arXiv subjects

S. Nakatsuji

Publications and source records attributed to S. Nakatsuji.

At least 73 records · Page 4Linked to original sources

arXiv2008

Weak quasistatic magnetism in the frustrated Kondo lattice Pr_2Ir_2O_7

Muon spin relaxation experiments have been performed in the pyrochlore iridate Pr_2Ir_2O_7 for temperatures in the range 0.025-250 K. Kubo-Toyabe relaxation functions are observed up to > 200 K, indicating static magnetism over this temperature range. The T -> 0 static muon spin relaxation rate Delta(0) ~ 8 mus^-1 implies a weak quasistatic moment (~0.1 mu_B). The temperature dependence of Delta is highly non-mean-field-like, decreasing smoothly by orders of magnitude but remaining nonzero below ~150 K. The data rule out ordering of the full Pr^3+ CEF ground-state moment (3.0 mu_B) down to 0.025 K. The weak static magnetism is most likely due to hyperfine-enhanced ^141Pr nuclear magnetism. The dynamic relaxation rate lambda increases markedly below ~20 K, probably due to slowing down of spin fluctuations in the spin-liquid state. At low temperatures lambda is strong and temperature-independent, indicative of a high density of low-lying spin excitations as is common in frustrated antiferromagnets.

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arXiv2007

Spin dynamics and spin freezing behavior in the two-dimensional antiferromagnet NiGa$_{2}$S$_{4}$ revealed by Ga-NMR, NQR and $μ$SR measurements

We have performed $^{69,71}$Ga nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) and muon spin rotation/resonance on the quasi two-dimensional antiferromagnet (AFM) NiGa$_2$S$_4$, in order to investigate its spin dynamics and magnetic state at low temperatures. Although there exists only one crystallographic site for Ga in NiGa$_2$S$_4$, we found two distinct Ga signals by NMR and NQR. The origin of the two Ga signals is not fully understood, but possibly due to stacking faults along the c axis which induce additional broad Ga NMR and NQR signals with different local symmetries. We found the novel spin freezing occurring at $T_{\rm f}$, at which the specific heat shows a maximum, from a clear divergent behavior of the nuclear spin-lattice relaxation rate $1/T_{1}$ and nuclear spin-spin relaxation rate $1/T_{2}$ measured by Ga-NQR as well as the muon spin relaxation rate $λ$. The main sharp NQR peaks exhibit a stronger tendency of divergence, compared with the weak broader spectral peaks, indicating that the spin freezing is intrinsic in NiGa$_2$S$_4$. The behavior of these relaxation rates strongly suggests that the Ni spin fluctuations slow down towards $T_{\rm f}$, and the temperature range of the divergence is anomalously wider than that in a conventional magnetic ordering. A broad structureless spectrum and multi-component $T_1$ were observed below 2 K, indicating that a static magnetic state with incommensurate magnetic correlations or inhomogeneously distributed moments is realized at low temperatures. However, the wide temperature region between 2 K and $T_{\rm f}$, where the NQR signal was not observed, suggests that the Ni spins do not freeze immediately below $T_{\rm f}$, but keep fluctuating down to 2 K with the MHz frequency range.

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arXiv2007

Unusual superexchange pathways in a Ni triangular lattice of NiGa$_2$S$_4$ with negative charge-transfer energy

We have studied the electronic structure of the Ni triangular lattice in NiGa$_2$S$_4$ using photoemission spectroscopy and subsequent model calculations. The cluster-model analysis of the Ni 2$p$ core-level spectrum shows that the S 3$p$ to Ni 3$d$ charge-transfer energy is $\sim$ -1 eV and the ground state is dominated by the $d^9L$ configuration ($L$ is a S 3$p$ hole). Cell perturbation analysis for the NiS$_2$ triangular lattice indicates that the strong S 3$p$ hole character of the ground state provides the enhanced superexchange interaction between the third nearest neighbor sites.

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arXiv2007

Field-induced paramagnons at the metamagnetic transition in Ca1.8Sr0.2RuO4

The magnetic excitations in Ca1.8Sr0.2RuO4 were studied across the metamagnetic transition and as a function of temperature using inelastic neutron scattering. At low temperature and low magnetic field the magnetic response is dominated by a complex superposition of incommensurate antiferromagnetic fluctuations. Upon increasing the magnetic field across the metamagnetic ransition, paramagnon and finally well-defined magnon scattering is induced, partially suppressing the incommensurate signals. The high-field phase in Ca1.8Sr0.2RuO4 has, therefore, to be considered as an intrinsically ferromagnetic state stabilized by the magnetic field.

