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Kee Hoon Kim

Publications and source records attributed to Kee Hoon Kim.

At least 19 recordsLinked to original sources

Composition-dependent bulk properties of intercalated transition metal dichalcogenides $Co_{1/3(1\pm\delta)}NbS_{2}$

We report a systematic study of the composition-dependent bulk properties in $Co_{1/3(1\pm\delta)}NbS_{2}$ single crystals across a series of precisely controlled cobalt compositions with -4%<$\delta$<8%. By tuning the cobalt stoichiometry, we find that the topological Hall effect is critically sensitive to the intercalant cobalt composition and is completely suppressed when the cobalt composition exceeds $\delta$=+4%. We observe that the longitudinal conductivity is also strongly influenced by the cobalt composition, reaching its maximum value just before the disappearance of the topological Hall effect. Furthermore, heat capacity measurements reveal distinct Sommerfeld coefficients ($\gamma$) across different compositions, which exhibit a clear linear scaling with the inverse of the ordinary Hall coefficient ($R_H^{-1}$). These results demonstrate that composition tuning in $Co_{1/3(1\pm\delta)}NbS_{2}$ systematically modifies the low-energy electronic degree of freedom, moving beyond a simple dilute impurity picture. Finally, we use the microscopic spin Hamiltonian to explain the stability of experimentally observed M-point modulation vector and the corresponding triple-Q magnetic order. Our findings highlight that the topological properties of this system are highly tunable through precise control of the intercalant concentration, offering a new perspective on the competition between electronic and magnetic orders in intercalated transition-metal dichalcogenides.

cond-mat.mtrl-sci

Tuning magnetic, lattice, and transport properties in CoNb3S6 via Fe doping

We present a comprehensive investigation of the effects of Fe doping on the lattice dynamics, magnetic ordering, and magneto-transport properties of the intercalated van der Waals antiferromagnets Co1-xFexNb3S6 (x = 0.1 and 0.3). Temperature- and polarization-dependent Raman scattering measurements reveal a pronounced blue shift of the 180 cm-1 phonon mode with increasing Fe concentration, indicating enhanced sensitivity of lattice vibrations to Fe-induced structural and mass effects. While the temperature evolution of the phonon modes is dominated by conventional anharmonic phonon softening, subtle anomalies observed near the Néel temperature for x = 0.1 point to weak spin-phonon coupling. Electrical transport and magnetic susceptibility data show clear signatures of the antiferromagnetic phase transitions at TN ~ 20.5-23.7 K for x = 0.1 and TN ~ 32.0 K for x = 0.3. Out-of-plane magnetization measurements reveal hysteretic behavior with two field-induced transitions for x =0.1, which evolve into a single hysteresis loop at x =0.3, signaling a subtle reconstruction of the magnetic ground state. Magneto-transport measurements for x = 0.1 further display a butterfly-shaped hysteretic magnetoresistance and a weak topological Hall effect; however, both features are strongly suppressed at x = 0.3. These results illustrate the critical role of Fe-induced magnetic structure reconstruction in fine-tuning topological and magnetic transport phenomena in intercalated van der Waals antiferromagnets.

cond-mat.mtrl-sci

Spectroscopic Evidence of Competing Diagonal Spin Interactions and Spin Disproportionation in the Bilayer Nickelate La$_3$Ni$_2$O$_7$

