arXiv subjects

S. Khim

Publications and source records attributed to S. Khim.

At least 19 recordsLinked to original sources

arXiv2026

Investigation of CeRh$_2$As$_2$ order parameters via ultrasound propagation anomalies

Unconventional superconductors with nearly degenerate pairing states are rare. CeRh$_2$As$_2$ has recently emerged as one of the few existing multi-phase superconductors. It exhibits a first-order phase transition between two distinct superconducting states when a magnetic field is applied along the crystallographic $c$-axis. While this behavior has been linked to locally broken inversion symmetry, a phase diagram based on a multi-component superconducting order parameter remains a possibility. Furthermore, superconductivity appears to coexist with an ordered state (phase I). Despite being the subject of many studies, little is known about the nature of the order parameters in both superconducting phases and phase I. Here, we use ultrasound-propagation measurements at low temperatures, in high magnetic fields and under hydrostatic pressure to address this issue. Our results strongly suggest that the superconducting order parameter in both phases is single-component, corroborating the role of local non-centrosymmetry in the development of multi-phase superconductivity in CeRh$_2$As$_2$. In addition, analysis of the elastic anomalies within the Landau framework of phase transitions strongly suggests the presence of an incommensurate magnetic order parameter in phase I.

cond-mat.supr-con↗

arXiv2025

The phase diagram of CeRh$_{2}$As$_{2}$ for out-of-plane magnetic field

The heavy-fermion superconductor CeRh$_{2}$As$_{2}$ ($T_{\textrm{c}} = 0.35\, \textrm{K}$) shows two superconducting (SC) phases, SC1 and SC2, when a magnetic field is applied parallel to the $c$ axis of the tetragonal unit cell. All experiments to date indicate that the change in SC order parameter detected at $\mu_{\textrm{0}}H^{*} \approx 4\, \textrm{T}$ is due to strong Rashba spin-orbit coupling at the Ce sites caused by the locally non-centrosymmetric environments of the otherwise globally centrosymmetric crystalline structure. Another phase (phase I) exists in this material below $T_{\textrm{0}} = 0.54\, \textrm{K}$. In a previous specific heat study [K. Semeniuk et al. Phys. Rev. B, $107$, L220504 (2023)] we have shown that phase I persists up to a field $\mu_{\textrm{0}}H_{0} \approx 6\, \textrm{T}$, larger than $H^{*}$. From thermodynamic arguments we expected the phase-I boundary line to cross phase SC2 at a tetracritical point. However, we could not find any signature of the phase-I line inside the SC2 phase and speculated that this was due to the fact that the $T_{0}(H)$ line is almost perpendicular to the $H$ axis and, therefore, invisible to $T$-dependent measurements. This would imply a weak competition between the two order parameters. Here, we report magnetic field dependent measurements of the magnetostriction and ac-susceptibility on high-quality single crystals. We see clear evidence of the singularity at $H_{0}$ inside the SC2 phase and confirm our previous prediction. Furthermore, we observe the transition across the $T^{*}(H)$ line in $T$-dependent specific heat measurements, which show that the $T^{*}(H)$ line is not perpendicular to the field axis, but has a positive slope. Our work supports recent $\mu$SR results which suggest coexistence of phase I with superconductivity.

cond-mat.str-el↗

arXiv2024

Origin of the non-Fermi-liquid behavior in CeRh2As2

Unconventional superconductivity in heavy-fermion systems appears often near magnetic quantum critical points (QCPs). This seems to be the case also for CeRh2As2 (Tc $\approx$ 0.31 K). CeRh2As2 shows two superconducting (SC) phases, SC1 and SC2, for a magnetic field along the c axis of the tetragonal unit cell, but only the SC1 phase is observed for a field along the basal plane. Furthermore, another ordered state (phase-I) is observed below T0 $\approx$ 0.48 K whose nature is still unclear: Thermodynamic and magnetic measurements pointed to a non magnetic multipolar state, but recent $\mu$SR and NQR/NMR experiments have clearly detected antiferromagnetic (AFM) order below T0 . Also, quasi-two-dimensional AFM fluctuations were observed in NMR and neutron-scattering experiments above T0. The proximity of a QCP is indicated by non-Fermi-liquid (NFL) behavior observed above the ordered states in both specific heat $C(T)/T \propto T^{-0.6}$ and resistivity $\rho(T) \propto T^{0.5}$. These T-dependencies are not compatible with any generic AFM QCP. Because of the strong magnetic-field anisotropy of both the SC phase and phase I, it is possible to study a field-induced SC QCP as well a phase-I QCP by varying the angle $\alpha$ between the field and the c axis. Thus, by examining the behavior of the electronic specific-heat coefficient C(T)/T across these QCPs, we can determine which phase is associated with the NFL behavior. Here, we present low-temperature specific-heat measurements taken in a magnetic field as high as 21 T applied at several angles $\alpha$. We observe that the NFL behavior does very weakly depend on the field and on the angle $\alpha$, a result that is at odd with that observations in standard magnetic QCPs. This suggests a nonmagnetic origin of the quantum critical fluctuations.

