arXiv subjects

S. Nakatsuji

Publications and source records attributed to S. Nakatsuji.

At least 37 records · Page 2Linked to original sources

arXiv2017

Evidence for Magnetic Weyl Fermions in a Correlated Metal

Recent discovery of both gapped and gapless topological phases in weakly correlated electron systems has introduced various relativistic particles and a number of exotic phenomena in condensed matter physics. The Weyl fermion is a prominent example of three dimensional (3D), gapless topological excitation, which has been experimentally identified in inversion symmetry breaking semimetals. However, their realization in spontaneously time reversal symmetry (TRS) breaking magnetically ordered states of correlated materials has so far remained hypothetical. Here, we report a set of experimental evidence for elusive magnetic Weyl fermions in Mn$_3$Sn, a non-collinear antiferromagnet that exhibits a large anomalous Hall effect even at room temperature. Detailed comparison between our angle resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations reveals significant bandwidth renormalization and damping effects due to the strong correlation among Mn 3$d$ electrons. Moreover, our transport measurements have unveiled strong evidence for the chiral anomaly of Weyl fermions, namely, the emergence of positive magnetoconductance only in the presence of parallel electric and magnetic fields. The magnetic Weyl fermions of Mn$_3$Sn have a significant technological potential, since a weak field ($\sim$ 10 mT) is adequate for controlling the distribution of Weyl points and the large fictitious field ($\sim$ a few 100 T) in the momentum space. Our discovery thus lays the foundation for a new field of science and technology involving the magnetic Weyl excitations of strongly correlated electron systems.

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arXiv2017

Large Spontaneous Hall Effects in Chiral Topological Magnets

As novel topological phases in correlated electron systems, we have found two examples of non-ferromagnetic states that exhibit a large anomalous Hall effect. One is the chiral spin liquid compound Pr$_{2}$Ir$_{2}$O$_{7}$, which exhibits a spontaneous Hall effect in a spin liquid state due to spin ice correlation. The other is the chiral antiferromagnets Mn$_{3}$Sn and Mn$_{3}$Ge that exhibit a large anomalous Hall effect at room temperature. The latter shows a sign change of the anomalous Hall effect by a small change in the magnetic field by a few 100 G, which should be useful for various applications. We will discuss that the magnetic Weyl metal states are the origin for such a large anomalous Hall effect observed in both the spin liquid and antiferromagnet that possess almost no magnetization.

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arXiv2017

Disordered Route to the Coulomb Quantum Spin Liquid: Random Transverse Fields on Spin Ice in Pr$_2$Zr$_2$O$_7$

Inelastic neutron scattering reveals a broad continuum of excitations in Pr$_2$Zr$_2$O$_7$, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields ($Δ$) acting on the non-Kramers Pr$^{3+}$ crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution $ρ(Δ)\propto (Δ^2+Γ^2)^{-1}$ where $ Γ=0.27(1)$ meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr$_2$Zr$_2$O$_7$ actually induces a quantum spin liquid.

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arXiv2016

Multiband electronic transport in $α$-Yb$_{1-x}$Sr$_{x}$AlB$_{4}$ [x = 0, 0.19(3)] single crystals

We report on the evidence for the multiband electronic transport in $α$-YbAlB$_{4}$ and $α$-Yb$_{0.81(2)}$Sr$_{0.19(3)}$AlB$_{4}$. Multiband transport reveals itself below 10 K in both compounds via Hall effect measurements, whereas anisotropic magnetic ground state sets in below 3 K in $α$-Yb$_{0.81(2)}$Sr$_{0.19(3)}$AlB$_{4}$. Our results show that Sr$^{2+}$ substitution enhances conductivity, but does not change the quasiparticle mass of bands induced by heavy fermion hybridization.

