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S. Nakatsuji

Publications and source records attributed to S. Nakatsuji.

At least 19 recordsLinked to original sources

Uniaxial stress enhanced anisotropic magnetoresistance and superconductivity in the kagome superconductor LaRu$_{3}$Si$_{2}$

Elucidating the role of the kagome electronic structure in determining the various quantum ground states is of fundamental importance. In this work, we employ in-plane uniaxial stress as a tuning parameter to probe the electronic structure and its impact on the superconducting and normal-state properties of the kagome superconductor LaRu$_{3}$Si$_{2}$, combining magnetotransport measurements with first-principles calculations. We identify a pronounced anisotropy in both the upper critical field and the normal-state magnetoresistance, indicating strong electronic anisotropy despite the three-dimensional crystal structure. Furthermore, we find that the superconducting transition temperature $T_{\rm c}$ increases under in-plane stress applied within the kagome plane, although the enhancement is modest, reaching approximately 0.3 K at 0.6 GPa. Furthermore, the absolute magnetoresistance exhibits a pronounced increase from about 22${\%}$ at zero stress to 35${\%}$ at 0.6 GPa, indicating a substantial modification of the normal state above $T_{\rm c}$. Previous studies have reported time-reversal-symmetry (TRS) breaking below a temperature scale that coincides with the onset of magnetoresistance. The simultaneous enhancement of both $T_{\rm c}$ and magnetoresistance under stress therefore suggests a positive correlation between superconductivity and normal-state electronic and magnetic properties in LaRu$_{3}$Si$_{2}$. Detailed calculations demonstrate that stress-induced changes in $T_{\rm c}$ arise from the joint evolution of the total density of states and the flat band, whereas the large magnetoresistance enhancement is dominated by the stress-driven downward shift of the Ru $dz^{2}$ kagome flat band.

cond-mat.supr-con

Dome-Shaped Superconducting Phase Diagram Linked to Charge Order in LaRu$_{3}$Si$_{2}$

The interplay between superconductivity and charge order is a central focus in condensed matter research, with kagome lattice systems offering unique insights. The kagome superconductor LaRu$_{3}$Si$_{2}$ ($T_{\rm c}$ ${\simeq}$ 6.5 K) exhibits a hierarchy of charge order transitions: primary ($T_{\rm co,I}$ ${\simeq}$ 400 K), secondary ($T_{\rm co,II}$ ${\simeq}$ 80 K), and an additional transition at ($T^{*}$ $\simeq$ 35 K). The transitions at $T_{\rm co,II}$ and $T^{*}$ are linked to electronic and magnetic responses as revealed by muon-spin rotation and magnetotransport experiments. However, the connection between superconductivity, charge order, and electronic responses has remained elusive. By employing magnetotransport and X-ray diffraction techniques under pressures of up to 40 GPa, we observe that $T_{\rm c}$ rises to 9 K at 2 GPa, remains nearly constant up to 12 GPa, and then decreases to 2 K at 40 GPa, resulting in a dome-shaped phase diagram. The resistivity anomaly at $T^{*}$ and magnetoresistance also exhibit a similar dome-shaped pressure dependence. Furthermore, we find that charge order transitions from long-range to short-range above 12 GPa, correlating with the suppression of $T_{\rm c}$, suggesting superconductivity is closely tied to the charge-ordered state. Specifically, $T_{\rm c}$ peaks when charge order and the normal-state electronic responses are optimized. In contrast to systems like the cuprates, transition metal dichalcogenides, and other kagome materials, where superconductivity typically competes with charge order, LaRu$_{3}$Si$_{2}$ displays a pronounced interdependence between these two phenomena. This distinctive behavior sheds new light on the connection between superconductivity and charge order, offering avenues for theoretical advancements in understanding superconductivity.