A comprehensive spectroscopic map of the electronic, magnetic, and lattice excitations is presented for the bilayer nickelate La$_3$Ni$_2$O$_7$ using Raman scattering at ambient pressure. Upon entering the spin density wave state below 153 K, the $A_{1g}$ channel exhibits an abrupt electronic spectral gap with a clear isosbestic point. In contrast, the $B_{1g}$ and $B_{2g}$ channels are dominated by pronounced two-magnon (2M) excitations, representing an unambiguous signature of incipient Mottness. These 2M signals in both channels constitute direct evidence for two distinct in-plane spin exchange interactions along the Ni-O bonding and its diagonal directions. Calculations based on the spin wave theory further reveal that the 2M mode in the $B_{2g}$ channel arises from the competition between two bond-diagonal antiferromagnetic interactions mediated by nickel $d_{x^2-y^2}$ orbitals. Furthermore, emergent low-energy 2M excitations below 10 meV are found to originate from distinct, weaker spin moments, strongly supporting spin disproportionation. Simultaneously, an anomalous softening of $B_{1g}$ phonons from 280 down to 4.5 K is uncovered, suggesting the presence of an incipient lattice instability leading to checkerboard-type breathing modulations. Collectively, these findings identify a ground state of the bilayer nickelate characterized by competing bond-diagonal interactions, spin disproportionation, and an incipient lattice instability, establishing key ingredients for understanding the mechanism of nickelate superconductivity.

cond-mat.str-el

Orbital-Selective Quasiparticle Depletion across the Density Wave Transition in Trilayer Nickelate La$_4$Ni$_3$O$_{10}$

We investigate the evolution of polarized electronic Raman response in trilayer nickelate La$_4$Ni$_3$O$_{10}$, uncovering a systematic reduction of the incoherent electron continuum across the density wave transition in the $A_{1g}$ and $B_{1g}$ representations. Analysis based on the Fermi surface band curvatures points to quasiparticle coherence in momentum positions with dominant $d_{x^2-y^2}$ orbital character. Our findings establish the symmetry channels and the active role of $d_{x^2-y^2}$ orbitals involved in the density wave formation, offering important insight into the electronic and magnetic correlations in the nickelate.

cond-mat.str-el

Coupling between electrons and charge density wave fluctuation and its possible role in superconductivity

In most of charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-PdxTaSe2. Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields result closely resembling the known values of the superconducting dome. Our results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights on the competing relationship not only for CDW, but also for other competing orders.

cond-mat.supr-con

One-ninth magnetization plateau stabilized by spin entanglement in a kagome antiferromagnet

The spin-1/2 antiferromagnetic Heisenberg model on a Kagome lattice is geometrically frustrated, which is expected to promote the formation of many-body quantum entangled states. The most sought-after among these is the quantum spin liquid phase, but magnetic analogs of liquid, solid, and supersolid phases may also occur, producing fractional plateaus in the magnetization. Here, we investigate the experimental realization of these predicted phases in the Kagome material YCu3(OD)6+xBr3-x (x=0.5). By combining thermodynamic and Raman spectroscopic techniques, we provide evidence for fractionalized spinon excitations and observe the emergence of a 1/9 magnetization plateau. These observations establish YCu3(OD)6+xBr3-x as a model material for exploring the 1/9 plateau phase.

cond-mat.str-el

Fingerprints for anisotropic Kondo lattice behavior in the quasiparticle dynamics of the kagome metal Ni$_3$In

We present a temperature- and polarization-resolved phononic and electronic Raman scattering study in combination with the first-principles calculations on the kagome metal Ni$_3$In with anisotropic transport properties and non-Fermi liquid behavior. At temperatures below 50 K and down to 2 K, several Raman phonon modes, including particularly an interlayer shear mode, exhibit appreciable frequency and linewidth renormalization, reminiscent of the onset of the Kondo screening without an accompanying structural or magnetic phase transition. In addition, a low-energy electronic continuum observed in polarization perpendicular to the kagome planes reveals strong temperature dependence below 50 K, implying thermal depletion of incoherent quasiparticles, while the in-plane continuum remains invariant. These concomitant electronic and phononic Raman signatures suggest that Ni$_3$In undergoes an anisotropic electronic crossover from an incoherent to a coherent Kondo lattice regime below 50 K. We discuss the origin of the anisotropic incoherent-coherent crossover in association with the possible anisotropic Kondo hybridization involving localized Ni-$3d_{xz}$ flat-band electrons.