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arXiv2016

Low-Energy Excitations and Ground State Selection in Quantum Breathing Pyrochlore Antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$

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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arXiv2016

Quantum Criticality and Inhomogeneous Magnetic Order in Fe-doped alpha-YbAlB4

The intermediate-valent polymorphs $α$- and $β$-YbAlB$_4$ exhibit quantum criticality and other novel properties not usually associated with intermediate valence. Iron doping induces quantum criticality in $α$-YbAlB$_4$ and magnetic order in both compounds. We report results of muon spin relaxation ($μ$SR) experiments in the intermediate-valent alloys $α$-YbAl$_{1-x}$Fe$_x$B$_4$, $x = 0.014$ and 0.25. For $x = 0.014$ we find no evidence for magnetic order down to 25 mK\@. The dynamic muon spin relaxation rate $λ_d$ exhibits a power-law temperature dependence $λ_d \propto T^{-a}$, $a = 0.40(4)$, in the temperature range 100 mK--2 K, in disagreement with predictions by theories of antiferromagnetic (AFM) or valence quantum critical behavior. For $x = 0.25$, where AFM order develops in the temperature range 7.5--10 K, where we find coexistence of meso- or macroscopically segregated paramagnetic and AFM phases, with considerable disorder in the latter down to 2 K.

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arXiv2016

Dimensional Reduction in Quantum Dipolar Antiferromagnets

We report ac susceptibility, specific heat, and neutron scattering measurements on a dipolar-coupled antiferromagnet LiYbF$_4$. For the thermal transition, the order-parameter critical exponent is found to be 0.20(1) and the specific-heat critical exponent -0.25(1). The exponents agree with the 2D XY/h$_4$ universality class despite the lack of apparent two-dimensionality in the structure. The order-parameter exponent for the quantum phase transitions is found to be 0.35(1) corresponding to (2+1)D. These results are in line with those found for LiErF$_4$ which has the same crystal structure, but largely different T$_N$, crystal field environment and hyperfine interactions. Our results therefore experimentally establish that the dimensional reduction is universal to quantum dipolar antiferromagnets on a distorted diamond lattice.

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arXiv2016

Slater to Mott crossover in the metal to insulator transition of Nd2Ir2O7

We present an angle-resolved photoemission study of the electronic structure of the three-dimensional pyrochlore iridate Nd2Ir2O7 through its magnetic metal-insulator transition. Our data reveal that metallic Nd2Ir2O7 has a quadratic band, touching the Fermi level at the Gamma point, similarly to that of Pr2Ir2O7. The Fermi node state is, therefore, a common feature of the metallic phase of the pyrochlore iridates. Upon cooling below the transition temperature, this compound exhibits a gap opening with an energy shift of quasiparticle peaks like a band gap insulator. The quasiparticle peaks are strongly suppressed, however, with further decrease of temperature, and eventually vanish at the lowest temperature, leaving a non-dispersive flat band lacking long-lived electrons. We thereby identify a remarkable crossover from Slater to Mott insulators with decreasing temperature. These observations explain the puzzling absence of Weyl points in this material, despite its proximity to the zero temperature metal-insulator transition.

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arXiv2015

Quadratic Fermi Node in a 3D Strongly Correlated Semimetal

Strong spin-orbit coupling fosters exotic electronic states such as topological insulators and superconductors, but the combination of strong spin-orbit and strong electron-electron interactions is just beginning to be understood. Central to this emerging area are the 5d transition metal iridium oxides. Here, in the pyrochlore iridate Pr2Ir2O7, we identify a nontrivial state with a single point Fermi node protected by cubic and time-reversal symmetries, using a combination of angle-resolved photoemission spectroscopy and first principles calculations. Owing to its quadratic dispersion, the unique coincidence of four degenerate states at the Fermi energy, and strong Coulomb interactions, non-Fermi liquid behavior is predicted, for which we observe some evidence. Our discovery implies that Pr2Ir2O7 is a parent state that can be manipulated to produce other strongly correlated topological phases, such as topological Mott insulator, Weyl semi-metal, and quantum spin and anomalous Hall states.

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arXiv2015

Perturbation on Hyperfine-enhanced $^{141}$Pr Nuclear Spin Dynamics Associated with Antiferroquadrupolar Order in PrV$_2$Al$_{20}$

The nature of multipolar order and hyperfine-enhanced (HE) $^{141}$Pr nuclear spin dynamics in PrV$_2$Al$_{20}$ was investigated using the muon spin relaxation technique. No explicit sign of time-reversal symmetry breaking was found below the multipolar order temperature $T_Q\sim 0.6$ K in a zero applied field as anticipated on the basis of the antiferroquadrupolar (AFQ) order picture proposed by Sakai and Nakatsuji [J. Phys. Soc. Jpn. 80, 063701 (2011)]. Further evidence of the nonmagnetic ground state was obtained from the observation of HE $^{141}$Pr nuclear spin fluctuations in the MHz scale. A marked increase in the muon spin-lattice relaxation rate (1/$T_{\rm 1,μ}$) was observed below 1 K with decreasing temperature, which was attributed to the perturbation on the HE $^{141}$Pr nuclear spin dynamics associated with the development of AFQ correlations. The longitudinal field dependence of 1/$T_{\rm 1,μ}$ revealed that the enhanced $^{141}$Pr nuclear spin accidentally has an effective gyromagnetic ratio close to that of the muon.