cond-mat.supr-con

Intertwined Charge and Spin Density Waves in a Topological Kagome Material

Using neutrons and x-rays we show the topological kagome antiferromagnet Mn$_3$Sn for $T<285$~K forms a homogeneous spin and charge ordered state comprising a longitudinally polarized spin density wave (SDW) with wavevector $\textbf{k}_β=k_β{\bf \hat{c}}$, a helical modulated version of the room temperature anti-chiral magnetic order with $\textbf{k}_χ=k_χ{\bf \hat{c}}$, and charge density waves with wave vectors $2\textbf{k}_β, 2\textbf{k}_χ$, and $\textbf{k}_β+\textbf{k}_χ$. Though $\textbf{k}_χ$ and $\textbf{k}_β$ coincide for $200~{\rm K}<T<230$~K, they exhibit distinct continuous $T-$dependencies before locking to commensurate values of $\textbf{k}_β = \frac{1}{12}\textbf{c}^{*}$ and $\textbf{k}_χ = \frac{5}{48}\textbf{c}^{*}$ at low$-T$. Density functional theory indicates this complex modulated state may be associated with the nesting of Fermi surfaces from correlated flat kagome bands, which host Weyl nodes that are annihilated as it forms.

cond-mat.str-el

Microscopic study of the impurity effect in the kagome superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$

We report on the effect of magnetic impurities on the microscopic superconducting (SC) properties of the kagome-lattice superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$ using muon spin relaxation/rotation. A strong suppression of the superconducting critical temperature $T_{\rm c}$, the SC volume fraction, and the superfluid density was observed. We further find a correlation between the superfluid density and $T_{\rm c}$ which is considered a hallmark feature of unconventional superconductivity. Most remarkably, measurements of the temperature-dependent magnetic penetration depth $λ$ reveal a change in the low-temperature behavior from exponential saturation to a linear increase, which indicates that Fe doping introduces nodes in the superconducting gap structure at concentrations as low as $x=$~0.015. Our results point to a rare example of unconventional superconductivity in the correlated kagome lattice and accessible tunability of the superconducting gap structure, offering new insights into the microscopic mechanisms involved in superconducting order.

cond-mat.supr-con

Charge orders with distinct magnetic response in a prototypical kagome superconductor LaRu$_{3}$Si$_{2}$

The kagome lattice has emerged as a promising platform for hosting unconventional chiral charge order at high temperatures. Notably, in LaRu$_{3}$Si$_{2}$, a room-temperature charge-ordered state with a propagation vector of ($\frac{1}{4}$,~0,~0) has been recently identified. However, understanding the interplay between this charge order and superconductivity, particularly with respect to time-reversal-symmetry breaking, remains elusive. In this study, we employ single crystal X-ray diffraction, magnetotransport, and muon-spin rotation experiments to investigate the charge order and its electronic and magnetic responses in LaRu$_{3}$Si$_{2}$ across a wide temperature range down to the superconducting state. Our findings reveal the emergence of a charge order with a propagation vector of ($\frac{1}{6}$,~0,~0) below $T_{\rm CO,2}$ ${\simeq}$ 80 K, coexisting with the previously identified room-temperature primary charge order ($\frac{1}{4}$,~0,~0). The primary charge-ordered state exhibits zero magnetoresistance. In contrast, the appearance of the secondary charge order at $T_{\rm CO,2}$ is accompanied by a notable magnetoresistance response and a pronounced temperature-dependent Hall effect, which experiences a sign reversal, switching from positive to negative below $T^{*}$ ${\simeq}$ 35 K. Intriguingly, we observe an enhancement in the internal field width sensed by the muon ensemble below $T^{*}$ ${\simeq}$ 35 K. Moreover, the muon spin relaxation rate exhibits a substantial increase upon the application of an external magnetic field below $T_{\rm CO,2}$ ${\simeq}$ 80 K. Our results highlight the coexistence of two distinct types of charge order in LaRu$_{3}$Si$_{2}$ within the correlated kagome lattice, namely a non-magnetic charge order ($\frac{1}{4}$,~0,~0) below $T_{\rm co,1}$ ${\simeq}$ 400 K and a time-reversal-symmetry-breaking charge order below $T_{\rm CO,2}$.