cond-mat.str-el

Observation of linear magnetoelectric effect in a Dirac magnon antiferromagnet Cu$_3$TeO$_6$

Cu$_3$TeO$_6$, a three-dimensional antiferromagnet forming a unique spin-web lattice of spin-1/2 Cu2+ ions below the Neel temperature T$_N$ = 62 K, has recently been found to exhibit topological Dirac or nodal magnon dispersion. In this study, we report the discovery of the linear magnetoelectric (ME) effects in Cu$_3$TeO$_6$ below TN. Our pyroelectric current measurements at a constant magnetic field (H) reveal a linear increase of electric polarization (P) with H for both P // H and P $\perp$ H configurations; a maximum P // [110] = 20 $μ$C/m$^2$ is obtained at u0H // [1-10] = 14 T, corresponding to a linear ME coefficient 1.8 ps/m. Magnetic point group analysis and Monte-Carlo simulations confirm that finite linear ME coefficients are allowed in the off-diagonal and diagonal ME tensor components, consistent with the magnetic point group of $\bar{3}'$. As the parity-time symmetry can be broken in the presence of H or electric field E in the linear ME materials, we envisage that Cu$_3$TeO$_6$ should exhibit a H- or E-induced transformation in the topological magnon dispersion from a Dirac point/nodal line type into two Weyl point types.

cond-mat.str-el

Pressure-dependent structure of BaZrO$_3$ crystals as determined by Raman Spectroscopy

The structure of dielectric perovskite BaZrO$_3$, long known to be cubic at room temperature without any structural phase transition with variation of temperature, has been recently disputed to have different ground state structures with lower symmetries involving octahedra rotation. The pressure-dependent Raman scattering measurements can identify the hierarchy of energetically-adjacent polymorphs, helping in turn understand its ground state structure at atmospheric pressure. Here, Raman scattering spectra of high-quality BaZrO$_3$ single crystals grown by the optical floating zone method are investigated in a pressure range from 1 atm to 42 GPa. First, based on the analyses of the infrared and Raman spectra measured at the atmosphere, it is found that all observed vibrational modes can be assigned according to the cubic $Pm\bar{3}m$ structure. In addition, by applying pressure, two structural phase transitions are found at 8.4 and 19.2 GPa, one from the cubic to the rhombohedral $R\bar{3}c$ phase and the other from the rhombohedral to the tetragonal $I4/mcm$ phase. Based on the two pressure-induced structural phase transitions, the true ground state structure of BaZrO$_3$ at room temperature and ambient pressure is corroborated to be cubic while the rhombohedral phase is the closest second.

cond-mat.mtrl-sci

Interplay of charge density waves, disorder, and superconductivity in 2$H$-TaSe$_2$ elucidated by NMR

Single crystals of pristine and 6% Pd-intercalated 2H-TaSe$_2$ have been studied by means of $^{77}$Se nuclear magnetic resonance (NMR). The temperature dependence of the $^{77}$Se spectrum, with an unexpected line narrowing upon Pd intercalation, unravels the presence of correlated local lattice distortions far above the transition temperature of the charge density wave (CDW) order, thereby supporting a strong-coupling CDW mechanism in 2H-TaSe$_2$. While, the Knight shift data suggest that the incommensurate CDW transition involves a partial Fermi surface gap opening. As for spin dynamics, the $^{77}$Se spin-lattice relaxation rate $T_1^{-1}$ as a function of temperature shows that a pseudogap behavior dominates the low-energy spin excitations even within the CDW phase, and gets stronger along with superconductivity in the Pd-6% sample. We discuss that CDW fluctuations may be responsible for the pseudogap as well as superconductivity, although the two phenomena are unlikely to be directly linked each other.

cond-mat.str-el

4D visualization of the photoexcited coherent magnon by an X-ray free electron laser

