arXiv subjects

Naoki Kikugawa

Publications and source records attributed to Naoki Kikugawa.

At least 19 recordsLinked to original sources

arXiv2026

Entropy mapping under uniaxial pressure utilizing the elastocaloric effect

Uniaxial pressure is a powerful tuning parameter for quantum materials, but conventional thermodynamic probes such as specific heat are difficult to realize in the constrained geometries of strain apparatus. We develop a quantitative analysis framework for a.c. elastocaloric effect measurements that enable the reconstruction of the absolute entropy and hence specific heat across complex phase diagrams. The absolute accuracy is achieved by combining measurements in the strong coupling regime at low frequencies with high signal-to-noise measurements in the quasi-adiabatic regime at high frequencies. Applying the approach to the correlated superconductor Sr$_2$RuO$_4$, we obtain an absolute entropy map across the phase diagram including across phase transitions deep into the superconducting state. We demonstrate that from such data one can derive the absolute specific heat which is currently not possible through other approaches. This data reinforces the finding that the quenching of entropy within the superconductor Sr$_2$RuO$_4$ is strongest at the critical strain consistent with the superconducting gap being maximized at the Van Hove singularity (VHs). Furthermore, we demonstrate that, although $Δc /(γT) $ does increase at the VH strain, this increase is much weaker than previously inferred from more indirect caloric experiments.

cond-mat.supr-con↗

arXiv2026

Quantum Oscillations of $\mathrm{Sr}_2\mathrm{RuO}_4$ under c-Axis Uniaxial Stress

Uniaxial stress has now been widely used to study correlated electron materials. However, Fermi surface-resolved experimental data on the evolution of the electronic structure under piezoelectrically applied stress are sparse, with no reports of de Haas-van Alphen (dHvA) effects under uniaxial stress. Here we present dHvA measurements under $c$-axis uniaxial stress on the unconventional superconductor $\mathrm{Sr}_2\mathrm{RuO}_4$. This allows us to study the evolution of the electronic structure directly and to gain insight into the contradicting behavior of the predicted enhancement of the electronic density of states and the observed suppression of $T_\text{c}$. We are able to follow all Fermi surfaces for stress up to $-1.8$~GPa and find that the cross-sectional areas of the hole-like $α$ sheet increase and electron-like $β$ sheet decrease. At the same time, the area of the electron-like $γ$ sheet increases. Therefore, in contrast to in-plane uniaxial stress, charge transfer is the mechanism for approaching the electron-to-hole Lifshitz transition and the associated Van Hove singularity. Additionally, we find that the effective masses on all three Fermi sheets are slightly enhanced as the Lifshitz transition is approached. We compare the dHvA results with quantum oscillations in the magnetostriction and band structure calculations, and find good agreement. At a more general level, our findings show that quantum oscillation measurements under uniaxial stress, combined with band-structure calculations, offer a promising new route for studying quantum materials.

cond-mat.str-el↗

arXiv2026

A correlated insulator at the surface of the polar metal Ca$_3$Ru$_2$O$_7$

We investigate the electronic structure at the surface of the correlated oxide Ca$_3$Ru$_2$O$_7$, a low-symmetry ruthenate oxide which hosts an unconventional polar-metal phase. From a combination of angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy measurements, we demonstrate that the surface hosts an insulating phase, a distinct departure from metallicity within the bulk. Utilizing quantitative low-energy electron diffraction in conjunction with electronic structure calculations, we show how this results from a combined surface structure relaxation and the impact of marked electronic correlations in this system. Our findings highlight the proximity of Ca$_3$Ru$_2$O$_7$ to an insulating metallic state, and illustrate how subtle structural distortions can control its emergent electronic phases.