cond-mat.supr-con

Charge order above room-temperature in a prototypical kagome superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$

The kagome lattice is an intriguing and rich platform for discovering, tuning and understanding the diverse phases of quantum matter, which is a necessary premise for utilizing quantum materials in all areas of modern and future electronics in a controlled and optimal way. The system LaRu$_{3}$Si$_{2}$ was shown to exhibit typical kagome band structure features near the Fermi energy formed by the Ru-$dz^{2}$ orbitals and the highest superconducting transition temperature $T_{\rm c}$ ${\simeq}$ 7K among the kagome-lattice materials. However, the effect of electronic correlations on the normal state properties remains elusive. Here, we report the discovery of charge order in La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$ ($x$ = 0, 0.01, 0.05) beyond room-temperature. Namely, single crystal X-ray diffraction reveals charge order with a propagation vector of ($\frac{1}{4}$,0,0) below $T_{\rm CO-I}$ ${\simeq}$ 400K in all three compounds. At lower temperatures, we see the appearance of a second set of charge order peaks with a propagation vector of ($\frac{1}{6}$,0,0). The introduction of Fe, which is known to quickly suppress superconductivity, does not drastically alter the onset temperature for charge order. Instead, it broadens the scattered intensity such that diffuse scattering appears at the same onset temperature, however does not coalesce into sharp Bragg diffraction peaks until much lower in temperature. Our results present the first example of a charge ordered state at or above room temperature in the correlated kagome lattice with bulk superconductivity.

cond-mat.supr-con

Bond Ordering and Molecular Spin-Orbital Fluctuations in the Cluster Mott Insulator GaTa$_4$Se$_8$

For materials where spin-orbit coupling is competitive with electronic correlations, the spatially anisotropic spin-orbital wavefunctions can stabilize degenerate states that lead to many and diverse quantum phases of matter. Here, we find evidence for a dynamical spin-orbital state preceding a T$^*$=50 K order-disorder spin-orbital ordering transition in the $j\!=\!3/2$ lacunar spinel GaTa$_4$Se$_8$. Above T$^*$, GaTa$_4$Se$_8$ has an average cubic crystal structure, but total scattering measurements indicate local non-cubic distortions of Ta$_4$ tetrahedral clusters for all measured temperatures $2 < T < 300$ K. Inelastic neutron scattering measurements reveal the dynamic nature of these local distortions through symmetry forbidden optical phonon modes that modulate $j\!=\!3/2$ molecular orbital occupation as well as intercluster Ta-Se bonds. Spin-orbital ordering at T$^*$ cannot be attributed to a classic Jahn-Teller mechanism and based on our findings, we propose that intercluster interactions acting on the scale of T$^*$ act to break global symmetry. The resulting staggered intercluster dimerization pattern doubles the unit cell, reflecting a spin-orbital valence bond ground state.

cond-mat.str-el

Piezomagnetic switching of anomalous Hall effect in an antiferromagnet at room temperature

Piezomagnetism couples strain linearly to magnetic order producing magnetization. Thus, unlike magnetostriction, it enables bidirectional control of a net magnetic moment. If this effect becomes large at room temperature, it may be technologically relevant, similar to its electric analogue, piezoelectricity. To date, however, the studies of the piezomagnetic effect have been primarily restricted to antiferromagnetic (AF) insulators at cryogenic temperatures. Here we report the discovery of a large piezomagnetism in a metal at room temperature. Strikingly, by using the AF Weyl semimetal Mn$_3$Sn, known for its nearly magnetization-free anomalous Hall effect (AHE), we find that an application of small uniaxial strain of the order of 0.1 % can control both the sign and size of the AHE. Our experiment and theory show that the piezomagnetism can control the AHE distinctly from the magnetization, which will be useful for spintronics applications.

