arXiv subjects

Hironori Sakai

Publications and source records attributed to Hironori Sakai.

At least 19 recordsLinked to original sources

arXiv2026

Spin-orbit-entangled $J_{\rm eff}=\frac{1}{2}$ magnetism and unconventional spin freezing in the bond-disordered pyrochlore antiferromagnet NaCdCo$_2$F$_7$

Bond disorder in frustrated pyrochlore antiferromagnets can give rise to fundamentally different quantum ground states depending on the nature of the local magnetic moments. Here, we show that the bond-disordered $J_{\rm eff}=\frac{1}{2}$ pyrochlore antiferromagnet NaCdCo$_2$F$_7$ realizes an unconventional spin-glass-like state with continued dynamics, in stark contrast to its isostructural $S=\frac{1}{2}$ NaCdCu$_2$F$_7$ counterpart. High-field magnetization and Co $L_{2,3}$-edge XAS/XMCD establish spin-orbit-entangled $J_{\rm eff}=\frac{1}{2}$ Co$^{2+}$ moments with a substantial unquenched orbital contribution, consistent with local $XY$ anisotropy seen in the isostructural Na$A''$Co$_2$F$_7$ ($A''$ = Ca, Sr) analogues. $μ$SR and $^{23}$Na NMR measurements reveal progressive slowing of spin fluctuations below $\sim10$ K, culminating in a partially frozen state with persistent low-temperature dynamics that deviates from a canonical spin glass. Comparison with the isostructural bond-disordered pyrochlore NaCdCu$_2$F$_7$, which realizes a random-singlet state, reveals a fundamentally different response of spin-orbit-entangled Co$^{2+}$ moments to bond disorder. These results identify spin-orbit coupling as a key ingredient governing the fate of bond-disordered frustrated pyrochlore magnets.

cond-mat.str-el↗

arXiv2026

Paramagnetic electron-nuclear spin entanglement in HoCo2Zn20

We investigated electron-nuclear spin entanglement in the paramagnetic ground state of the Ho-based cubic compound HoCo2Zn20. From analyses of magnetization and specific heat data, we determined the cubic crystalline electric field (CEF) parameters, the magnetic exchange constant, and the hyperfine coupling constant between the 4f magnetic moment and the 165Ho nuclear spin. Our results show that the Gamma5 CEF ground state is split by the hyperfine coupling, with an energy width of 1.3 K at 0 T, and that the true paramagnetic ground state is a quasi-sextet arising primarily from entanglement between the f-electron effective spin S = 1 and the 165Ho nuclear spin I = 7/2. We further demonstrate that, depending on the CEF parameters, the paramagnetic ground state can switch to an electron-nuclear coupled dectet. These findings underscore the importance of accurately identifying the electron-nuclear level scheme for understanding the low-temperature properties of rare-earth compounds containing spin-active nuclei.

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arXiv2026

Electron-Hole Scattering Dichotomy and Anisotropic Warping in Quasi-Two-Dimensional Fermi Surfaces of UTe2

We present a combined experimental and theoretical study of the detailed Fermi-surface (FS) geometry of UTe2, a heavy-fermion superconductor that has recently attracted considerable attention as a promising candidate for spin-triplet pairing. Using angle-dependent magnetoresistance oscillations, a bulk- and low-energy-sensitive transport probe for quasi-two-dimensional (Q2D) electronic structures, we directly determine the in-plane FS geometry. We found that the Q2D FS exhibits a rectangular cross-sectional shape with strongly anisotropic warping, originating from the hybridization of two orthogonal quasi-one-dimensional bands. Through a quantitative comparison between experiment and theoretical calculations, we further reveal a large electron-hole scattering dichotomy: the quasiparticle lifetime on the electron FS is substantially shorter than that on the hole FS. This dichotomy is naturally explained by anisotropic, low-dimensional antiferromagnetic fluctuations, which selectively enhance scattering on the electron FS. This suggests a dominant role of the electron pockets for the emergence of superconductivity. Our results clarify a direct relation between FS geometry, magnetic fluctuations, and momentum-dependent quasiparticle lifetimes, and thus providing a crucial basis for the microscopic understanding of pairing mechanism, and impose stringent constraints on the gap symmetry of spin-triplet superconductivity in UTe2.