X-ray free electron lasers (XFEL) create femtosecond X-ray pulses with high brightness and high longitudinal coherence allowing to extend X-ray spectroscopy and scattering techniques into the ultrafast time-domain. These X-rays are a powerful probe for studying coherent quasiparticle excitations in condensed matter triggered by an impulsive optical laser pump. However, unlike coherent phonons, other quasiparticles have been rarely observed due to small signal changes and lack of standards for the identification. Here, we exploit resonant magnetic X-ray diffraction using an XFEL to visualize a photoexcited coherent magnon in space and time. Large intensity oscillations in antiferromagnetic and ferromagnetic Bragg reflections from precessing moment are observed in a multiferroic Y-type hexaferrite. The precession trajectory reveals that a large, long-lived, photoinduced magnetic-field changes the net magnetization substantially through the large-amplitude of the magnon. This work demonstrates an efficient XFEL probe for the coherent magnon in the spotlight for opto-spintronics application.

cond-mat.str-el

Magnetic properties of S = 5/2 anisotropic triangular chain Bi3FeMo2O12

Competing magnetic interactions in low-dimensional quantum magnets can lead to the exotic ground state with fractionalized excitations. Herein, we present our results on an S = 5/2 quasi-one-dimensional spin system Bi3FeMo2O12. The structure of Bi3FeMo2O12 consists of very well separated, infinite zig-zag S = 5/2 spin chains. The observation of a broad maximum around 10 K in the magnetic susceptibility suggests the presence of short-range spin correlations. Magnetic susceptibility data do not fit to S=5/2 uniform spin chain model due to the presence of 2nd nearest-neighbor coupling (J2) along with the 1st nearest-neighbor coupling J1 of the zig-zag chain. The electronic structure calculations infer that the value of J1 is comparable with J2 (J2/J1~1.1) with a negligible inter-chain interaction (J'/J ~ 0.01), implying that Bi3FeMo2O12 is a highly frustrated triangular chain system. The absence of magnetic long-range ordering down to 0.2 K is seen in the heat capacity data, despite a relatively large antiferromagnetic Curie-Weiss temperature of -40 K. The magnetic heat capacity follows nearly a linear behavior at low temperatures indicating that the S = 5/2 anisotropic triangular chain exhibits the gapless excitations.

cond-mat.str-el

Nearly room temperature ferromagnetism in pressure-induced correlated metallic state of van der Waals insulator CrGeTe$_3$

A complex interplay of different energy scales involving Coulomb repulsion, spin-orbit coupling and Hund's coupling energy in two-dimensional (2D) van der Waals (vdW) material produces novel emerging physical state. For instance, ferromagnetism in vdW charge transfer insulator CrGeTe$_3$, that provides a promising platform to simultaneously manipulate the magnetic and electrical properties for potential device implementation using few layers thick materials. Here, we show a continuous tuning of magnetic and electrical properties of CrGeTe$_3$ single crystal using pressure. With application of pressure, CrGeTe$_3$ transforms from a FM insulator with Curie temperature, $T_{\rm{C}} \sim $ 66 K at ambient condition to a correlated 2D Fermi metal with $T_{\rm{C}}$ exceeding $\sim$ 250 K. Notably, absence of an accompanying structural distortion across the insulator-metal transition (IMT) suggests that the pressure induced modification of electronic ground states are driven by electronic correlation furnishing a rare example of bandwidth-controlled IMT in a vdW material.

cond-mat.str-el

Possible persistence of multiferroic order down to bilayer limit of van der Waals material NiI$_{2}$

Realizing a state of matter in two dimensions has repeatedly proven a novel route of discovering new physical phenomena. Van der Waals (vdW) materials have been at the center of these now extensive research activities. They offer a natural way of producing a monolayer of matter simply by mechanical exfoliation. This work demonstrates that the possible multiferroic state with coexisting antiferromagnetic and ferroelectric orders possibly persists down to the bilayer flake of NiI$_{2}$. By exploiting the optical second-harmonic generation technique, both magnitude and direction of the ferroelectric order, arising from the cycloidal spin order, are successfully traced. The possible multiferroic state's transition temperature decreases from 58 K for the bulk to about 20 K for the bilayer. Our observation will spur extensive efforts to demonstrate multi-functionality in vdW materials, which have been tried mostly by using heterostructures of singly ferroic ones until now.