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arXiv2006

Magnetoelastic coupling across the metamagnetic transition in Ca$_{2-x}$Sr$_x$RuO$_4$ (0.2 < x < 0.5)

The magnetoelastic coupling in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ and in Ca$_{1.5}$Sr$_{0.5}$RuO$_4$ has been studied combining high-resolution dilatometer and diffraction techniques. Both compounds exhibit strong anomalies in the thermal-expansion coefficient at zero and at high magnetic field as well as an exceptionally large magnetostriction. All these structural effects, which are strongest in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$, point to a redistribution of electrons between the different $t_{2g}$ orbitals tuned by temperature and magnetic field. The temperature and the field dependence of the thermal-expansion anomalies in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ yield evidence for a critical end-point lying close to the low-temperature metamagnetic transition; however, the expected scaling relations are not well fulfilled.

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arXiv2006

Electronic structures of layered perovskite Sr2MO4 (M=Ru, Rh, and Ir)

We investigated the electronic structures of the two-dimensional layered perovskite Sr$_{2}$\textit{M}O$_{4}$ (\textit{M}=4\textit{d} Ru, 4\textit{d} Rh, and 5\textit{d} Ir) using optical spectroscopy and polarization-dependent O 1\textit{s} x-ray absorption spectroscopy. While the ground states of the series of compounds are rather different, their optical conductivity spectra $σ(ω)$ exhibit similar interband transitions, indicative of the common electronic structures of the 4\textit{d} and 5\textit{d} layered oxides. The energy splittings between the two $e_{g}$ orbitals, $i.e.$, $d_{3z^{2}-r^{2}}$ and $d_{x^{2}-y^{2}}$, are about 2 eV, which is much larger than those in the pseudocubic and 3\textit{d} layered perovskite oxides. The electronic properties of the Sr$_{2}$\textit{M}O$_{4}$ compounds are discussed in terms of the crystal structure and the extended character of the 4\textit{d} and 5\textit{d} orbitals.

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arXiv2005

Thermodynamic Properties of (Ca,Sr)$_2$RuO$_4$ in Magnetic Fields

We have studied the influence of a magnetic field on the thermodynamic properties of Ca$_{2-x}$Sr$_{x}$RuO$_4$ in the intermediate metallic region with tilt and rotational distortions ($0.2\leq x \leq 0.5$). We find strong and anisotropic thermal expansion anomalies at low temperatures, which are suppressed and even reversed by a magnetic field. The metamagnetic transition of Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ is accompanied by a large magnetostriction. Furthermore, we observe a strong magnetic-field dependence of $c_p/T$, that can be explained by magnetic fluctuations.

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arXiv2005

Unpaired Electrons in the Heavy-Fermion Superconductor CeCoIn_{5}

Thermal conductivity and specific heat were measured in the superconducting state of the heavy fermion material Ce_{1-x}La_{x}CoIn_{5}. With increasing impurity concentration x, the suppression of T_{c} is accompanied by the increase in the residual electronic specific heat expected of a d-wave superconductor, but it occurs in parallel with a decrease in residual electronic thermal conductivity. This contrasting behavior reveals the presence of uncondensed electrons coexisting with nodal quasiparticles. An extreme multiband scenario is proposed, with a d-wave superconducting gap on the heavy-electron sheets of the Fermi surface and a negligible gap on the light, three-dimensional pockets.

cond-mat.supr-con↗

arXiv2005

Orbital ordering transition in Ca$_2$RuO$_4$ observed with resonant x-ray diffraction

Resonant x-ray diffraction performed at the $\rm L_{II}$ and $\rm L_{III}$ absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca$_2$RuO$_4$ single crystals. A large resonant enhancement due to electric dipole $2p\to 4d$ transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at $\rm T_{N}=110$ K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction signal, this transition can be attributed to orbital ordering of the Ru $t_{2g}$ electrons. The propagation vector of the orbital order is inconsistent with some theoretical predictions for the orbital state of Ca$_2$RuO$_4$.