cond-mat.str-el↗

arXiv2022

Field-angle dependence reveals odd-parity superconductivity in CeRh$_2$As$_2$

CeRh$_2$As$_2$ is an unconventional superconductor with multiple superconducting phases and $T_\mathrm{c} = 0.26$ K. When $H\parallel c$, it shows a field-induced transition at $μ_0H^* = 4$ T from a low-field superconducting state SC1 to a high-field state SC2 with a large critical field of $μ_0H_\mathrm{c2} = 14$ T. In contrast, for $H\perp c$, only the SC1 with $μ_0H_\mathrm{c2} = 2$ T is observed. A simple model based on the crystal symmetry was able to reproduce the phase-diagrams and their anisotropy, identifying SC1 and SC2 with even and odd parity superconducting states, respectively. However, additional orders were observed in the normal state which might have an influence on the change of the superconducting state at $H^*$. Here, we present a comprehensive study of the angle dependence of the upper critical fields using magnetic ac-susceptibility, specific heat and torque on single crystals of CeRh$_2$As$_2$. The experiments show that the state SC2 is strongly suppressed when rotating the magnetic field away from the $c$ axis and it disappears for an angle of 35$^{\circ}$. This behavior agrees perfectly with our extended model of a pseudospin triplet state with $\vec{d}$ vector in the plane and hence allows to nail down that SC2 is indeed the suggested odd-parity state.

cond-mat.supr-con↗

arXiv2022

Conventional type-II superconductivity in locally non-centrosymmetric LaRh$_2$As$_2$ single crystals

We report on the observation of superconductivity in LaRh$_2$As$_2$, which is the analogue without $f$-electrons of the heavy-fermion system with two superconducting phases CeRh$_2$As$_2$. A zero-resistivity transition, a specific-heat jump and a drop in magnetic ac susceptibility consistently point to a superconducting transition at a transition temperature of $T_c = 0.28$\,K. The magnetic field-temperature superconducting phase diagrams determined from field-dependent ac-susceptibility measurements reveal small upper critical fields $μ_{\mathrm{0}}H_{c2} \approx 12$\,mT for $H\parallel ab$ and $μ_{\mathrm{0}}H_{c2} \approx 9$\,mT for $H\parallel c$. The observed $H_{c2}$ is larger than the estimated thermodynamic critical field $H_c$ derived from the heat-capacity data, suggesting that LaRh$_2$A$s_2$ is a type-II superconductor with Ginzburg-Landau parameters $κ^{ab}_{GL} \approx 1.9$ and $κ^{c}_{GL}\approx 2.7$. The microscopic Eliashberg theory indicates superconductivity to be in the weak-coupling regime with an electron-phonon coupling constant $λ_{e-ph} \approx 0.4$. Despite a similar $T_c$ and the same crystal structure as the Ce compound, LaRh$_2$As$_2$ displays conventional superconductivity, corroborating the substantial role of the 4$f$ electrons for the extraordinary superconducting state in CeRh$_2$As$_2$.

cond-mat.supr-con↗

arXiv2021

Possible quadrupole density wave in the superconducting Kondo lattice CeRh2As2

CeRh2As2 has recently been reported to be a rare case of multi-phase unconventional superconductor [S. Khim et al., arXiv:2101.09522] close to a quantum critical point (QCP). Here, we present a comprehensive study of its normal state properties and of the phase (I) below To ~ 0.4 K which preempts superconductivity at Tc = 0.26 K. The 2nd-order phase transition at To presents signatures in specific heat and thermal expansion, but none in magnetization and ac-susceptibility, indicating a non-magnetic origin of phase I. In addition, an upturn of the in-plane resistivity at To points to a gap opening at the Fermi level in the basal plane. Thermal expansion indicates a strong positive pressure dependence of To , dTo/dp = 1.5 K/GPa, in contrast to the strong negative pressure coefficient observed for magnetic order in Ce-based Kondo lattices close to a QCP. Similarly, an in-plane magnetic field shifts To to higher temperatures and transforms phase I into another non-magnetic phase (II) through a 1st-order phase transition at about 9 T. Using renormalized band structure calculations, we found that the Kondo effect (TK ~ 30 K) leads to substantial mixing of the excited crystalline-electric-field (CEF) states into the ground state. This allows quadrupolar degrees of freedom in the resulting heavy bands at the Fermi level which are prone to nesting. The huge sensitivity of the quadrupole moment on hybridization together with nesting would cause an unprecedented case of phase transition into a quadrupole-density-wave (QDW) state at a temperature To << TK , which would explain the nature of phase I and II.

