arXiv subjects

Seunghyun Khim

Publications and source records attributed to Seunghyun Khim.

At least 37 records · Page 2Linked to original sources

arXiv2024

Investigation of the hyperfine coupling constant of locally noncentrosymmetric heavy-fermion superconductor CeRh$_{2}$As$_{2}$

We performed $^{75}$As-NMR measurements in $H\parallel ab$ to investigate the normal-state magnetic properties of CeRh$_2$As$_2$, a recently-discovered heavy-fermion superconductor. We compared the NMR Knight shift $K$ with the magnetic susceptibility $χ_{ab}$, and estimated the hyperfine coupling constant $A_{\mathrm{hf}}$ from the slope of the $K-χ$ plot. We observed that the magnitude of $A_{\mathrm{hf},ab}$ at the As(1) site changes at around 20 K owing to emerging the heavy-fermion state, which was also observed in $A_{\mathrm{hf}}$ at the As(2) site and in $H\parallel c$. The sign of $A_{\mathrm{hf},ab}$ at the As(1) site is negative in low temperature. These are important for the analysis of the NMR results of CeRh$_2$As$_2$ in the superconducting state.

cond-mat.supr-con↗

arXiv2024

Decoupling multi-phase superconductivity from normal state ordering in CeRh$_2$As$_2$

CeRh$_2$As$_2$ is a multi-phase superconductor with $T_{\textrm{c}}=0.26\,\textrm{K}$. The two superconducting (SC) phases, SC1 and SC2, observed for a magnetic field $H$ parallel to the $c$ axis of the tetragonal unit cell, have been interpreted as even- and odd-parity SC states, separated by a phase boundary at $μ_{\textrm{0}}H^{*}=4\,\textrm{T}$. Such parity switching is possible due to a strong Rashba spin-orbit coupling at the Ce sites located in locally non-centrosymmetric environments of the globally centrosymmetric lattice. Existence of another ordered state (Phase I) below a temperature $T_{\textrm{0}}\approx0.4\,\textrm{K}$ suggests an alternative interpretation of the $H^{*}$ transition: It separates a mixed SC+I (SC1) and a pure SC (SC2) state. Here, we present a detailed study of higher quality single crystals of CeRh$_2$As$_2$, showing much sharper signatures at $T_{\textrm{c}}=0.31\,\textrm{K}$ and $T_{\textrm{0}}=0.48\,\textrm{K}$. We refine the $T$-$H$ phase diagram of CeRh$_2$As$_2$ and demonstrate that $T_{0}(H)$ and $T_{\textrm{c}}(H)$ lines meet at $μ_{\textrm{0}}H\approx6\,\textrm{T}$, well above $H^{*}$, implying no influence of Phase I on the SC phase switching. A basic analysis with the Ginzburg-Landau theory indicates a weak competition between the two orders.

cond-mat.supr-con↗

arXiv2023

Parity transition of spin-singlet superconductivity using sub-lattice degrees of freedom

Recently, a superconducting (SC) transition from low-field (LF) to high-field (HF) SC states was reported in CeRh$_2$As$_2$, indicating the existence of multiple SC states. It has been theoretically noted that the existence of two Ce sites in the unit cell, the so-called sub-lattice degrees of freedom owing to the local inversion symmetry breaking at the Ce sites, can lead to the appearance of multiple SC phases even under an interaction inducing spin-singlet superconductivity. CeRh$_2$As$_2$ is considered as the first example of multiple SC phases owing to this sub-lattice degree of freedom. However, microscopic information about the SC states has not yet been reported. In this study, we measured the SC spin susceptibility at two crystallographically inequivalent As sites using nuclear magnetic resonance for various magnetic fields. Our experimental results strongly indicate a spin-singlet state in both SC phases. In addition, the antiferromagnetic phase, which appears within the SC phase, only coexists with the LF SC phase; there is no sign of magnetic ordering in the HF SC phase. The present work reveals unique SC properties originating from the locally noncentrosymmetric characteristics.