cond-mat.supr-con↗

arXiv2026

Intimate relationship between spin configuration in the triplet pair and superconductivity in UTe$_2$

Spin-triplet superconductivity is an intriguing quantum coherent state with both spin and orbital degrees of freedom, which holds significant potential for future applications in quantum technology. However, how the spin of the triplet pairs responds to an external magnetic field remains poorly understood. This is mainly due to the absence of suitable spin-triplet superconductors. Here, we report results of Knight-shift and ac-susceptibility measurements on UTe$_2$. We demonstrate that the spin susceptibility, which slightly decreases compared to the normal-state value below the superconducting (SC) transition temperature $T_{\rm c}$, is rapidly restored and nearly recovers to the normal-state values around 5 T, well below the SC upper critical field $H_{c2}$ when the magnetic field is applied along the $c$ axis ($H \parallel c$). In addition, we found that $H_{\rm c2}$ of superconductivity becomes larger when the SC spin aligns with the magnetic field. By considering the results on $H \parallel b$, our results suggest the presence of a close relationship between the spin configuration of the triplet pair and $H_{\rm c2}$, as well as the anisotropic pinning interaction acting on the triplet pairs. These phenomena, which have never been observed in spin-singlet superconductors, represent characteristic features unique to spin-triplet superconductors. We discuss the similarities between superconductivity in UTe$_2$ and superfluid $^3$He, focusing on their spin-triplet pairing states.

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arXiv2026

Random singlet physics in the $S = \frac{1}{2}$ pyrochlore antiferromagnet NaCdCu$_2$F$_7$

We report a random singlet ground state in the $S=\frac{1}{2}$ Heisenberg pyrochlore antiferromagnet NaCdCu$_2$F$_7$. Cationic Na$^+$/Cd$^{2+}$ disorder on the pyrochlore $A$ site generates a broad distribution of Cu$^{2+}$--F$^-$--Cu$^{2+}$ exchange couplings, introducing intrinsic magnetic bond disorder. Despite strong antiferromagnetic interactions ($θ_{\mathrm{CW}}=-72$~K), no magnetic order or global spin freezing is observed in DC and AC susceptibility, specific heat or $^{23}$Na nuclear magnetic resonance to 120 mK, with muon spin relaxation experiments confirming persistent spin dynamics to 58 mK. $T$-linear specific heat, a Curie-like susceptibility tail, and power-law scaling with data collapse in $χ(T)$, $M(H)$, $C_{\mathrm{mag}}/T$, $^{23}$Na $(1/T_1T)$ and the muon spin polarization $P(t)$ reveal a disorder-driven network of random singlets and orphan spins. Scaling across multiple bulk and local probes is consistent with a broad distribution of exchange energies, $P[\mathcal{J}] \sim \mathcal{J}^{-α}$. This behavior contrasts with previously-studied Na$A''B_2$F$_7$ pyrochlore fluorides, where magnetic bond disorder precipitates spin-glass freezing, underscoring the crucial role of strong $S=\frac{1}{2}$ quantum fluctuations in NaCdCu$_2$F$_7$.

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arXiv2025

$b$-axis and $c$-axis Knight shift measurements in the superconducting state on ultraclean UTe$_2$ with $T_c$ = 2.1 K

Knight shifts along the $b$ and $c$ axes ($K_b$ and $K_c$) at two crystallographically distinct Te sites were measured down to 70 mK using $^{125}$Te nuclear magnetic resonance (NMR) on an ultraclean UTe$_2$ single crystal with a superconducting (SC) transition temperature $T_{\mathrm{c}}$ = 2.1 K. This was carried out to determine the $\boldsymbol{d}$-vector components, which are the order parameter in the spin-triplet pairing. Although the decrease in $K_b$ and $K_c$ is comparable to the theoretical estimation of the SC diamagnetic shielding effect, it is confirmed, by taking the difference between two Knight shifts at the distinct Te sites, that the spin susceptibility along the $b$ and $c$ axes decreases in the SC state. Taking into account the large decrease in $K_a$ in the SC state, we conclude that the $\boldsymbol{d}$ vector has components along all three crystal axes.