cond-mat.str-el↗

arXiv2025

Origins of spontaneous magnetic fields in Sr$_2$RuO$_4$

The nature of the broken time reversal symmetry (BTRS) state in Sr$_2$RuO$_4$ remains elusive, and its relation to superconductivity remains controversial. There are various universal predictions for the BTRS state when it is associated with a multicomponent superconducting order parameter. In particular, in the BTRS superconducting state, spontaneous fields appear around crystalline defects, impurities, superconducting domain walls and sample surfaces. However, this phenomenon has not yet been experimentally demonstrated for any BTRS superconductor. Here, we aimed to verify these predictions for Sr$_2$RuO$_4$ by performing muon spin relaxation ($μ$SR) measurements on Sr$_{2-y}$La$_{y}$RuO$_4$ single crystals at ambient pressure and stoichiometric Sr$_2$RuO$_4$ under hydrostatic pressure. The study allowed us to conclude that spontaneous fields in the BTRS superconducting state of Sr$_2$RuO$_4$ appear around non-magnetic inhomogeneities and, at the same time, decrease with the suppression of $T_{\rm c}$. The observed behaviour is consistent with the prediction for multicomponent BTRS superconductivity in Sr$_2$RuO$_4$. The results of the work are relevant to understanding BTRS superconductivity in general, as they demonstrate, for the first time, the relationship among the superconducting order parameter, the BTRS transition, and crystal-structure inhomogeneities.

cond-mat.supr-con↗

arXiv2025

High-resolution magnetostriction measurements of the Pauli-limited superconductor Sr2RuO4

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.

cond-mat.supr-con↗

arXiv2025

Multipolar Phase Transition in the 4$f^2$ fcc lattice compound PrCdNi$_{4}$

Transport and magnetic properties of a 4$f^{2}$ fcc lattice compound, PrCdNi$_4$, were studied. The magnetic susceptibility, $χ(T)$, follows the Curie--Weiss law from 300 K to 20 K, as expected for a free Pr$^{3+}$ ion. As the temperature decreases below 5 K, $χ(T)$ approaches a constant, indicating van-Vleck paramagnetic behavior. The specific heat, $C(T)$, displays a broad shoulder at around 4 K, which can be reproduced by a doublet triplet two-level model with an energy gap of 12 K. These results suggest a non-magnetic $Γ_3$ doublet ground state of the Pr$^{3+}$ ion in the cubic crystalline electric field. $C(T)$ exhibits a peak at $T_{\rm O}$ = 1.0 K and this peak remains robust against magnetic fields up to 5 T. In powder neutron diffraction measurements, no magnetic reflection was observed at 0.32 K $<$ $T_{\rm O}$. Two anomalies at $B$ = 2.1 and 5.3 T in magnetoresistance $ρ(B)$ at 0.05 K likely originate from switching in the order parameter. These results suggest that the phase transition at $T_{\rm O}$ is ascribed to an antiferro-type order of the electric quadrupole or magnetic octupole of the $Γ_3$ doublet in the 4$f^2$ fcc lattice.

cond-mat.str-el↗

arXiv2024

$T_c$ and the elastocaloric effect of Sr$_2$RuO$_4$ under $\langle 110 \rangle$ uniaxial stress: no indications of transition splitting

There is considerable evidence that the superconductivity of Sr2RuO4 has two components. Among this evidence is a jump in the shear elastic modulus $c_{66}$ at the critical temperature $T_c$, observed in ultrasound measurements. Such a jump is forbidden for homogeneous single-component order parameters, and implies that $T_c$ should develop as a cusp under the application of shear strain with $\langle 110 \rangle$ principal axes. This shear strain should split the onset temperatures of the two components, if they coexist, or select one component if they do not. Here, we report measurements of $T_c$ and the elastocaloric effect of Sr2RuO4 under uniaxial stress applied along the $[110]$ lattice direction. Within experimental resolution, we resolve neither a cusp in the stress dependence of $T_c$, nor any second transition in the elastocaloric effect data. We show that reconciling these null results with the observed jumps in $c_{66}$ requires extraordinarily fine tuning to a triple point of the Ginzburg-Landau parameter space. In addition, our results are inconsistent with homogeneous time reversal symmetry breaking at a temperature $T_2 \leq T_c$ as identified in muon spin relaxation experiments.

cond-mat.supr-con↗

arXiv2024

Negatively enhanced thermopower near a Van Hove singularity in electron-doped Sr$_2$RuO$_4$