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arXiv2005

Orbital-selective Mass Enhancements in Multi-band Ca$_{2-x}$Sr$_{x}$RuO$_{4}$ Systems Analyzed by the Extended Drude Model

We investigated optical spectra of quasi-two-dimensional multi-band Ca$% _{2-x} $Sr$_{x}$RuO$_{4}$ systems. The extended Drude model analysis on the ab-plane optical conductivity spectra indicates that the effective mass should be enhanced near $x=0.5$. Based on the sum rule argument, we showed that the orbital-selective Mott-gap opening for the $d_{yz/zx}$ bands, the widely investigated picture, could not be the origin of the mass enhancement. We exploited the multi-band effects in the extended Drude model analysis, and demonstrated that the intriguing heavy mass state near $x=0.5$ should come from the renormalization of the $d_{xy}$ band.

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arXiv2005

Quantitative analysis of Sr2RuO4 ARPES spectra: Many-body interactions in a model Fermi liquid

ARPES spectra hold a wealth of information about the many-body interactions in a correlated material. However, the quantitative analysis of ARPES spectra to extract the various coupling parameters in a consistent manner is extremely challenging, even for a model Fermi liquid system. We propose a fitting procedure which allows quantitative access to the intrinsic lineshape, deconvolved of energy and momentum resolution effects, of the correlated 2-dimensional material Sr2RuO4. For the first time in correlated 2-dimensional materials, we find an ARPES linewidth that is narrower than its binding energy, a key property of quasiparticles within Fermi liquid theory. We also find that when the electron-electron scattering component is separated from the electron-phonon and impurity scattering terms it decreases with a functional form compatible with Fermi liquid theory as the Fermi energy is approached. In combination with the previously determined Fermi surface, these results give the first complete picture of a Fermi liquid system via ARPES. Furthermore, we show that the magnitude of the extracted imaginary part of the self-energy is in remarkable agreement with DC transport measurements.

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arXiv2005

Irreversible dynamics of the phase boundary in U(Ru0.9)Rh0.04)2Si2 and implications for ordering

We report measurements and analysis of the specific heat and magnetocaloric effect at the phase boundary into the single magnetic field-induced phase (phase II) of U(Ru{0.96}Rh{0.04})2Si2, which yield striking similarities to the valence transition of Yb{1-x}YxInCu4. To explain these similarities, we propose a bootstrap mechanism by which a structural distortion causes an electric quadrupolar order parameter within phase II to become coupled to the 5f-electron hybridization, giving rise to a valence change at the transition.

cond-mat.str-el↗

arXiv2005

Severe Fermi Surface Reconstruction at a Metamagnetic-Transition in Ca$_{2-x}$Sr$_x$RuO$_4$ (for $0.2 \leq x \leq 0.5$)

We report an electrical transport study in Ca$_{2-x}$Sr$_{x}$RuO$_4$ single crystals at high magnetic fields ($B$). For $x =0.2$, the Hall constant $R_{xy}$ decreases sharply at an anisotropic metamagnetic (MM) transition reaching its value for Sr$_2$RuO$_4$ at high fields. A sharp decrease in the $A$ coefficient of the resistivity $T^2$-term and a change in the structure of the angular magnetoresistance oscillations (AMRO) for $B$ rotating in the planes, confirms the reconstruction of the Fermi surface (FS). Our observations and LDA calculations indicate a strong dependence of the FS on the Ca concentration and suggest the coexistence of itinerant and localized electronic states in single layered ruthenates.

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arXiv2005

High pressure diffraction studies on Ca2RuO4

We studied the crystal and magnetic structure of Ca2RuO4 by different diffraction techniques under high pressure. The observed first order phase transition at moderate pressure (0.5 GPa) between the insulating phase and the metallic high pressure phase is characterized by a broad region of phase coexistence. The following structural changes are observed as function of pressure: a) a discontinuous change of both the tilt and rotation angle of the RuO6-Octahedra at this transition, b) a gradual decrease of the tilt angle in the high pressure phase (p>0.5 GPa) and c) the disappearance of the tilt above 5.5GPa leading to a higher symmetry structure. By single crystal neutron diffraction at low temperature, the ferromagnetic component of the high pressure phase and a rearrangement of antiferromagnetic order in the low pressure phase was observed.