cond-mat.str-el↗

arXiv2021

Field-induced transition from even to odd parity superconductivity in CeRh$_2$As$_2$

We report the discovery of two-phase unconventional superconductivity in CeRh$_2$As$_2$. Using thermodynamic probes, we establish that the superconducting critical field of its high-field phase is as high as 14 T, remarkable in a material whose transition temperature is 0.26 K. Furthermore, a $c$-axis field drives a transition between two different superconducting phases. In spite of the fact that CeRh$_2$As$_2$ is globally centrosymmetric, we show that local inversion-symmetry breaking at the Ce sites enables Rashba spin-orbit coupling to play a key role in the underlying physics. More detailed analysis identifies the transition from the low- to high-field states to be associated with one between states of even and odd parity.

cond-mat.supr-con↗

arXiv2020

Probing spin correlations using angle resolved photoemission in a coupled metallic/Mott insulator system

A nearly free electron metal and a Mott insulating state can be thought of as opposite ends of possibilities for the motion of electrons in a solid. In the magnetic oxide metal PdCrO$_{2}$, these two coexist as alternating layers. Using angle resolved photoemission, we surprisingly find sharp band-like features in the one-electron removal spectral function of the correlated subsystem. We show that these arise because a hole created in the Mott layer moves to and propagates in the metallic layer while retaining memory of the Mott layer's magnetism. This picture is quantitatively supported by a strong coupling analysis capturing the physics of PdCrO$_{2}$ in terms of a Kondo lattice Hamiltonian. Our findings open new routes to use the non-magnetic probe of photoemission to gain insights into the spin-susceptibility of correlated electron systems.

cond-mat.str-el↗

arXiv2020

Controlled introduction of defects to delafossite metals by electron irradiation

The delafossite metals PdCoO$_{2}$, PtCoO$_{2}$ and PdCrO$_{2}$ are among the highest conductivity materials known, with low temperature mean free paths of tens of microns in the best as-grown single crystals. A key question is whether these very low resistive scattering rates result from strongly suppressed backscattering due to special features of the electronic structure, or are a consequence of highly unusual levels of crystalline perfection. We report the results of experiments in which high energy electron irradiation was used to introduce point disorder to the Pd and Pt layers in which the conduction occurs. We obtain the cross-section for formation of Frenkel pairs in absolute units, and cross-check our analysis with first principles calculations of the relevant atomic displacement energies. We observe an increase of resistivity that is linear in defect density with a slope consistent with scattering in the unitary limit. Our results enable us to deduce that the as-grown crystals contain extremely low levels of in-plane defects of approximately $0.001\%$. This confirms that crystalline perfection is the most important factor in realizing the long mean free paths, and highlights how unusual these delafossite metals are in comparison with the vast majority of other multi-component oxides and alloys. We discuss the implications of our findings for future materials research.

cond-mat.mtrl-sci↗

arXiv2019

The Fermi surface of PtCoO2 from quantum oscillations and electronic structure calculations

The delafossite series of layered oxides include some of the highest conductivity metals ever discovered. Of these, PtCoO2, with a room temperature resistivity of 1.8 microOhmcm for in-plane transport, is the most conducting of all. The high conduction takes place in triangular lattice Pt layers, separated by layers of Co-O octahedra, and the electronic structure is determined by the interplay of the two types of layer. We present a detailed study of quantum oscillations in PtCoO2, at temperatures down to 35 mK and magnetic fields up to 30 T. As for PdCoO2 and PdRhO2, the Fermi surface consists of a single cylinder with mainly Pt character, and an effective mass close to the free electron value. Due to Fermi-surface warping, two close-lying high frequencies are observed. Additionally, a pronounced difference frequency appears. By analysing the detailed angular dependence of the quantum-oscillation frequencies, we establish the warping parameters of the Fermi surface. We compare these results to the predictions of first-principles electronic structure calculations including spin-orbit coupling on Pt and Co and on-site correlation U on Co, and hence demonstrate that electronic correlations in the Co-O layers play an important role in determining characteristic features of the electronic structure of PtCoO2.