cond-mat.mtrl-sci

Strong coupling nature of kagome superconductivity in LaRu$_3$Si$_2$

We report muon spin rotation ($μ$SR) experiments together with first-principles calculations on microscopic properties of superconductivity in the kagome superconductor LaRu$_3$Si$_2$ with $T_{\rm c}$ ${\simeq}$ 7K. We find that the calculated normal state band structure features a kagome flat band and Dirac as well as van Hove points formed by the Ru-$dz^2$ orbitals near the Fermi level. Below $T_{\rm c}$, $μ$SR reveals isotropic type-II superconductivity, which is robust against hydrostatic pressure up to 2 GPa. Intriguingly, the ratio 2$Δ/k_{\rm B}T_{\rm c}$ ${\simeq}$ 4.3 (where $Δ$ is the superconducting energy gap) is in the strong coupling limit, and $T_{\rm c}$/$λ_{eff}^{-2}$ (where $λ$ is the penetration depth) is comparable to that of high-temperature unconventional superconductors. We also find that electron-phonon coupling alone can only reproduce small fraction of $T_{\rm c}$ from calculations, which suggests other factors in enhancing $T_{\rm c}$ such as the correlation effect from the kagome flat band, the van Hove point on the kagome lattice, and high density of states from narrow kagome bands. Our experiments and calculations taken together point to strong coupling and the unconventional nature of kagome superconductivity in LaRu$_3$Si$_2$.

cond-mat.supr-con

Monopolar and dipolar relaxation in spin ice Ho$_2$Ti$_2$O$_7$

When degenerate states are separated by large energy barriers, the approach to thermal equilibrium can be slow enough that physical properties are defined by the thermalization process rather than the equilibrium. The exploration of thermalization pushes experimental boundaries and provides refreshing insights into atomic scale correlations and processes that impact steady state dynamics and prospects for realizing solid state quantum entanglement. We present a comprehensive study of magnetic relaxation in Ho$_2$Ti$_2$O$_7$ based on frequency-dependent susceptibility measurements and neutron diffraction studies of the real-time atomic-scale response to field quenches. Covering nearly ten decades in time scales, these experiments uncover two distinct relaxation processes that dominate in different temperature regimes. At low temperatures (0.6K<T<1K) magnetic relaxation is associated with monopole motion along the applied field direction through the spin-ice vacuum. The increase of the relaxation time upon cooling indicates reduced monopole conductivity driven by decreasing monopole concentration and mobility as in a semiconductor. At higher temperatures (1K<T<2K) magnetic relaxation is associated with the reorientation of monopolar bound states as the system approaches the single-spin tunneling regime. Spin fractionalization is thus directly exposed in the relaxation dynamics.

cond-mat.str-el

Antichiral spin order its Goldstone modes and their hybridization with phonons in the topological semimetal Mn3Ge

Quantum materials with strong transport responses to disparate physical quantities are of great fundamental significance and may hold technological potentials. The interplay between interactions and topology drive such responses through the effects of spontaneous symmetry breaking and the associated domain configurations on quantum transport. Here we provide a comprehensive description of the magnetism of Mn3Ge, an antiferromagnetic kagomebased semimetal with room temperature transport anomalies associated with topologically protected Weyl nodes. Using polarized neutron diffraction, we show the all-important magnetic structure is anti-chiral and coplanar carrying the symmetry of a ferromagnet without appreciable magnetization. We probe and classify the long wavelength excitations that determine its macroscopic responses including a set of collective magneto-elastic modes. We develop a phenomenological spin Hamiltonian with exchange, Dzyaloshinskii-Moriya, and crystal field interactions to describe its collective magnetism. The itinerant character of the magnetism that drives quantum transport is apparent in spin wave damping and extended magnetic interactions. Our work provides the scientific basis for manipulation of the chiral antiferromagnetic texture of Mn3Ge to control its topological quantum transport.

