3-I-V [= 3- (3-iodophenyl)-1,5-diphenylverdazyl] and 3-Br-4-F-V [= 3-(3-bromo-4-fluorophenyl)-1,5- diphenylverdazyl]. Their crystal strucutures are found to be isomorphous to that of previously reported spin ladder 3-Cl-4-F-V. Through the quantitative analysis of their molecular arrangements and magnetic properties, we confirm that these materials form ferromagnetic chain-based spin ladders with slightly modulated magnetic interactions. These results present the first quantitative demonstration of the fine-tuning of magnetic interactions in the molecular- based materials.
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Submitted 12 February, 2014;
originally announced February 2014.
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Possible Evolution of Antiferromagnetism in Zn-Doped Heavy-Fermion Superconductor CeCoIn5
Authors:
Makoto Yokoyama,
Kenji Fujimura,
Sara Ishikawa,
Masashi Kimura,
Takeshi Hasegawa,
Ikuto Kawasaki,
Kenichi Tenya,
Yohei Kono,
Toshiro Sakakibara
Abstract:
We have succeeded in growing single crystals of the heavy-fermion superconductor CeCo(In1-xZnx)5 with x<=0.07. Measurements of specific heat, electrical resistivity, dc magnetization and ac susceptibility revealed that the superconducting (SC) transition temperature Tc decreases from 2.25 K (x=0) to 1.8 K (x=0.05) by doping Zn into CeCoIn5. Furthermore, these measurements indicate a development of…
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We have succeeded in growing single crystals of the heavy-fermion superconductor CeCo(In1-xZnx)5 with x<=0.07. Measurements of specific heat, electrical resistivity, dc magnetization and ac susceptibility revealed that the superconducting (SC) transition temperature Tc decreases from 2.25 K (x=0) to 1.8 K (x=0.05) by doping Zn into CeCoIn5. Furthermore, these measurements indicate a development of a new ordered phase below T_o ~ 2.2 K for x=>0.05, characterized by the reduced magnetization and electrical resistivity in the ordered phase, and the enhancement of specific heat at T_o. This phase transition can be also recognized by the shoulder-like anomaly seen at H_o ~ 55 kOe in the field variations of the magnetization at low temperatures, which is clearly distinguished from the superconducting critical fields Hc2=49 kOe for x=0.05 and 42 kOe for x=0.07. We suggest from these results that the antiferromagnetic (AFM) order is generated by doping Zn, and the interplay between the SC and AFM orders is realized in CeCo(In1-xZnx)5.
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Submitted 3 February, 2014;
originally announced February 2014.
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Various regimes of quantum behavior in S = 1/2 Heisenberg antiferromagnetic chain with fourfold periodicity
Authors:
H. Yamaguchi,
T. Okubo,
K. Iwase,
T. Ono,
Y. Kono,
S. Kittaka,
T. Sakakibara,
A. Matsuo,
K. Kindo,
Y. Hosokoshi
Abstract:
We have succeeded in synthesizing single crystals of the verdazyl radical beta-2,6-Cl2-V [= beta-3-(2,6-dichlorophenyl)-1,5-diphenylverdazyl]. The ab initio MO calculation indicated the formation of an S = 1/2 Heisenberg antiferromagnetic chain with four-fold magnetic periodicity consisting of three types of exchange interactions.We have successfully explained the magnetic and thermodynamic proper…
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We have succeeded in synthesizing single crystals of the verdazyl radical beta-2,6-Cl2-V [= beta-3-(2,6-dichlorophenyl)-1,5-diphenylverdazyl]. The ab initio MO calculation indicated the formation of an S = 1/2 Heisenberg antiferromagnetic chain with four-fold magnetic periodicity consisting of three types of exchange interactions.We have successfully explained the magnetic and thermodynamic properties based on the expected spin model by using the quantum Monte Carlo method. Furthermore, we revealed that the alternating and unique Ising ferromagnetic chains become effective in the specific field regions and observed a cooperative phenomenon caused by the magnetic order and quantum fluctuations. These results demonstrate that verdazyl radical could form unconventional spin model with interesting quantum behavior and provide a new way to study a variety of quantum spin systems.
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Submitted 19 November, 2013;
originally announced November 2013.