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arXiv2015

Intact Quasiparticles at an Unconventional Quantum Critical Point

We report measurements of in-plane electrical and thermal transport properties in the limit $T \rightarrow 0$ near the unconventional quantum critical point in the heavy-fermion metal $β$-YbAlB$_4$. The high Kondo temperature $T_K$ $\simeq$ 200 K in this material allows us to probe transport extremely close to the critical point, at unusually small values of $T/T_K < 5 \times 10^{-4}$. Here we find that the Wiedemann-Franz law is obeyed at the lowest temperatures, implying that the Landau quasiparticles remain intact in the critical region. At finite temperatures we observe a non-Fermi liquid T-linear dependence of inelastic scattering processes to energies lower than those previously accessed. These processes have a weaker temperature dependence than in comparable heavy fermion quantum critical systems, and suggest a new temperature scale of $T \sim 0.3 K$ which signals a sudden change in character of the inelastic scattering.

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arXiv2014

Field evolution of quantum critical and heavy Fermi-liquid components in the magnetization of the mixed valence compound beta-YbAlB4

We present the high-precision magnetization data of the valence fluctuating heavy fermion superconductor $β$-YbAlB$_4$ in a wide temperature range from 0.02 K to 320 K spanning four orders of magnitude. We made detailed analyses of the $T/B$ scaling of the magnetization, and firmly confirmed the unconventional zero-field quantum criticality (QC) without tuning. We examined other possible scaling relationship such as $T/(B-B_c)^δ$ scaling, and confirmed that $δ= 1$ provides the best quality of the fit with an upper bound on the critical magnetic field $\vert B_c \vert <0.2$~mT. We further discuss the heavy Fermi-liquid component of the magnetization after subtracting the QC component estimated based on the $T/B$ scaling. The temperature dependence of the heavy Fermi-liquid component is found very similar to the magnetization of the polymorph $α$-YbAlB$_4$. In addition, the heavy Fermi-liquid component is suppressed in the magnetic field above $\sim$ 5 T as in $α$-YbAlB$_4$. This was also confirmed by the magnetization measurements up to $\sim 50$ T for both $α$- and $β$-YbAlB$_4$. Interestingly, the detailed analyses revealed that the only a part of $f$ electrons participates in the zero-field QC and the heavy fermion behavior. We also present a temperature - magnetic field phase diagram of \ybal to illustrate how the characteristic temperature and field scales evolves near the QC.

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arXiv2014

Experimental Realization of a Quantum Breathing Pyrochlore Antiferromagnet

The synthesis and characterization of a new Yb-based material Ba3Yb2Zn5O11 are reported. This material is identified as the first model system of a pseudospin-1/2 quantum antiferromagnet on "breathing" pyrochlore lattice characterized by an alternating array of small and large Yb tetrahedra. Despite dominant antiferromagnetic interactions J ~ 7 K, a large amount of magnetic entropy (25%) remains at 0.38 K, indicating that each small Yb tetrahedron forms a unique doubly degenerate singlet state. These results are well described by the Heisenberg pseudospin-1/2 single tetrahedron model.