The layered perovskite Sr$_2$RuO$_4$ serves as a model material of the two-dimensional (2D) Fermi liquid but also exhibits various emergent phenomena including the non-Fermi-liquid (NFL) behavior under external perturbations such as uniaxial pressure and chemical substitutions. Here we present the thermoelectric transport of electron-doped system Sr$_{2-y}$La$_{y}$RuO$_4$, in which a filling-induced Lifshitz transition occurs at the Van Hove singularity (VHS) point of $y\approx 0.2$. We find that the sign of the low-temperature thermopower becomes negative only near the VHS point, where the NFL behavior has been observed in the earlier work. This observation is incompatible with either a numerical calculation within a constant relaxation-time approximation or a toy-model calculation for the 2D Lifshitz transition adopting an elastic carrier scattering. As a promising origin of the observed negatively enhanced thermopower, we propose a skewed NFL state, in which an inelastic scattering with a considerable odd-frequency term plays a crucial role to negatively enhance the thermopower.

cond-mat.str-el↗

arXiv2024

Determination of the dynamic Young's modulus of quantum materials in piezoactuator-driven uniaxial pressure cells using a low-frequency a.c. method

We report on a new technique for measuring the dynamic Young's modulus, $E$, of quantum materials at low temperatures as a function of static tuning strain, $ε$, in piezoactuator-driven pressure cells. In addition to a static tuning of stress and strain, we apply a small-amplitude, finite-frequency a.c. (1 Hz$ \lesssim ω\lesssim $1000 Hz) uniaxial stress, $σ_{ac}$, to the sample and measure the resulting a.c. strain, $ε_{ac}$, using a capacitive sensor to obtain the associated modulus $E$. We demonstrate the performance of the new technique through proof-of-principle experiments on the unconventional superconductor Sr$_2$RuO$_4$, which is known for its rich temperature-strain phase diagram. In particular, we show that the magnitude of $E$, measured using this a.c. technique at low frequencies, exhibits a pronounced nonlinear elasticity, which is in very good agreement with previous Young's modulus measurements on Sr$_2$RuO$_4$ under [100] strain using a d.c. method (Noad et al., Science 382, 447-450 (2023)). By combining the new a.c. Young's modulus measurements with a.c. elastocaloric measurements in a single measurement, we demonstrate that these a.c. techniques are powerful in detecting small anomalies in the elastic properties of quantum materials. Finally, using the case of Sr$_2$RuO$_4$ as an example, we demonstrate how the imaginary component of the modulus can provide additional information about the nature of ordered phases.

cond-mat.mtrl-sci↗

arXiv2024

Controllable suppression of the unconventional superconductivity in bulk and thin-film Sr$_{2}$RuO$_{4}$ via high-energy electron irradiation

In bulk Sr$_{2}$RuO$_{4}$, the strong sensitivity of the superconducting transition temperature $T_{\text{c}}$ to nonmagnetic impurities provides robust evidence for a superconducting order parameter that changes sign around the Fermi surface. In superconducting epitaxial thin-film Sr$_{2}$RuO$_{4}$, the relationship between $T_{\text{c}}$ and the residual resistivity $ρ_0$, which in bulk samples is taken to be a proxy for the low-temperature elastic scattering rate, is far less clear. Using high-energy electron irradiation to controllably introduce point disorder into bulk single-crystal and thin-film Sr$_{2}$RuO$_{4}$, we show that $T_{\text{c}}$ is suppressed in both systems at nearly identical rates. This suggests that part of $ρ_0$ in films comes from defects that do not contribute to superconducting pairbreaking, and establishes a quantitative link between the superconductivity of bulk and thin-film samples.

cond-mat.supr-con↗

arXiv2024

Anomalous Hall effect with plateaus observed in a magnetic Weyl semimetal NdAlGe at low temperatures