cond-mat.mtrl-sci

Tuning the interplay between nematicity and spin fluctuations in Na$_{1-x}$Li$_x$FeAs superconductors

Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and $^{75}$As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na$_{1-x}$Li$_x$FeAs; For $x\leq 0.02$, the nematic transition promotes SFs. In contrast, for $x\geq 0.03$, the system undergoes a non-magnetic phase transition at a temperature $T_0$ into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.

cond-mat.str-el

Contrasting magnetoelectric behavior in multiferroic hexaferrites as understood by crystal symmetry analyses

Magnetoelectric (ME) properties under rotating magnetic field H are comparatively investigated in two representative hexaferrites Y-type Ba0.5Sr1.5Zn2(Fe0.92Al0.08)12O22 and Z-type Ba0.52Sr2.48Co2Fe24O41, both of which have exhibited a similar transverse conical spin structure and giant ME coupling near room temperature. When the external H is rotated clockwise by 2pi, in-plane P vector is rotated clockwise by 2pi in the Y-type hexaferrite and counterclockwise by 4pi in the Z-type hexaferrite. A symmetry-based analysis reveals that the faster and opposite rotation of P vector in the Z-type hexaferrite is associated with the existence of a mirror plane perpendicular to c-axis. Moreover, such a peculiar crystal symmetry also results in contrasting microscopic origins for the spin-driven ferroelectricity; only the inverse DM interaction is responsible for the Y-type hexaferrite while additional p-d hybridization becomes more important in the Z-type hexaferrite. This work demonstrates the importance of the crystal symmetry in the determination of ME properties in the hexaferrites and provides a fundamental framework for understanding and applying the giant ME coupling in various ferrites with hexagonal crystal structure.

cond-mat.mtrl-sci

Observation of new magnetic ground state in frustrated quantum antiferromagnet spin liquid system Cs2CuCl4

Cs2CuCl4 is known to possess a quantum spin liquid phase with antiferromagnetic interaction below 2.8 K. We report the observation of a new metastable magnetic phase of the triangular frustrated quantum spin system Cs2CuCl4 induced by the application of hydrostatic pressure. We measured the magnetic properties of Cs2CuCl4 following the application and release of pressure after 3 days. We observed a previously unknown ordered magnetic phase with a transition temperature of 9 K. Furthermore, the recovered sample with new magnetic ground state possesses an equivalent crystal structure to the uncompressed one with antiferromagnetic quantum spin liquid phase.

cond-mat.str-el

Quantitative measurements of size-dependent magnetoelectric coupling in Fe3O4 nanoparticles

Bulk magnetite (Fe3O4), the loadstone used in magnetic compasses, has been known to exhibit magnetoelectric (ME) properties below ~10 K; however, corresponding ME effects in Fe3O4 nanoparticles have been enigmatic. We investigate quantitatively the ME coupling of spherical Fe3O4 nanoparticles with uniform diameters (d) from 3 to 15 nm embedded in an insulating host, using a sensitive ME susceptometer. The intrinsic ME susceptibility (MES) of the Fe3O4 nanoparticles is measured, exhibiting a maximum value of ~0.6 ps/m at 5 K for d=15 nm. We found that the MES is reduced with reduced d but remains finite until d=~5 nm, which is close to the critical thickness for observing the Verwey transition. Moreover, with reduced diameter, the critical temperature below which the MES becomes conspicuous increased systematically from 9.8 K in the bulk to 19.7 K in the nanoparticles with d=7 nm, reflecting the core-shell effect on the ME properties. These results point to a new pathway for investigating ME effect in various nanomaterials.

cond-mat.str-el