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Seunghyun Khim

Publications and source records attributed to Seunghyun Khim.

At least 19 recordsLinked to original sources

Unconventional superconductivity in locally non-centrosymmetric CeNi$_2$As$_2$

Recent years have seen intense research on heavy fermion superconductivity, inspired by the discovery of multiple superconducting phases in UTe$_\text{2}$ and CeRh$_\text{2}$As$_\text{2}$. In the latter material, two superconducting phases observed under applied magnetic field oriented along the crystallographic $\textit{c}$ direction are associated with local inversion symmetry breaking. To advance understanding of these phenomena, it is highly desirable to find further examples of heavy fermion superconductivity in materials with locally non-centrosymmetric structure. We have succeeded in this quest, by growing single crystals of the CaBe$_\text{2}$Ge$_\text{2}$ isomorph of CeNi$_\text{2}$As$_\text{2}$. The resulting superconductivity brings more than we had foreseen. In addition to providing the opportunity to compare and contrast with that of CeRh$_\text{2}$As$_\text{2}$, the condensation occurs from an incoherent normal state quantitatively similar to that of UBe$_\text{13}$. Our findings therefore raise profound questions not just about superconductivity in the locally non-centrosymmetric structures, but about unconventional superconductivity itself.

cond-mat.supr-con↗

La substitution studies on the heavy-fermion superconductor CeRh$_2$As$_2$

CeRh$_2$As$_2$ has been receiving considerable attention due to its unusual two-phase superconductivity. The superconducting (SC) phase appears at $T_{\mathrm{c}}$ = 0.35 K in an ordered state (phase I) of the Ce-4$f$ moments, which develops below $T_{\mathrm{0}}$ = 0.55 K. The microscopic nature of phase I has not been fully established yet. We report a single-crystal study of the effect of La substitution on these low-temperature phases in Ce$_{1-\textit{x}}$La$_\textit{x}$Rh$_2$As$_2$ up to $x$ = 0.1. The lattice parameters increase monotonically with $x$, corresponding to an effective negative pressure of approximately -0.3 GPa for $x$ = 0.1. While the Ce$^{3+}$ local valence state and the non-Fermi-liquid behavior are preserved, the resistivity coherence maximum $T^{*}_{\mathrm{max}}$ $\approx$ 45 K in the pristine sample shifts to lower temperatures with increasing $x$, indicating a suppression of the Kondo energy scale upon lattice expansion. On the other hand, both $T_{\mathrm{c}}$ and $T_{\mathrm{0}}$ are rapidly suppressed to below 0.1 K for $x$ $>$ 0.05. Notably, such a rapid decrease of $T_{\mathrm{c}}$ under moderate negative pressure is unexpected, but is rather consistent with substitution-induced disorder effect which leads to strong pair breaking in unconventional superconductors. The observed fragility of phase I under both pressure and disorder may imply its itinerant origin.

cond-mat.str-el↗

Thermodynamics of $T_{\rm c}$ suppression in far-overdoped Tl$_2$Ba$_2$CuO$_6$

The physical origin of the suppression of superconductivity with hole doping in overdoped cuprates remains unclear. We measure the electronic specific heat of microgram-scale Tl$_2$Ba$_2$CuO$_6$ crystals and find sharp superconducting anomalies persisting far into the overdoped regime. A weak-coupling BCS-like framework incorporating the known Fermi surface and cation disorder quantitatively reproduces the observed anomalies for $T_{\rm c}=14$-$25$ K and their weak doping dependence. The results show $T_{\rm c}(p)$ to be driven predominantly by a smoothly decreasing pairing strength.

cond-mat.supr-con↗

Non-equilibrium Effects in Vibrational Modes Pumped by Inelastic Tunneling

The properties of strongly correlated electron materials exhibit a surprising sensitivity to small lattice distortions, providing an opportunity for their tuning by selective distortion driving, usually achieved by optical excitations. Using inelastic electron tunneling in scanning tunneling microscopy, we demonstrate that at the surface of a strongly correlated electron material, we can drive vibrational excitations out of equilibrium, by studying the dynamics of localized modes on the Pd-terminated surface of the delafossite oxide PdCrO2. This surface forms a tiling of hydrogen clusters of varying sizes and shapes upon hydrogen adsorption. Our findings reveal that vibrational excitations in the clusters exhibit longer lifetimes than on typical metal surfaces. Detailed analysis of the spectroscopy data reveals signatures of non-equilibrium effects in the excitations which we attribute to the extended lifetimes of these modes. Theoretical calculations support that the long-lived nature of the excitations is related to the unique properties of the substrate.