cond-mat.supr-con↗

arXiv2023

Interaction of in-plane Drude carrier with c-axis phonon in $\rm PdCoO_2$

We performed polarized reflection and transmission measurements on the layered conducting oxide $\rm PdCoO_2$ thin films. For the ab-plane, an optical peak near $Ω$ $\approx$ 750 cm$^{-1}$ drives the scattering rate $γ^{*}(ω)$ and effective mass $m^{*}(ω)$ of the Drude carrier to increase and decrease respectively for $ω$ $\geqq$ $Ω$. For the c-axis, a longitudinal optical phonon (LO) is present at $Ω$ as evidenced by a peak in the loss function Im[$-1/\varepsilon_{c}(ω)$]. Further polarized measurements in different light propagation (q) and electric field (E) configurations indicate that the Peak at $Ω$ results from an electron-phonon coupling of the ab-plane carrier with the c-LO phonon, which leads to the frequency-dependent $γ^{*}(ω)$ and $m^{*}(ω)$. This unusual interaction was previously reported in high-temperature superconductors (HTSC) between a non-Drude, mid-infrared band and a c-LO. On the contrary, it is the Drude carrier that couples in $\rm PdCoO_2$. The coupling between the ab-plane Drude carrier and c-LO suggests that the c-LO phonon may play a significant role in the characteristic ab-plane electronic properties of $\rm PdCoO_2$ including the ultra-high dc-conductivity, phonon-drag, and hydrodynamic electron transport.

cond-mat.mtrl-sci↗

arXiv2023

Non-local electrodynamics in ultra-pure PdCoO$_{2}$

The motion of electrons in the vast majority of conductors is diffusive, obeying Ohm's law. However, the recent discovery and growth of high-purity materials with extremely long electronic mean free paths has sparked interest in non-ohmic alternatives, including viscous and ballistic flow. Although non-ohmic transport regimes have been discovered across a range of materials, including two-dimensional electron gases, graphene, topological semimetals, and the delafossite metals, determining their nature has proved to be challenging. Here, we report on a new approach to the problem, employing broadband microwave spectroscopy of the delafossite metal PdCoO$_{2}$ in three distinct sample geometries that would be identical for diffusive transport. The observed differences, which go as far as differing power laws, take advantage of the hexagonal symmetry of PdCoO$_{2}$. This permits a particularly elegant symmetry-based diagnostic for non-local electrodynamics, with the result favouring ballistic over strictly hydrodynamic flow. Furthermore, it uncovers a new effect for ballistic electron flow, owing to the highly facetted shape of the hexagonal Fermi surface. We combine our extensive dataset with an analysis of the Boltzmann equation to characterize the non-local regime in PdCoO$_{2}$. More broadly, our results highlight the potential of broadband microwave spectroscopy to play a central role in investigating exotic transport regimes in the new generation of ultra-high conductivity materials.

cond-mat.mes-hall↗

arXiv2023

Investigation of Planckian behavior in a high-conductivity oxide: PdCrO$_2$

The layered delafossite metal PdCrO$_2$ is a natural heterostructure of highly conductive Pd layers Kondo coupled to localized spins in the adjacent Mott insulating CrO$_2$ layers. At high temperatures $T$ it has a $T$-linear resistivity which is not seen in the isostructural but non-magnetic PdCoO$_2$. The strength of the Kondo coupling is known, as-grown crystals are extremely high purity and the Fermi surface is both very simple and experimentally known. It is therefore an ideal material platform in which to investigate 'Planckian metal' physics. We do this by means of controlled introduction of point disorder, measurement of the thermal conductivity and Lorenz ratio and studying the sources of its high temperature entropy. The $T$-linear resistivity is seen to be due mainly to elastic scattering and to arise from a sum of several scattering mechanisms. Remarkably, this sum leads to a scattering rate within 10$\%$ of the Planckian value of $k_BT/$$\hbar$.

cond-mat.str-el↗

arXiv2022

Two-dimensional XY-type Magnetic Properties of Locally Noncentrosymmetric Superconductor CeRh$_2$As$_2$