cond-mat.str-el↗

arXiv2019

Perfect separation of intraband and interband excitations in PdCoO$_2$

The temperature dependence of the optical properties of the delafossite PdCoO$_2$ has been measured in the a-b planes over a wide frequency range. The optical conductivity due to the free-carrier (intraband) response falls well below the interband transitions, allowing the plasma frequency to be determined from the $f$-sum rule. Drude-Lorentz fits to the complex optical conductivity yield estimates for the free-carrier plasma frequency and scattering rate. The in-plane plasma frequency has also been calculated using density functional theory. The experimentally-determined and calculated values for the plasma frequencies are all in good agreement; however, at low temperature the optically-determined scattering rate is much larger than the estimate for the transport scattering rate, indicating a strong frequency-dependent renormalization of the optical scattering rate. In addition to the expected in-plane infrared-active modes, two very strong features are observed that are attributed to the coupling of the in-plane carriers to the out-of-plane longitudinal optic modes.

cond-mat.mtrl-sci↗

arXiv2019

Field-induced instability of the quantum-spin-liquid ground state in the $J_{\rm eff}=\frac{1}{2}$ triangular-lattice compound NaYbO$_2$

Polycrystalline samples of NaYbO$_2$ are investigated by bulk magnetization and specific-heat measurements, as well as by nuclear magnetic resonance (NMR) and electron spin resonance (ESR) as local probes. No signatures of long-range magnetic order are found down to 0.3~K, evidencing a highly frustrated spin-liquid-like ground state in zero field. Above 2\,T, signatures of magnetic order are observed in thermodynamic measurements, suggesting the possibility of a field-induced quantum phase transition. The $^{23}$Na NMR relaxation rates reveal the absence of magnetic order and persistent fluctuations down to 0.3~K at very low fields and confirm the bulk magnetic order above 2~T. The $H$-$T$ phase diagram is obtained and discussed along with the existing theoretical concepts for layered spin-$\frac{1}{2}$ triangular-lattice antiferromagnets

cond-mat.str-el↗

arXiv2018

Increasing stripe-type fluctuations in $A$Fe$_{2}$As$_{2}$ ($A$ = K, Rb, Cs) superconductors probed by $^{75}$As NMR spectroscopy

We report $^{75}$As nuclear magnetic resonance measurements on single crystals of RbFe$_{2}$As$_{2}$ and CsFe$_{2}$As$_{2}$. Taking previously reported results for KFe$_{2}$As$_{2}$ into account, we find that the anisotropic electronic correlations evolve towards a magnetic instability in the $A$Fe$_{2}$As$_{2}$ series (with $A$ = K, Rb, Cs). Upon isovalent substitution with larger alkali ions, a drastic enhancement of the anisotropic nuclear spin-lattice relaxation rate and decreasing Knight shift reveal the formation of pronounced spin fluctuations with stripe-type modulation. Furthermore, a decreasing power-law exponent of the nuclear spin-lattice relaxation rate $(1/T_{1})_{H\parallel{ab}}$, probing the in-plane spin fluctuations, evidences an emergent deviation from Fermi-liquid behavior. All these findings clearly indicate that the expansion of the lattice in the $A$Fe$_{2}$As$_{2}$ series tunes the electronic correlations towards a quantum critical point at the transition to a yet unobserved, ordered phase.

cond-mat.str-el↗

arXiv2017

Itinerant ferromagnetism of the Pd-terminated polar surface of PdCoO$_2$

We study the electronic structure of the Pd-terminated surface of the non-magnetic delafossite oxide metal PdCoO$_2$. Combining angle-resolved photoemission spectroscopy and density-functional theory, we show how an electronic reconstruction driven by surface polarity mediates a Stoner-like magnetic instability towards itinerant surface ferromagnetism. Our results reveal how this leads to a rich multi-band surface electronic structure, and provide spectroscopic evidence for an intriguing sample-dependent coupling of the surface electrons to a bosonic mode which we attribute to electron-magnon interactions. Moreover, we find similar surface state dispersions in PdCrO$_2$, suggesting surface ferromagnetism persists in this sister compound despite its bulk antiferromagnetic order.

cond-mat.str-el↗

arXiv2017

Maximal Rashba-like spin splitting via kinetic energy-driven inversion symmetry breaking