cond-mat.str-el↗

arXiv2005

Lattice dynamics and the electron-phonon interaction in Ca$_2$RuO$_4$

We present a Raman scattering study of Ca$_2$RuO$_4$, in which we investigate the temperature-dependence of the lattice dynamics and the electron-phonon interaction below the metal-insulator transition temperature ({\it T}$_{\rm MI}$). Raman spectra obtained in a backscattering geometry with light polarized in the ab-plane reveal 9 B$_{1g}$ phonon modes (140, 215, 265, 269, 292, 388, 459, 534, and 683 cm$^{-1}$) and 9 A$_g$ phonon modes (126, 192, 204, 251, 304, 322, 356, 395, and 607 cm$^{-1}$) for the orthorhombic crystal structure (Pbca$-$D$_{2h}^{15}$). With increasing temperature toward {\it T}$_{\rm MI}$, the observed phonon modes shift to lower energies and exhibit reduced spectral weights, reflecting structural changes associated with the elongation of the RuO$_6$ octahedra. Interestingly, the phonons exhibit significant increases in linewidths and asymmetries for {\it T} $>$ {\it T}$_{\rm N}$. These results indicate that there is an increase in the effective number of electrons and the electron-phonon interaction strengths as the temperature is raised through {\it T}$_{\rm N}$, suggesting the presence of orbital fluctuations in the temperature regime {\it T}$_{\rm N}$ $<$ {\it T} $<$ {\it T}$_{\rm MI}$.

cond-mat.str-el↗

arXiv2005

Gradual transition from insulator to semimetal of Ca$_{1-x}$Eu$_{x}$B$_{6}$ with increasing Eu concentration

The local environment of Eu$^{2+}$ ($4f^{7}$, $S=7/2$) in Ca$_{1-x}$Eu$_{x}$B$_{6}$ ($0.003\leqslant x\leqslant 1.00$) is investigated by means of electron spin resonance (ESR). For $x\lesssim 0.003$ the spectra show resolved \textit{fine} and \textit{hyperfine} structures due to the cubic crystal \textit{electric} field and nuclear \textit{hyperfine} field, respectively. The resonances have Lorentzian line shape, indicating an \textit{insulating} environment for the Eu$^{2+}$ ions. For $0.003\lesssim x\lesssim 0.07$, as $x$ increases, the ESR lines broaden due to local distortions caused by the Eu/Ca ions substitution. For $0.07\lesssim x\lesssim 0.30$, the lines broaden further and the spectra gradually change from Lorentzian to Dysonian resonances, suggesting a coexistence of both \textit{insulating} and \textit{metallic} environments for the Eu$^{2+}$ ions. In contrast to Ca$_{1-x}$Gd$_{x}$B$_{6}$, the \textit{fine} structure is still observable up to $x\approx 0.15$. For $x\gtrsim 0.30 $ the \textit{fine} and \textit{hyperfine} structures are no longer observed, the line width increases, and the line shape is purely Dysonian anticipating the \textit{semimetallic} character of EuB$_{6}$. This broadening is attributed to a spin-flip scattering relaxation process due to the exchange interaction between conduction and Eu$^{2+}$ $4f$ electrons. High field ESR measurements for $x\gtrsim 0.15$ reveal smaller and anisotropic line widths, which are attributed to magnetic polarons and Fermi surface effects, respectively.

cond-mat.str-el↗

arXiv2004

Magnetic field-tuned quantum critical point in CeAuSb_2

Transport, magnetic and thermal properties at high magnetic fields (H) and low temperatures (T) of the heavy fermion compound CeAuSb_2 are reported. At H=0 this layered system exhibits antiferromagnetic order below T_N = 6 K. Applying B along the inter-plane direction, leads to a continuous suppression of T_N and a quantum critical point at H_c ~ 5.4 T. Although it exhibits Fermi liquid behavior within the Neel phase, in the paramagnetic state the fluctuations associated with H_c give rise to unconventional behavior in the resistivity (sub-linear in T) and to a TlnT dependence in the magnetic contribution to the specific heat. For H > H_c and low T the electrical resistivity exhibits an unusual T^3-dependence.

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arXiv2004

Mechanism of hopping transport in disordered Mott insulators

By using a combination of detailed experimental studies and simple theoretical arguments, we identify a novel mechanism characterizing the hopping transport in the Mott insulating phase of Ca$_{2-x}$Sr$_x$RuO$_4$ near the metal-insulator transition. The hopping exponent $α$ shows a systematic evolution from a value of $α=1/2$ deeper in the insulator to the conventional Mott value $α=1/3$ closer to the transition. This behavior, which we argue to be a universal feature of disordered Mott systems close to the metal-insulator transition, is shown to reflect the gradual emergence of disorder-induced localized electronic states populating the Mott-Hubbard gap.

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