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arXiv2025

Intrinsic low-temperature magnetic properties on the ultra-clean UTe$_2$ with $T_{\rm c}$ = 2.1 K revealed by $^{125}$Te NMR

To investigate the intrinsic magnetic properties of UTe$_2$, we performed $^{125}$Te-NMR measurements on the ultra-clean single-crystalline UTe$_2$ with superconducting transition temperature $T_{\rm c}$ = 2.1~K and compared the results with those of the $T_{\rm c}$ = 1.6~K sample. The broadening of the linewidth of the NMR spectrum in the $a$-axis magnetic field and the low-temperature magnetic fluctuations observed in the 1.6~K sample are suppressed in the ultra-clean sample, indicating that such magnetic properties originate from a tiny amount of U deficiency. The present results suggest that the magnetic properties in UTe$_2$ are sensitive to the U deficiency. We also observed a peculiar angular dependence of the NMR quantities due to large magnetic anisotropy with the $a$-axis as the magnetic easy axis.

cond-mat.supr-con↗

arXiv2024

Clear Reduction in Spin Susceptibility and Superconducting Spin Rotation for $H \parallel a$ in the Early-Stage Sample of Spin-Triplet Superconductor UTe$_2$

We report the re-measurement of the $a$-axis spin susceptibility component in an early-stage sample of the spin-triplet superconductor UTe$_2$ with the transition temperature of $T_{\rm SC}$ = 1.6 K. Using Knight-shift measurements along the $b$ axis and at a 10-degree tilt from the $b$ axis towards the $a$ axis, we accurately determined the $a$-axis component without directly measuring the $a$-axis Knight shift. Our results reveal a decrease of approximately 3\% in the $a$-axis spin susceptibility in the superconducting state under $a$-axis magnetic field $μ_0 H_a \sim 0.1$ T, indicating that the spin susceptibility decreases similarly in both early-stage and ultraclean samples with $T_{\rm SC}$ = 2.1 K. The previously reported absence of the reduction in Knight shift is attributed to the missing of signal from the superconducting region and to the detection of residual signals from the non-superconducting region instead. We also found that the decrease in the $a$-axis spin susceptibility is immediately suppressed with increasing the $a$-axis magnetic field and is estimated to be completely suppressed at around 1.5 T due to superconducting spin rotation.

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arXiv2024

Dramatic elastic response at the critical end point in UTe$_2$

The first-order transition line in the \textit{H-T} phase diagram of itinerant electron metamagnets terminates at the critical end point-analogous to the critical point on the gas-liquid condensation line in the \textit{p-T} phase diagram. To unravel the impact of critical magnetic fluctuations on the crystal lattice of a metamagnet at the critical end point, we performed an ultrasonic study of the itinerant electron metamagnet UTe$_2$ across varying temperatures and magnetic fields. At temperatures exceeding 9 K, a distinct V-shaped anomaly emerges, precisely centered at the critical field of the metamagnetic transition in the isothermal field dependence of elastic constants. This anomaly arises from lattice instability, triggered by critical magnetic fluctuations via strong magnetoelastic interactions. Remarkably, this effect is maximized precisely at the critical-end-point temperature. Comparative measurements of another itinerant metamagnet, UCoAl, reveal intriguing commonalities. Despite significant differences in the paramagnetic ground state, lattice symmetry, and the expected metamagnetic transition process between UTe$_2$ and UCoAl, both exhibit similar anomalies in elastic properties near the critical end point. These shared aspects may hold universality for other itinerant electron metamagnets.