cond-mat.str-el

Unconventional free charge in the correlated semimetal Nd2Ir2O7

Nd2Ir2O7 is a correlated semimetal with the pyrochlore structure, in which competing spin-orbit coupling and electron-electron interactions are believed to induce a time-reversal symmetry broken Weyl semimetal phase characterized by pairs of topologically protected Dirac points at the Fermi energy. However, the emergent properties in these materials are far from clear, and exotic new states of matter have been conjectured. Here we demonstrate optically that at low temperatures the free carrier spectral weight is proportional to T^2 where T is the temperature, as expected for massless Dirac electrons. However, we do {\em not} observe the corresponding T^3 term in the specific heat. That the system is not in a Fermi liquid state is further corroborated by the "Planckian" T-linear temperature dependence of the momentum relaxation rate and the progressive opening of a correlation-induced gap at low temperatures. These observations can not be reconciled within the framework of band theory of electron-like quasiparticles and point toward the effective decoupling of the charge transport from the single particle sector.

cond-mat.str-el

Homogenous reduced moment in a gapful scalar chiral kagome antiferromagnet

We present present a quantitative experimental investigation of the scalar chiral magnetic order with in $\rm{Nd_3Sb_3Mg_2O_{14}}$. Static magnetization reveals a net ferromagnetic ground state, and inelastic neutron scattering from the hyperfine coupled nuclear spin reveals a local ordered moment of 1.76(6) $μ_B$, just 61(2)% of the saturated moment size. The experiments exclude static disorder as the source of the reduced moment. A 38(1) $μ$eV gap in the magnetic excitation spectrum inferred from heat capacity rules out thermal fluctuations and suggests a multipolar explanation for the moment reduction. We compare $\rm{Nd_3Sb_3Mg_2O_{14}}$ to Nd pyrochlores and show that it is close to a moment fragmented state.

cond-mat.str-el

Terahertz conductivity of the magnetic Weyl semimetal Mn$_{3}$Sn films

Mn$_{3}$Sn is a non-collinear antiferromagnet which displays a large anomalous Hall effect at room temperature. It is believed that the principal contribution to its anomalous Hall conductivity comes from Berry curvature. Moreover, dc transport and photoemission experiments have confirmed that Mn$_{3}$Sn may be an example of a time-reversal symmetry breaking Weyl semimetal. Due to a small, but finite moment in the room temperature inverse triangular spin structure, which allows control of the Hall current with external field, this material has garnered much interest for next generation memory devices and THz spintronics applications. In this work, we report a THz range study of oriented Mn$_{3}$Sn thin films as a function of temperature. At low frequencies we found the optical conductivity can be well described by a single Drude oscillator. The plasma frequency is strongly suppressed in a temperature dependent fashion as one enters the 260 K helical phase. This may be associated with partial gapping of the Fermi surfaces that comes from breaking translational symmetry along the c-axis. The scattering rate shows quadratic temperature dependence below 200 K, highlighting the possible important role of interactions in this compound.

cond-mat.str-el

Evaluation of spin diffusion length and spin Hall angle of antiferromagnetic Weyl semimetal Mn$_3$Sn

Antiferromagnetic Weyl semimetal Mn$_3$Sn has shown to generate strong intrinsic anomalous Hall effect (AHE) at room temperature, due to large momentum-space Berry curvature from the time-reversal symmetry breaking electronic bands of the Kagome planes. This prompts us to investigate intrinsic spin Hall effect, a transverse phenomenon with identical origin as the intrinsic AHE. We report inverse spin Hall effect experiments in nanocrystalline Mn$_3$Sn nanowires at room temperature using spin absorption method which enables us to quantitatively derive both the spin diffusion length and the spin Hall angle in the same device. We observed clear absorption of the spin current in the Mn$_3$Sn nanowires when kept in contact with the spin transport channel of a lateral spin-valve device. We estimate spin diffusion length $λ_{s(Mn_3Sn)}$ $\sim$0.75 $\pm$0.67 nm from the comparison of spin signal of an identical reference lateral spin valve without Mn$_3$Sn nanowire. From inverse spin Hall measurements, we evaluate spin Hall angle $θ_{SH}$ $\sim$5.3 $\pm$ 2.4 $\%$ and spin Hall conductivity $σ_{SH}$ $\sim$46.9 $\pm$ 3.4 ($\hbar/e$) ($Ω$ cm)$^{-1}$. The estimated spin Hall conductivity agrees with both in sign and magnitude to the theoretically predicted intrinsic $σ_{SH}^{int}$ $\sim$36-96 ($\hbar/e$) ($Ω$ cm)$^{-1}$. We also observed anomalous Hall effect at room temperature in nano-Hall bars prepared at the same time as the spin Hall devices. Large anomalous Hall conductivity along with adequate spin Hall conductivity makes Mn$_3$Sn a promising material for ultrafast and ultrahigh-density spintronics devices.