cond-mat.mtrl-sci↗

Cryogenic focused-ion-beam microstructuring enabling quantitative $c$-axis transport measurements in Tl$_2$Ba$_2$CuO$_{6+δ}$

Absolute transport measurements in correlated quantum materials are often limited by disorder, inhomogeneity, geometric uncertainty, and small crystal size. Focused ion beam (FIB) technology offers a route to overcome many of these limitations by enabling transport devices with precisely defined geometry to be fabricated from lamellae extracted from carefully selected regions of a crystal, but its application to cuprate superconductors has been hindered by ion-beam-induced damage. Here we study the clean overdoped cuprate Tl2201 and show that conventional FIB processing causes thermally driven oxygen loss, while cryogenic FIB microstructuring largely suppresses this degradation and preserves the crystal structure from the bulk to the atomic scale. Microstructured devices quantitatively reproduce established in-plane resistivity and Hall carrier density measurements without rescaling. Applying this approach to $c$-axis transport, we obtain absolute $ρ_c(T)$ values approximately three times larger than previously reported, bringing the transport anisotropy into quantitative agreement with the known Fermi surface geometry within an isotropic relaxation-time approximation. These results resolve a long-standing discrepancy between transport and quantum oscillation measurements in overdoped Tl2201 and establish cryogenic FIB microstructuring as a route to reliable quantitative transport measurements in quantum materials where disorder, inhomogeneity, geometry, or small crystal size have previously limited experimental accuracy.

cond-mat.supr-con↗

Incommensurate modulation with $Q=0$ A-type Antiferromagnetic Order in CeRh$_2$As$_2$ revealed by NQR studies

We performed $^{75}$As nuclear quadrupole resonance (NQR) and nuclear magnetic resonance (NMR) measurements on a higher-quality single-crystalline CeRh$_2$As$_2$, a heavy-fermion superconductor exhibiting multiple superconducting (SC) phases under magnetic fields along the $c$ axis. This SC multiphase is believed to originate from staggered Rashba spin-orbit coupling associated with locally broken inversion symmetry. In addition to superconductivity, CeRh$_2$As$_2$ exhibits phase I below $T_0\sim0.5$ K and an antiferromagnetic (AFM) state below $T_{N}\sim 0.25$ K in the early-stage samples. In the higher-quality sample, the AFM transition becomes more pronounced, and $T_{N}$ increases to nearly coincide with $T_{SC}$. The NQR spectra at the As(1) site imply an internal field with an incommensurate distribution, indicating a two-dimensional incommensurate modulation of the magnetic structure superimposed on a $Q=0$ A-type AFM component. Moreover, a pronounced decrease in the NQR intensity at $T_0$ well-above $T_{N}$ and an abrupt increase in the internal field at $T_{N}$ suggest the emergence of a slowly fluctuating AFM order at $T_0$ which becomes static at $T_{N}$.

cond-mat.supr-con↗

Uniaxial-Stress-Induced Magnetic Transitions in the Triangular-Lattice Antiferromagnet PdCrO2

Uniaxial stress is a promising method to tune magnetic frustration, allowing its effects to be studied in a precise way. In this work, uniaxial stress is applied to the triangular-lattice antiferromagnet PdCrO2. The Cr-Cr magnetic interaction is very sensitive to interatomic separation, so laboratory-achievable stress can induce substantial changes in magnetic structure. Results from three types of measurement are presented: X-ray diffraction, the stress-strain relationship, and neutron diffraction. The combined data show that the elastic moduli of PdCrO2 are strongly affected by stress-induced changes in magnetic structure. A new, first-order stress-induced magnetic transition is observed, at which the lattice constant shrinks by 0.21%. The lattice stiffens dramatically across this transition: the Young's modulus increases by about 80 GPa, and the Poisson ratio falls from about 1 to about 0.4. This stiffening indicates that the magnetic order "locks," that is, becomes insensitive to lattice strain. This locking might occur because the new stress-induced magnetic order nests the Fermi surface of the Pd sheets. Other frustrated magnets, including candidate spin liquids, may show similarly strong coupling between magnetic and elastic degrees of freedom.