We performed $^{75}$As-NMR measurements to investigate the normal-state magnetic properties of CeRh$_2$As$_2$, a recently-discovered heavy-fermion superconductor. The magnitude and temperature dependence of the Knight shift at the As(2) site indicate easy-plane-type magnetic anisotropy in CeRh$_2$As$_2$. With regard to spin fluctuations, the temperature dependence of the nuclear spin-lattice relaxation rate $1/T_1$ arising from the 4$f$ electrons decreases from high-temperature constant behavior on cooling at $\sim$ 40~K, which is typical behavior of heavy-fermion systems. In addition, $1/T_1$ becomes constant at low temperatures, suggesting spatially two-dimensional antiferromagnetic fluctuations. Two-dimensional magnetic correlations in the real space are quite rare among heavy-fermion superconductors, and they may be a key factor in the unique superconducting multi-phase in CeRh$_2$As$_2$.

cond-mat.supr-con↗

arXiv2022

Low-Temperature Thermal Conductivity of CeRh$_{2}$As$_{2}$

CeRh$_2$As$_2$ is a rare unconventional superconductor ($T_c=0.26$ K) characterized by two adjacent superconducting phases for a magnetic field $H \parallel c$-axis of the tetragonal crystal structure. Antiferromagnetic order, quadrupole-density-wave order ($T_0 = 0.4$ K) and the proximity of this material to a quantum-critical point have also been reported: The coexistence of these phenomena with superconductivity is currently under discussion. Here, we present thermal conductivity and electrical resistivity measurements on a single crystal of CeRh$_2$As$_2$ between 60 mK and 200 K and in magnetic fields ($H \parallel c$) up to 8 T. Our measurements at low $T$ verify the Wiedemann-Franz law within the error bars. The $T$ dependence of the thermal conductivity $κ(T)$ shows a pronounced drop below $T_c$ which is also field dependent and thus interpreted as the signature of superconductivity. However, the large residual resistivity and the lack of sharp anomalies in $κ(T)$ at the expected transition temperatures clearly indicate that samples of much higher purity are required to gain more information about the superconducting gap structure.

cond-mat.supr-con↗

arXiv2022

Ubiquitous enhancement of nematic fluctuations across the phase diagram of iron based superconductors probed by the Nernst effect

The role of nematic fluctuations for unconventional superconductivity has been subject of intense discussions for many years. In iron-based superconductors, the most established probe for electronic-nematic fluctuations, i.e. the elastoresistivity seems to imply that superconductivity is reinforced by electronic-nematic fluctuations, since the elastoresistivity amplitude peaks at or close to optimal $T_C$. However, on the over-doped side of the superconducting dome, the diminishing elastoresistivity suggests a negligible importance in the mechanism of superconductivity. Here we introduce the Nernst coefficient as a genuine probe for electronic nematic fluctuations, and we show that the amplitude of the Nernst coefficient tracks the superconducting dome of two prototype families of iron-based superconductors, namely Rh-doped $BaFe_{2}As_{2}$ and Co-doped $LaFeAsO$. Our data thus provide fresh evidence that in these systems nematic fluctuations foster the superconductivity throughout the phase diagram.

cond-mat.supr-con↗

arXiv2021

Heisenberg spins on an anisotropic triangular lattice: PdCrO2 under uniaxial stress

When Heisenberg spins interact antiferromagnetically on a triangular lattice and nearest-neighbor interactions dominate, the ground state is 120$^{\circ}$ antiferromagnetism. In this work, we probe the response of this state to lifting the triangular symmetry, through investigation of the triangular antiferromagnet PdCrO$_2$ under uniaxial stress by neutron diffraction and resistivity measurements. The periodicity of the magnetic order is found to change rapidly with applied stress; the rate of change indicates that the magnetic anisotropy is roughly forty times the stress-induced bond length anisotropy. At low stress, the incommensuration period becomes extremely long, on the order of 1000 lattice spacings; no locking of the magnetism to commensurate periodicity is detected. Separately, the magnetic structure is found to undergo a first-order transition at a compressive stress of $\sim$0.4 GPa, at which the interlayer ordering switches from a double- to a single-q structure.