Engineering and enhancing inversion symmetry breaking in solids is a major goal in condensed matter physics and materials science, as a route to advancing new physics and applications ranging from improved ferroelectrics for memory devices to materials hosting Majorana zero modes for quantum computing. Here, we uncover a new mechanism for realising a much larger energy scale of inversion symmetry breaking at surfaces and interfaces than is typically achieved. The key ingredient is a pronounced asymmetry of surface hopping energies, i.e. a kinetic energy-driven inversion symmetry breaking, whose energy scale is pinned at a significant fraction of the bandwidth. We show, from spin- and angle-resolved photoemission, how this enables surface states of 3d and 4d-based transition-metal oxides to surprisingly develop some of the largest Rashba-like spin splittings that are known. Our findings open new possibilities to produce spin textured states in oxides which exploit the full potential of the bare atomic spin-orbit coupling, raising exciting prospects for oxide spintronics. More generally, the core structural building blocks which enable this are common to numerous materials, providing the prospect of enhanced inversion symmetry breaking at judiciously-chosen surfaces of a plethora of compounds, and suggesting routes to interfacial control of inversion symmetry breaking in designer heterostructures.

cond-mat.str-el↗

arXiv2017

Single crystal growth, structure and electronic properties of metallic delafossite PdRhO_{2}

We report growth of single crystals of the non-magnetic metallic delafossite PdRhO_{2}, comparing the results from three different methods. Complete crystallographic data were obtained from single crystal X-ray diffraction, and electronic structure calculations made using the refined structural parameters. Focused-ion beam microstructuring was used to prepare a sample for measurements of the in- and out-of-plane electrical resistivity, and the large observed anisotropy is qualitatively consistent with the cylindrical Fermi surface predicted by the calculations.

cond-mat.mes-hall↗

arXiv2016

Experimental realization of type-II Weyl state in non-centrosymmetric TaIrTe$_4$

Recent breakthrough in search for the analogs of fundamental particles in condensed matter systems lead to experimental realizations of 3D Dirac and Weyl semimetals. Weyl state can be hosted either by non-centrosymmetric or magnetic materials and can be of the first or the second type. Several non-centrosymmetric materials have been proposed to be type-II Weyl semimetals, but in all of them the Fermi arcs between projections of multiple Weyl points either have not been observed directly or they were hardly distinguishable from the trivial surface states which significantly hinders the practical application of these materials. Here we present experimental evidence for type-II non-centrosymmetric Weyl state in TaIrTe$_4$ where it has been predicted theoretically. We find direct correspondence between ARPES spectra and calculated electronic structure both in the bulk and the surface and clearly observe the exotic surface states which support the quasi-1D Fermi arcs connecting only four Weyl points. Remarkably, these electronic states are spin-polarized in the direction along the arcs, thus highlighting TaIrTe$_4$ as a novel material with promising application potential.

cond-mat.mes-hall↗

arXiv2016

Interplay of charge density wave and multiband superconductivity in 2$H$-Pd$_x$TaSe$_2$

2$H$-TaSe$_2$ has been one of unique transition metal dichalcogenides exhibiting several phase transitions due to a delicate balance among competing electronic ground states. An unusual metallic state at high-$T$ is sequentially followed by an incommensurate charge density wave (ICDW) state at $\approx$ 122 K and a commensurate charge density wave (CCDW) state at $\approx$ 90 K, and superconductivity at $T_{\rm{C}}\sim$0.14 K. Upon systematic intercalation of Pd ions into TaSe$_2$, we find that CCDW order is destabilized more rapidly than ICDW to indicate a hidden quantum phase transition point at $x$$\sim$0.09-0.10. Moreover, $T_{\rm{C}}$ shows a dramatic enhancement up to 3.3 K at $x$ = 0.08, $\sim$24 times of $T_{\rm{C}}$ in 2$H$-TaSe$_2$, in proportional to the density of states $N(E_F)$. Investigations of upper critical fields $H_{c2}$ in single crystals reveal evidences of multiband superconductivity as temperature-dependent anisotropy factor $γ_H$ = $H_{c2}^{ab}$/$H_{c2}^{c}$, quasi-linear increase of $H_{c2}^{c}(T)$, and an upward, positive-curvature in $H_{c2}^{ab}(T)$ near $T_{\rm{C}}$. Furthermore, analysis of temperature-dependent electronic specific heat corroborates the presence of multiple superconducting gaps. Based on above findings and electronic phase diagram vs $x$, we propose that the increase of $N(E_F)$ and effective electron-phonon coupling in the vicinity of CDW quantum phase transition should be a key to the large enhancement of $T_{\rm{C}}$ in Pd$_x$TaSe$_2$.

cond-mat.supr-con↗