cond-mat.mes-hall

Discovery of Emergent Photon and Monopoles in a Quantum Spin Liquid

Quantum spin liquid (QSL) is an exotic quantum phase of matter whose ground state is quantum-mechanically entangled without any magnetic ordering. A central issue concerns emergent excitations that characterize QSLs, which are hypothetically associated with quasiparticle fractionalization and topological order. Here we report highly unusual heat conduction generated by the spin degrees of freedom in a QSL state of the pyrochlore magnet Pr$_2$Zr$_2$O$_7$, which hosts spin-ice correlations with strong quantum fluctuations. The thermal conductivity in high temperature regime exhibits a two-gap behavior, which is consistent with the gapped excitations of magnetic ($M$-) and electric monopoles ($E$-particles). At very low temperatures below 200\,mK, the thermal conductivity unexpectedly shows a dramatic enhancement, which well exceeds purely phononic conductivity, demonstrating the presence of highly mobile spin excitations. This new type of excitations can be attributed to emergent photons ($ν$-particle), coherent gapless spin excitations in a spin-ice manifold.

cond-mat.str-el

Kondo hybridization and quantum criticality in $β$-YbAlB$_4$ by laser-ARPES

We report an angle-resolved photoemission (ARPES) study of $β$-YbAlB$_4$, which is known to harbor unconventional quantum criticality (QC) without any tuning. We directly observe a quasiparticle peak (QP), emerging from hybridization, characterized by a binding energy and an onset of coherence both at about 4 meV. This value conforms with a previously observed reduced Kondo scale at about 40 K. Consistency with an earlier study of carriers in $β$-YbAlB$_4$ via the Hall effect strongly suggests that this QP is responsible for the QC in $β$-YbAlB$_4$. A comparison with the sister polymorph $α$-YbAlB$_4$, which is not quantum critical at ambient pressure, further supports this result. Indeed, within the limitation of our instrumental resolution, our ARPES measurements do not show tangible sign of hybridization in this locally isomorphic system, while the conduction band we observe is essentially the same as in $β$-YbAlB$_4$. We therefore claim that we identified by ARPES the carriers responsible for the QC in $β$-YbAlB$_4$. The observed dispersion and the underlying hybridization of this QP are discussed in the context of existing theoretical models.

cond-mat.str-el

Dielectric anomalies and interactions in the 3D quadratic band touching Luttinger semimetal Pr$_2$Ir$_2$O$_7$

Dirac and Weyl semimetals with linearly crossing bands are the focus of much recent interest in condensed matter physics. Although they host fascinating phenomena, their physics can be understood in terms of weakly interacting electrons. In contrast, more than 40 years ago, Abrikosov pointed out that quadratic band touchings are generically strongly interacting. We have performed terahertz spectroscopy on films of the conducting pyrochlore Pr$_2$Ir$_2$O$_7$, which has been shown to host a quadratic band touching. A dielectric constant as large as $\tilde{\varepsilon }/ε_0 \sim 180 $ is observed at low temperatures. In such systems the dielectric constant is a measure of the relative scale of interactions, which are therefore in our material almost two orders of magnitude larger than the kinetic energy. Despite this, the scattering rate exhibits a $T^2$ dependence, which shows that for finite doping a Fermi liquid state survives, however with a scattering rate close to the maximal value allowed.

cond-mat.str-el