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arXiv2023

Longitudinal spin fluctuations driving field-reinforced superconductivity in UTe$_2$

Our measurements of $^{125}$Te NMR relaxations reveal an enhancement of electronic spin fluctuations above $μ_0H^*\sim15$ T, leading to their divergence in the vicinity of the metamagnetic transition at $μ_0H_m\approx35$ T, below which field-reinforced superconductivity appears when a magnetic field ($H$) is applied along the crystallographic $b$ axis. The NMR data evidence that these fluctuations are dominantly longitudinal, providing a key to understanding the peculiar superconducting phase diagram in $H\|b$, where such fluctuations enhance the pairing interactions.

cond-mat.supr-con↗

arXiv2023

Superconducting-Spin Reorientation in Spin-Triplet Multiple Superconducting Phases of UTe2

Superconducting (SC) state has spin and orbital degrees of freedom, and spin-triplet superconductivity shows multiple SC phases due to the presence of these degrees of freedom. However, the observation of spin-direction rotation occurring inside the SC state (SC spin rotation) has hardly been reported. UTe2, a recently discovered topological superconductor, exhibits various SC phases under pressure: SC state at ambient pressure (SC1), high-temperature SC state above 0.5 GPa (SC2), and low-temperature SC state above 0.5 GPa (SC3). We performed nuclear magnetic resonance and AC susceptibility measurements on single-crystal UTe2. The b-axis spin susceptibility remains unchanged in SC2, unlike in SC1, and decreases below the SC2-SC3 transition with spin modulation. These unique properties in SC3 arise from the coexistence of two SC order parameters. Our NMR results confirm the spin-triplet superconductivity with SC spin parallel to b in SC2, and unveil the remaining of spin degrees of freedom in superconducting UTe2.

cond-mat.supr-con↗

arXiv2023

Low-temperature Magnetic Fluctuations Investigated by $^{125}$Te-NMR on the Uranium-based Superconductor UTe$_{2}$

To investigate the static and dynamic magnetic properties on the uranium-based superconductor UTe$_{2}$, we measured the NMR Knight shift $K$ and the nuclear spin-lattice relaxation rate $1/T_{1}$ in $H \parallel a$ by $^{125}$Te-NMR on a $^{125}$Te-enriched single-crystal sample. $1/T_1T$ in $H \parallel a$ is much smaller than $1/T_1T$ in $H \parallel b$ and $c$, and magnetic fluctuations along each axis are derived from the $1/T_1T$ measured in $H$ parallel to all three crystalline axes. The magnetic fluctuations are almost identical at two Te sites and isotropic at high temperatures, but become anisotropic below 40 K, where heavy-fermion state is formed. The character of magnetic fluctuations in UTe$_2$ is discussed with the comparison to its static susceptibility and the results on other U-based superconductors. It is considered that the magnetic fluctuations probed with the NMR measurements are determined by the magnetic properties inside the two-leg ladder formed by U atoms, which are dominated by the $q_a$ = 0 ferromagnetic fluctuations.

cond-mat.supr-con↗

arXiv2023

Large Reduction in the $a$-axis Knight Shift on UTe$_2$ with $T_{\rm c}$ = 2.1 K

Spin susceptibility in the superconducting (SC) state was measured in the higher-quality sample of uranium-based superconductor UTe$_2$ by using Knight-shift measurements for a magnetic field $H$ along all three crystalline axes. In the higher-quality sample, the SC transition temperature $T_{\rm c}$ is about 2.1 K, and the residual electronic term in the specific heat is almost zero. The NMR linewidth becomes narrower and is almost half of that in the previous sample with $T_{\rm c} \sim 1.6$ K when $H \parallel a$ and $c$. Although the Knight-shift behavior was not so different from the previous results for $H \parallel b$, and $c$, a large reduction in Knight shift along the $a$ axis was observed, in contrast with the previous $a$-axis Knight shift result. We discuss the origin of the difference between the previous and present results, and the possible SC state derived from the present results.