cond-mat.str-el↗

Directional ballistic magnetotransport in the delafossite metals PdCoO$_2$ and PtCoO$_2$

Studies of electronic transport in width-restricted channels of PdCoO$_2$ have recently revealed a novel `directional ballistic' regime, in which ballistic propagation of electrons on an anisotropic Fermi surface breaks the symmetries of bulk transport. Here we introduce a magnetic field to this regime, in channels of PdCoO$_2$ and PtCoO$_2$ along two crystallographically distinct directions and over a wide range of widths. We observe magnetoresistance distinct from that in the bulk, with features strongly dependent on channel orientation and becoming more pronounced the narrower the channel. Comparison to semi-classical theory establishes that magnetoresistance arises from field-induced modification of boundary scattering, and helps connect features in the data with specific electronic trajectories. However, the role of bulk scattering in our measurements is yet to be fully understood. Our results demonstrate that finite-size magnetotransport is sensitive to the anisotropy of Fermi surface properties, motivating future work to fully understand and exploit this sensitivity.

cond-mat.mes-hall↗

Basal-plane anisotropy of field-induced multipolar order in tetragonal CeRh$_2$As$_2$

Unconventional superconductivity in Ce-based Kondo-lattice materials emerges almost exclusively in the vicinity of weak dipolar magnetic orders, while higher multipolar orders are only known to occur in a few Pr-based unconventional superconductors and possibly URu$_2$Si$_2$. The multiphase superconductor CeRh$_2$As$_2$ appears to be a notable exception from this trend. Showing clear signatures of magnetism, this tetragonal system is suspected to host a concomitant quadrupolar order, which could be causing the strong enhancement of the ordering temperature when a magnetic field is applied perpendicular to the fourfold ($c$) axis of the lattice. In this work, we show that the field-temperature phase diagram of CeRh$_2$As$_2$ has a remarkable basal-plane anisotropy. This finding supports the scenario of coupled magnetic and multipolar ordering, which may have implications for the pairing mechanism of the superconductivity, and guides the development of the next iteration of theoretical models.

cond-mat.str-el↗

Conventional $s$-wave Superconductivity in LaRh$_2$As$_2$; the Analog without the 4$f$ Electrons of CeRh$_2$As$_2$

Superconductor LaRh$_2$As$_2$ has the same crystal structures as CeRh$_2$As$_2$, which exhibits superconducting (SC) multiphase in the $c$-axis magnetic field. Although the SC transition temperatures $T_c$ are similar, around 0.3 K, LaRh$_2$As$_2$ shows conventional type-II superconductivity with a small upper critical field $H_{c2}\sim$ 10 mT. At present, the SC properties of LaRh$_2$As$_2$ have not been clarified yet. We performed $^{75}$As-nuclear quadrupole resonance (NQR) measurements on LaRh$_2$As$_2$ to investigate the SC properties and gap structure. $1/T_1$ shows a clear coherence peak just below $T_c$ and an exponential decrease at lower temperatures, suggesting full-gap $s$-wave superconductivity. The numerical calculations based on an $s$-wave SC model reveal an SC gap size of $Δ(0)/k_{B}T_{c} \sim 1.48$, consistent with the weak-coupling $s$-wave superconductivity. These results suggest that the 4$f$ electrons in CeRh$_2$As$_2$ not only enhance the orbital limiting field but also contribute to the formation of unconventional superconductivity with SC multiphase.

cond-mat.supr-con↗

Adsorbate-induced formation of a surface-polarity-driven nonperiodic superstructure