In the $R$Al(Si,Ge) ($R$: lanthanides) family, both spatial inversion and time-reversal symmetries are broken. This may offer opportunities to study Weyl-fermion physics in nontrivial spin structures emerging from a noncentrosymmetric crystal structure. In this study, we investigated the anomalous Hall effect (AHE) in NdAlGe via magnetotransport, magnetization, and magnetic torque measurements down to 40 mK (0.4 K for magnetization). The single crystals grown by a laser-heated floating-zone method exhibit a single magnetic phase transition at $T_{\rm M}$ = 13.5 K, where the $T_{\rm M}$ is the transition temperature. With the magnetic field parallel to the easy $\lbrack$001$\rbrack$ axis, the AHE gradually evolves as the temperature decreases below $T_{\rm M}$. The anomalous Hall conductivity (AHC) reaches $\sim$320 $Ω^{-1}$cm$^{-1}$ at 40 mK in the magnetically saturated state. Except in low-temperature low-field plateau phases, the AHC and magnetization are proportional, and their ratio agrees with the ratios for conventional ferromagnets, suggesting that the intrinsic AHE occurs by the Karplus-Luttinger mechanism. Below $\sim$0.6 K, the curves of Hall resistivity against the field exhibit plateaus at low fields below $\sim$0.5 T, correlating with the plateaus in the magnetization curve. For the first plateau, the magnetization is one order of magnitude smaller than the magnetically saturated state, whereas the AHE is more than half that in the saturated state. This finding under well below $T_{\rm M}$ suggests that the AHE at the first plateau is not governed by the magnetization and may be interpreted based on a multipole or spin chirality.

cond-mat.str-el↗

arXiv2024

Anomalous upper critical field in the quasicrystal superconductor Ta$_{1.6}$Te

Superconductivity in quasicrystals poses a new challenge in condensed matter physics. We measured the resistance and ac magnetic susceptibility of a Ta$_{1.6}$Te dodecagonal quasicrystal, which is superconducting below $T_c \sim$ 1 K. We show that the upper critical field increases linearly with a large slope of $-$4.4 T/K with decreasing temperature down to 0.04 K, with no tendency to level off. The extrapolated zero-temperature critical field exceeds the Pauli limit by a factor of 2.3. We also observed flux-flow resistance with thermally activated behavior and an irreversibility field that is distinct from the upper critical field. We discuss these peculiarities in terms of the nonuniform superconducting gap and spin--orbit interaction in quasicrystal structures.

cond-mat.supr-con↗

arXiv2023

Superconducting Penetration Depth Through a Van Hove Singularity: Sr$_2$RuO$_4$ Under Uniaxial Stress

In the unconventional superconductor Sr$_2$RuO$_4$, uniaxial stress along the $[100]$ direction tunes the Fermi level through a Van Hove singularity (VHS) in the density of states, causing a strong enhancement of the superconducting critical temperature $T_\textrm{c}$. Here, we report measurements of the London penetration depth $λ$ as this tuning is performed. We find that the zero-temperature superfluid density, here defined as $λ(0)^{-2}$, increases by $\sim$15%, with a peak that coincides with the peak in $T_\textrm{c}$. We also find that the low temperature form of $λ(T)$ is quadratic over the entire strain range. Using scanning tunneling microscopy, we find that the gap increases from $Δ_0 \approx 350~μ$eV in unstressed Sr$_2$RuO$_4$ to $Δ_0 \approx 600~μ$eV in a sample strained to near the peak in $T_c$. With a nodal order parameter, an increase in the superconducting gap could bring about an increase in the superfluid density through reduced sensitivity to defects and through reduced non-local effects in the Meissner screening. Our data indicate that tuning to the VHS increases the gap throughout the Brillouin zone, and that non-local effects are likely more important than reduced scattering.

cond-mat.supr-con↗

arXiv2023

Giant lattice softening at a Lifshitz transition in Sr$_{2}$RuO$_{4}$

The interplay of electronic and structural degrees of freedom in solids is a topic of intense research. Experience and intuition suggest that structural changes drive conduction electron behavior, because the large number of valence electrons dominate the structural properties. As part of a seminal paper written over sixty years ago, Lifshitz discussed an alternative possibility: lattice softening driven by conduction electrons at topological Fermi surface transitions. The effect he predicted, however, was small, and has not been convincingly observed. Using measurements of the stress-strain relationship in the ultra-clean metal Sr$_{2}$RuO$_{4}$, we reveal a huge softening of the Young's modulus at a Lifshitz transition of a two-dimensional Fermi surface, and show that it is indeed entirely driven by the conduction electrons of the relevant energy band.

cond-mat.str-el↗

arXiv2023

In-plane magnetic penetration depth in Sr$_2$RuO$_4$: muon-spin rotation/relaxation study