cond-mat.supr-con↗

arXiv2022

Ferromagnetic Crossover within the Ferromagnetic Order of U$_{7}$Te$_{12}$

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 $μ_{\rm B}$ 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 $λ$-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.

cond-mat.str-el↗

arXiv2022

First Observation of de Haas-van Alphen Effect and Fermi Surfaces in Unconventional Superconductor UTe2

We report the first observation of the de Haas-van Alphen (dHvA) effect in the novel spin-triplet superconductor UTe2 using high quality single crystals with the high residual resistivity ratio (RRR) over 200. The dHvA frequencies, named alpha and beta, are detected for the field directions between c and a-axes. The frequency of branch beta increases rapidly with the field angle tilted from c to a-axis, while branch alpha splits, owing to the maximal and minimal cross-sectional areas from the same Fermi surface. Both dHvA branches, alpha and beta reveal two kinds of cylindrical Fermi surfaces with a strong corrugation at least for branch alpha. The angular dependence of the dHvA frequencies is in very good agreement with that calculated by the generalized gradient approximation (GGA) method taking into account the on-site Coulomb repulsion of U = 2 eV, indicating the main Fermi surfaces are experimentally detected. The detected cyclotron effective masses are large in the range from 32 to 57 m0 . They are approximately 10-20 times lager than the corresponding band masses, consistent with the mass enhancement obtained from the Sommerfeld coefficient and the calculated density of states at the Fermi level. The local density approximation (LDA) calculations of ThTe2 assuming U4+ with the 5f^2 localized model are in less agreement with our experimental results, in spite of the prediction for two cylindrical Fermi surfaces, suggesting a mixed valence states of U4+ and U3+ in UTe2.

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arXiv2022

Drastic change in magnetic anisotropy of UTe2 under pressure revealed by 125Te-NMR

To investigate the normal-state magnetic properties of UTe2 under pressure, we perform 125Te nuclear magnetic resonance (NMR) measurements up to 2 GPa. Below 1.2 GPa, the b-axis NMR Knight shift shows a broad maximum at the so-called T_chimax on cooling, which is consistent with the magnetization measurement under pressure. T_chimax decreases with increasing pressure and disappears at the critical pressure Pc = 1.7 GPa, above which superconductivity is destroyed. This tendency is also observed in the temperature dependence of the nuclear spin-lattice relaxation rate 1/T1. At low pressures, 1/T1 shows a conventional Fermi-liquid behavior (1/T1T = constant) at low temperatures, indicating the formation of the heavy-fermion state. Above Pc, 1/T1T follows a 1/T behavior without any crossover to the heavy-fermion state down to the lowest temperature (~3 K). In addition, the NMR signals disappear below 3~K, due to the influence of the magnetically ordered moments. From the pressure dependence of the T_chimax and Knight shift, it was found that the Fermi surface character is abruptly changed at Pc, and that superconductivity is observed only in the heavy-fermion state.

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arXiv2022

Superconducting order parameter in UTe$_2$ determined by Knight shift measurement

This study investigates the spin susceptibility in U-based superconductor UTe$_2$ in the superconducting (SC) state by using Knight shift measurements for a magnetic field $H$ along the $a$ axis, which is the magnetic easy axis of UTe$_2$. Although a tiny anomaly ascribed to the SC diamagnetic effect was observed just below the SC transition temperature $T_{\rm c}$, the $a$-axis Knight shift in the SC state shows no significant decrease, following the extrapolation from the normal-state temperature dependence. This indicates that the spin susceptibility is nearly unchanged below $T_{\rm c}$. Considering the previous Knight shift results for $H \parallel b$ and $H \parallel c$, the dominant SC state is determined to be $B_{\rm 3u}$ in the spin-triplet pairing, which is consistent with the spin anisotropy in the normal state. The present result shows that UTe$_2$ is a spin-triplet superconductor with spin degrees of freedom.

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arXiv2022

Slow Electronic Dynamics in the Paramagnetic State of UTe$_2$

$^{125}$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 magnetic or Fermi-surface instability would be the origin of the characteristic fluctuations.

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