The chemical and electronic properties of surfaces and interfaces are important for many technologically relevant processes, be it in information processing, where interfacial electronic properties are crucial for device performance, or in catalytic processes, which depend on the types and densities of active nucleation sites for chemical reactions. Quasi-periodic and nonperiodic crystalline surfaces offer new opportunities because of their inherent inhomogeneity, resulting in localisation and properties vastly different from those of surfaces described by conventional Bravais lattices. Here, we demonstrate the formation of a nonperiodic tiling structure on the surface of the frustrated antiferromagnet PdCrO2 due to hydrogen adsorption. The tiling structure exhibits no long-range periodicity but comprises few-atom hexagonally packed domains covering large terraces. Measurement of the local density of states by tunnelling spectroscopy reveals adsorption-driven modifications to the quasi-2D electronic structure of the surface layer, showing exciting opportunities arising from electron localisation.

cond-mat.mtrl-sci↗

Dichotomy of electron-phonon interactions in the delafossite PdCoO$_2$: From weak bulk to polaronic surface coupling

The metallic delafossites host ultra-high mobility carriers in the bulk, while at their polar surfaces, intrinsic electronic reconstructions stabilise markedly distinct electronic phases, from charge-disproportionated insulators, to Rashba-split heavy-hole gases and ferromagnetic metals. The understanding of these phases has been strongly informed by surface spectroscopic measurements, but previous studies have been complicated by the presence of spatially varying terminations of the material surface. Here, we demonstrate the potential of microscopic-area angle-resolved photoemission to overcome these challenges. Our measurements of the model compound PdCoO$_2$ yield extremely high-quality spectra of the electronic structure, which allows us to place new experimental constraints on the weak electron-phonon coupling in the bulk of PdCoO$_2$, while revealing much stronger interactions at its surfaces. While the CoO$_2$-terminated surface exhibits a conventional weak-coupling behavior, our measurements reveal surprising spectroscopic signatures of polaron formation at the Pd-terminated surface, despite its pronounced metallicity. Together, our findings reveal how mode and symmetry-selective couplings can markedly tune the electron-phonon interactions in a single host material, here opening routes to stabilise surprisingly persistent polaronic quasiparticles.

cond-mat.mtrl-sci↗

Appearance of $c$-axis magnetic moment in odd-parity antiferromagnetic state in CeRh$_2$As$_2$ revealed by $^{75}$As-NMR

CeRh$_2$As$_2$ shows the superconducting (SC) multiphase under the $c$-axis magnetic field, which is considered to originate from local inversion symmetry breaking at the Ce site. We reported that the antiferromagnetic (AFM) order is inside the SC phase and that the AFM state disappears at the transition field to the high-field SC phase. However, the magnetic structure in the AFM state has not been clarified yet. In this study, we performed $^{75}$As-NMR measurements in the SC phase in $H\parallel [110]$ to identify the magnetic structure. Comparing the NMR linewidth with $H \parallel c$, we found that the internal magnetic field is oriented to the $c$ axis. This suggests a $q = 0$ $A$-type AFM with the moments parallel to the $c$ axis. We also observed the reduction of the spin susceptibility, which indicates spin-singlet superconductivity in the low-field SC phase. This study provides an important clue to clarify the correlation between the SC multiphase, magnetism, and local inversion symmetry breaking.

cond-mat.supr-con↗

Exposing the odd-parity superconductivity in CeRh$_2$As$_2$ with hydrostatic pressure

Odd-parity superconductivity is a fundamentally interesting but rare state of matter with a potential for applications in topological quantum computing. Crystals with staggered locally noncentrosymmetric structures have been proposed as platforms where a magnetic field can induce a transition between even- and odd-parity superconducting (SC) states. The strongly correlated superconductor CeRh$_2$As$_2$ with the critical temperature $T_{\mathrm{c}}\approx0.4\,\mathrm{K}$ is likely the first example material showing such a phase transition, which occurs at the magnetic field $μ_{0}H^{*}=4\,\mathrm{T}$ applied along the crystallographic $c$ axis. CeRh$_2$As$_2$ also undergoes a phase transition of an unknown origin at $T_{0}=0.5\,\mathrm{K}$. By subjecting CeRh$_2$As$_2$ to hydrostatic pressure and mapping the resultant changes to the SC phase diagrams we investigated how the lattice compression and changes to the electronic correlations affect the stability and relative balance of the two SC states. The abnormally high in-plane upper critical field becomes even higher close to a quantum critical point of the $T_{0}$ order. Remarkably, the SC phase-switching field $H^{*}$ is drastically reduced under pressure, dropping to $0.3\,\mathrm{T}$ at $2.7\,\mathrm{GPa}$. This result signals an apparent strengthening of the local noncentrosymmetricity and forecasts a possible stabilization of the putative odd-parity state down to zero field, hitherto not considered by theoretical models.