cond-mat.str-el↗

arXiv2021

Observation of antiferromagnetic order as odd-parity multipoles inside the superconducting phase in CeRh$_{2}$As$_{2}$

Spatial inversion symmetry in crystal structures is closely related to the superconducting (SC) and magnetic properties of materials. Recently, several theoretical proposals that predict various interesting phenomena caused by the breaking of the local inversion symmetry have been presented. However, experimental validation has not yet progressed owing to the lack of model materials. Here we present evidence for antiferromagnetic (AFM) order in CeRh$_{2}$As$_{2}$ (SC transition temperature $T_{\rm SC} \sim 0.37$~K), wherein the Ce site breaks the local inversion symmetry. The evidence is based on the observation of different extents of broadening of the nuclear quadrupole resonance spectrum at two crystallographically inequivalent As sites. This AFM ordering breaks the inversion symmetry of this system, resulting in the activation of an odd-parity magnetic multipole. Moreover, the onset of antiferromagnetism $T_{\rm N}$ within an SC phase, with $T_{\rm N} < T_{\rm SC}$, is quite unusual in systems wherein superconductivity coexists or competes with magnetism. Our observations show that CeRh$_{2}$As$_{2}$ is a promising system to study how the absence of local inversion symmetry induces or influences unconventional magnetic and SC states, as well as their interaction.

cond-mat.supr-con↗

arXiv2021

Tuneable electron-magnon coupling of ferromagnetic surface states in PdCoO$_2$

Controlling spin wave excitations in magnetic materials underpins the burgeoning field of magnonics. Yet, little is known about how magnons interact with the conduction electrons of itinerant magnets, or how this interplay can be controlled. Via a surface-sensitive spectroscopic approach, we demonstrate a strong and highly-tuneable electron-magnon coupling at the Pd-terminated surface of the delafossite oxide PdCoO$_2$, where a polar surface charge mediates a Stoner transition to itinerant surface ferromagnetism. We show how the coupling can be enhanced 7-fold with increasing surface disorder, and concomitant charge carrier doping, becoming sufficiently strong to drive the system into a polaronic regime, accompanied by a significant quasiparticle mass enhancement. Our study thus sheds new light on electron-magnon interactions in solid-state materials, and the ways in which these can be controlled.

cond-mat.str-el↗

arXiv2021

Low-symmetry non-local transport in microstructured squares of delafossite metals

Intense work studying the ballistic regime of electron transport in two dimensional systems based on semiconductors and graphene had been thought to have established most of the key experimental facts of the field. In recent years, however, new forms of ballistic transport have become accessible in the quasi-two-dimensional delafossite metals, whose Fermi wavelength is a factor of 100 shorter than those typically studied in the previous work, and whose Fermi surfaces are nearly hexagonal in shape, and therefore strongly faceted. This has some profound consequences for results obtained from the classic ballistic transport experiment of studying bend and Hall resistances in mesoscopic squares fabricated from delafossite single crystals. We observe pronounced anisotropies in bend resistances and even a Hall voltage that is strongly asymmetric in magnetic field. Although some of our observations are non-intuitive at first sight, we show that they can be understood within a non-local Landauer-Büttiker analysis tailored to the symmetries of the square/hexagonal geometries of our combined device/Fermi surface system. Signatures of non-local transport can be resolved for squares of linear dimension of nearly 100 $μ$m, approximately a factor of 15 larger than the bulk mean free path of the crystal from which the device was fabricated.

cond-mat.mes-hall↗

arXiv2021

Quasiparticle interference and quantum confinement in a correlated Rashba spin-split 2D electron liquid