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arXiv2014

Quadrupolar Singlet Ground State of Praseodymium in a Modulated Pyrochlore

The complex structure and magnetism of Pr$_{2-x}$Bi$_x$Ru$_2$O$_7$ was investigated by neutron scattering and EXAFS. Pr has an approximate doublet ground-state and the first excited state is a singlet. This overall crystal field level scheme is similar to metallic Pr$_2$Ir$_2$O$_7$, which is also reported here. While the B-site (Ru) is well ordered throughout, this is not the case for the A-site (Pr/Bi). A distribution of the Pr-O2 bond length indicates the Pr environment is not uniform even for $x=0$. The Bi environment is highly disordered ostensibly due to the 6s lone pairs on Bi$^{3+}$. Correspondingly we find the non-Kramers doublet ground state degeneracy otherwise anticipated for Pr in the pyrochlore structure is lifted so as to produce a quadrupolar singlet ground state with a spatially varying energy gap. For $x=0$, below T$_N$, the Ru sublattice orders antiferromagnetically, with propagation vector \textbf{k}= (0,0,0), as for Y$_2$Ru$_2$O$_7$. No ordering associated with the Pr sublattice is observed down to 100 mK. The low energy magnetic response of Pr$_{2-x}$Bi$_x$Ru$_2$O$_7$ features a broad spectrum of magnetic excitations associated with inhomogeneous splitting of the Pr quasi-doublet ground state. For $x=0$ ($x=0.97$) the spectrum is temperature dependent (independent). It appears disorder associated with Bi alloying enhances the inhomogeneous Pr crystal field level splitting so that inter-site interactions become irrelevant for $x=0.97$. The structural complexity for the A-site may be reflected in the hysteretic uniform magnetization of B-site ruthenium in the Néel phase.

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arXiv2014

Absence of Jahn-Teller transition in the hexagonal Ba3CuSb2O9 single crystal

We present a comprehensive structural study on perovskite-type 6H-Ba3CuSb2O9, which exhibits a spin-orbital short-range ordering on a honeycomb-based lattice. By combining synchrotron x-ray diffraction, electron spin resonance, ultrasound measurement and Raman spectroscopy, we found that the static Jahn-Teller distortion is absent down to the lowest temperature in the present material, indicating orbital ordering is strongly suppressed. We discuss such an unusual state is realized with the help of spin degree of freedom, leading to a spin-orbital entangled liquid state.

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arXiv2014

T/B scaling of magnetization in the mixed valent compound β-YbAlB4

Here we provide the first clear evidence of Fermi-liquid breakdown in an intermediate valence system. We employ high precision magnetization measurements of the valence fluctuating superconductor beta-YbAlB4 to probe the quantum critical free energy down to temperatures far below the characteristic energy scale of the valence fluctuations. The observed T/B scaling in the magnetization over three decades not only indicates unconventional quantum criticality, but places an upper bound on the critical magnetic field |B_c| < 0.2 mT, a value comparable with the Earth's magnetic field and six orders of magnitude smaller than the valence fluctuation scale. This tiny value of the upper bound on B_c, well inside the superconducting dome, raises the fascinating possibility that valence fluctuating beta-YbAlB4 is intrinsically quantum critical, without tuning the magnetic field, pressure, or composition: the first known example of such a phenomenon in a metal.

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arXiv2014

Quantum criticality in a metallic spin liquid

When magnetic order is suppressed by frustrated interactions, spins form a highly correlated fluctuating "spin liquid" state down to low temperatures. Magnetic order of local moments can also be suppressed when they are fully screened by conduction electrons through the Kondo effect. Thus, the combination of strong geometrical frustration and Kondo screening may lead to novel types of quantum phase transitions. We report low-temperature thermodynamic measurements on the frustrated Kondo lattice Pr$_2$Ir$_2$O$_7$, which displays a chiral spin liquid state below 1.5 K due to the frustrated interaction between Ising 4f local moments and their interplay with Ir conduction electrons. Our results provide a first clear example of zero-field quantum critical scaling that emerges in a spin liquid state of a highly frustrated metal.

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arXiv2013

Synchrotron X-ray Spectroscopy Study on the Valence State in alpha- and beta-YbAlB4 at Low Temperatures and High Magnetic Fields

The valence state of Yb ions in beta-YbAlB4 and its polymorph alpha-YbAlB4 has been investigated by using X-ray absorption and emission spectroscopy in SPring-8 at temperatures from 2 to 280 K. The observed Yb valence is 2.78 +- 0.01 in beta-YbAlB4 at 2 K by using the X-ray emission spectroscopy. The valence is found to gradually increase with increasing temperature toward the trivalent state, and the characteristic temperature of the valence fluctuation is expected to be about 290 K. We also found a small increase in the Yb valence (~0.002) by applying a magnetic field of 32 T at 40 K to beta-YbAlB4.

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