We report on measurements of the in-plane magnetic penetration depth ($λ_{\rm ab}$) in single crystals of Sr$_2$RuO$_4$ down to $\simeq 0.015$ K by means of muon-spin rotation/relaxation. The linear temperature dependence of $λ^{-2}_{\rm ab}$ for $T\lesssim 0.7$ K suggests the presence of nodes in the superconducting gap. This statement is further substantiated by observation of the Volovik effect, $i.e.$ the reduction of $λ_{ab}^{-2}$ as a function of the applied magnetic field. The experimental zero-field and zero-temperature value of $λ_{\rm ab}=124(3)$ nm agrees with $λ_{\rm ab}\simeq 130$ nm, calculated based on results of electronic structure measurements reported in [Phys. Rev X 9, 021048 (2019)]. Our analysis reveals that a simple nodal superconducting energy gap, described by the lowest possible harmonic of a gap function, does not capture the dependence of $λ_{\rm ab}^{-2}$ on $T$, so the higher angular harmonics of the energy gap function need to be introduced.

cond-mat.supr-con↗

arXiv2023

CeFe$_2$Al$_{10}$: a Correlated Metal with a Fermi Surface Exhibiting Nonmetallic Conduction

Metals can be defined as materials with a Fermi surface or as materials exhibiting metallic conduction (i.e., $\mathrm{d} ρ/ \mathrm{d}T > 0$). Usually, these definitions both hold at low temperatures, such as liquid-helium temperatures, as the Fermi energy is sufficiently larger than the thermal energy. However, they may not both hold in correlated electron systems where the Fermi energy is reduced by renormalization. In this paper, we demonstrate that although the resistivity of CeFe$_2$Al$_{10}$ increases with decreasing temperature below $\sim20$ K, CeFe$_2$Al$_{10}$ is a metal with a Fermi surface. This assertion is based on the observation of Shubnikov--de Haas oscillations and a Hall resistivity that changes sign with the magnetic field, which requires the coexistence of electron and hole carriers. Our analysis of Shubnikov--de Haas and magnetotransport data indicates that the Fermi energies are as small as $\sim$30 K and that, despite the increasing carrier mobility with decreasing temperature as in conventional metals, the loss of thermally excited carriers leads to nonmetallic conduction ($\mathrm{d} ρ/ \mathrm{d}T < 0$) below $\sim20$ K. Furthermore, we investigate how this anomalous metal transforms to a more conventional metal with metallic conduction by the application of high pressure and a high magnetic field. This study illustrates the subtle distinction between semimetals and semiconductors in correlated electron systems. This distinction is relevant to investigations of correlated topological insulators and semimetals.

cond-mat.str-el↗

arXiv2023

Hierarchy of Lifshitz transitions in the surface electronic structure of Sr$_2$RuO$_4$ under uniaxial compression

We report the evolution of the electronic structure at the surface of the layered perovskite Sr$_2$RuO$_4$ under large in-plane uniaxial compression, leading to anisotropic $B_{1g}$ strains of ${\varepsilon_{xx}-\varepsilon_{yy}=-0.9\pm0.1\%}$. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr$_2$RuO$_4$ hosts. From comparison to tight-binding modelling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of states singularities to the Fermi level, in turn paving the way to the possible realisation of rich collective states at the Sr$_2$RuO$_4$ surface.

cond-mat.str-el↗

arXiv2023

Probing momentum-dependent scattering in uniaxially stressed Sr$_2$RuO$_4$ through the Hall effect

Under in-plane uniaxial stress, the largest Fermi surface sheet of the correlated metal Sr$_2$RuO$_4$ undergoes a Lifshitz transition from an electron-like to an open geometry. We investigate the effects of this transition on transport through measurement of the longitudinal resistivity $ρ_{xx}$ and the Hall coefficient $R_\text{H}$. At temperatures where scattering is dominated by electron-electron scattering, $R_\text{H}$ becomes more negative across the Lifshitz transition, opposite to expectations from the change in Fermi surface topology. We show that this change in $R_\text{H}$ is explainable only if scattering changes throughout the Brillouin zone, not just at the point in $k$-space where the Lifshitz transition occurs. In a model of orbital-dependent scattering, the electron-electron scattering rate on sections of Fermi surface with $xy$ orbital weight decreases dramatically. On the other hand, at temperatures where defect scattering dominates $ρ_{xx}$ and $R_\text{H}$ are essentially constant across the Lifshitz transition.

cond-mat.str-el↗