Exploiting inversion symmetry breaking (ISB) in systems with strong spin-orbit coupling promises control of spin through electric fields - crucial to achieve miniaturization in spintronic devices. Delivering on this promise requires a two-dimensional electron gas with a spin precession length shorter than the spin coherence length and a large spin splitting so that spin manipulation can be achieved over length scales of nanometers. Recently, the transition metal oxide terminations of delafossite oxides were found to exhibit a large Rashba spin splitting dominated by ISB. In this limit, the Fermi surface exhibits the same spin texture as for weak ISB, but the orbital texture is completely different, raising questions about the effect on quasiparticle scattering. We demonstrate that the spin-orbital selection rules relevant for conventional Rashba system are obeyed as true spin selection rules in this correlated electron liquid and determine its spin coherence length from quasiparticle interference imaging.

cond-mat.mes-hall↗

arXiv2021

Directional ballistic transport in the two-dimensional metal PdCoO2

In an idealized infinite crystal, the material properties are constrained by the symmetries of its unit cell. Naturally, the point-group symmetry is broken by the sample shape of any finite crystal, yet this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from anisotropic Fermi surfaces are needed. Here we show how strongly facetted Fermi surfaces and long quasiparticle mean free paths present in microstructures of PdCoO2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. Bar shaped transport devices narrower than the mean free path are carved from single crystals using focused ion beam (FIB) milling, such that the ballistic charge carriers at low temperatures frequently collide with both sidewalls defining a channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and transverse voltages appear in zero magnetic field. We robustly identify the channel direction as the source of symmetry breaking via ballistic Monte- Carlo simulations and numerical solution of the Boltzmann equation.

cond-mat.mes-hall↗

arXiv2020

In situ modification of delafossite type PdCoO2 bulk single crystal for reversible hydrogen sorption and fast hydrogen evolution

The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm^(-2), accompanied by high long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit reversible hydrogen sorption and desorption, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultra-high conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer

cond-mat.mtrl-sci↗

arXiv2020

$h/e$ Oscillations in Interlayer Transport of Delafossites

Transport of electrons in a bulk metal is usually well captured by their particle-like aspects, while their wave-like nature is commonly harder to observe. Microstructures can be are fully designed to reveal the quantum phase, for example mesoscopic metal rings resembling interferometers. Here we report a new type of phase coherent oscillation of the out-of-plane magnetoresistance in the layered delafossites PdCoO$_2$ and PtCoO$_2$. The oscillation period is equivalent to that determined by the magnetic flux quantum, $h/e$, threading an area defined by the atomic interlayer separation and the sample width. The phase of the electron wave function in these crystals appears remarkably robust over macroscopic length scales exceeding 10$μ$m and persisting up to elevated temperatures of $T$>50K. We show that, while the experimental signal cannot be explained in a standard Aharonov-Bohm analysis, it arises due to periodic field-modulation of the out-of-plane hopping. These results demonstrate extraordinary single-particle quantum coherence lengths in the delafossites, and identify a new form of quantum interference in solids.

cond-mat.mtrl-sci↗

arXiv2019

Effective Spin-1/2 Moments on a Yb$^{3+}$ Triangular Lattice: an ESR Study

We investigated the spin dynamics by electron spin resonance (ESR) of the Yb-based, effective spin-1/2 delafossites NaYbO$_{2}$, AgYbO$_{2}$, LiYbS$_{2}$, NaYbS$_{2}$, and NaYbSe$_{2}$ which all show an absence of magnetic order down to lowest reachable temperatures and thus are prime candidates to host a quantum spin-liquid ground state in the vicinity of long range magnetic order. Clearly resolved ESR spectra allow to obtain well-defined $g$ values which are determined by the crystal field of the distorted octahedral surrounding of the Yb-ions in trigonal symmetry. This local crystal field information provides important input to characterize the effective $S = 1/2$ Kramers doublet as well as the anisotropic exchange coupling between the Yb ions which is crucial for the nature of the groundstate. The ESR linewidth $ΔB$ is characterised by the spin dynamics and is mainly determined by the anisotropic exchange coupling. We discuss and compare $ΔB$ of the above mentioned delafossites focussing on the low temperature behaviour which is dominated by the growing influence of spin correlations.

cond-mat.str-el↗