cond-mat.supr-con↗

Pressure-tuned quantum criticality in the locally non-centrosymmetric superconductor CeRh$_2$As$_2$

The unconventional superconductor CeRh$_2$As$_2$ (critical temperature $T_{\mathrm{c}}\approx0.4\,\mathrm{K}$) displays an exceptionally rare magnetic-field-induced transition between two distinct superconducting (SC) phases, proposed to be states of even and odd parity of the SC order parameter, which are enabled by a locally noncentrosymmetric structure. The superconductivity is preceded by a phase transition of unknown origin at $T_{0}\approx0.5\,\mathrm{K}$. Electronic low-temperature properties of CeRh$_2$As$_2$ show pronounced non-Fermi-liquid behavior, indicative of a proximity to a quantum critical point (QCP). The role of quantum fluctuations and normal state orders for the superconductivity in a system with staggered Rashba interaction is currently an open question, pertinent to explaining the occurrence of two-phase superconductivity. In this work, using measurements of resistivity and specific heat under hydrostatic pressure, we show that the $T_{0}$ order vanishes completely at a modest pressure of $P_{0}=0.5\,\mathrm{GPa}$, revealing a QCP. In line with the quantum criticality picture, the linear temperature dependence of the resistivity at $P_{0}$ evolves into a Fermi-liquid quadratic dependence as quantum critical fluctuations are suppressed by increasing pressure. Furthermore, the domelike behavior of $T_{\mathrm{c}}$ around $P_{0}$ implies that the fluctuations of the $T_{0}$ order are involved in the SC pairing mechanism.

cond-mat.str-el↗

Avoided metallicity in a hole-doped Mott insulator on a triangular lattice

Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO$_2$ layer of the delafossite PdCrO$_2$, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.

cond-mat.str-el↗

Coexistence of local magnetism and superconductivity in the heavy-fermion CeRh$_2$As$_2$ revealed by $μ$SR studies

The superconducting (SC) state ($T_\mathrm{c}$ = 0.3 K) of the heavy-fermion compound CeRh$_2$As$_2$, which undergoes an unusual field-induced transition to another high-field SC state, emerges from an unknown ordered state below $T_\mathrm{o}$ = 0.55 K. While an electronic multipolar order of itinerant Ce-4$f$ states was proposed to account for the $T_\mathrm{o}$ phase, the exact order parameter has not been known to date. Here, we report on muon spin relaxation ($μ$SR) studies of the magnetic and SC properties in CeRh$_2$As$_2$ single crystals at low temperatures. We reveal a magnetic origin of the $T_\mathrm{o}$ order by identifying a spontaneous internal field below $T_\mathrm{o}$ = 0.55 K. Furthermore, we find evidence of a microscopic coexistence of local magnetism with bulk superconductivity. Our findings open the possibility that the $T_\mathrm{o}$ phase involves both dipole and higher order Ce-4$f$ moment degrees of freedom and accounts for the unusual non-Fermi liquid behavior.

cond-mat.str-el↗

Optical study on electronic structure of the locally non-centrosymmetric CeRh$_2$As$_2$

The electronic structures of the heavy-fermion superconductor CeRh$_2$As$_2$ with the local inversion symmetry breaking and the reference material LaRh$_2$As$_2$ have been investigated by using experimental optical conductivity ($σ_1(ω)$) spectra and first-principal DFT calculations. In the low-temperature $σ_1(ω)$ spectra of CeRh$_2$As$_2$, a $4f$-conduction electron hybridization and heavy quasiparticles are clearly indicated by a mid-infrared peak and a narrow Drude peak. In LaRh$_2$As$_2$, these features are absent in the $σ_1(ω)$ spectrum, however, it can nicely be reproduced by DFT calculations. For both compounds, the combination between a local inversion symmetry breaking and a large spin-orbit (SO) interaction plays an important role for the electronic structure, however, the SO splitting bands could not be resolved in the $σ_1(ω)$ spectra due to the small SO splitting size.

cond-mat.str-el↗