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Je-Geun Park

Publications and source records attributed to Je-Geun Park.

At least 19 recordsLinked to original sources

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

We report a systematic study of the composition-dependent bulk properties in $Co_{1/3(1\pmδ)}NbS_{2}$ single crystals across a series of precisely controlled cobalt compositions with -4%<$δ$<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 $δ$=+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 ($γ$) 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 $Co_{1/3(1\pmδ)}NbS_{2}$ 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

Magnetic Field-Tunable Repulsive Exciton-Exciton Interaction in the van der Waals Antiferromagnet NiPS$_3$

Two ultra-narrow absorption peaks around 1.5 eV, which are widely believed to originate from a transition from a spin-orbital entangled triplet to a singlet state, in the two-dimensional van der Waals crystal NiPS$_3$, have attracted considerable attention because of their pronounced spin-dependent character. An interesting question is whether ultrahigh magnetic fields modify an interaction-driven hybridization between those two peaks. In this work we perform systematic magneto-optical measurements of NiPS$_3$ in pulsed magnetic fields of up to 178 T and observe a pronounced mutual repulsion between the two sharp exciton peaks accompanied by a redistribution of oscillator strength, while the band edge shows no detectable field-induced shift within our experimental resolution. We construct a minimal two-level interaction model and compare it semi-quantitatively with the experimental data. Our results reveal a magnetic-field-tunable exciton-exciton coupling as the dominant high-field response of NiPS$_3$, and clarify this material as a new experimental platform for exploring strongly correlated exciton physics in magnetic van der Waals insulators.

cond-mat.str-el

Probing intrinsic magnetic phases in low-dimensional nearly twin-free NiPS$_3$ single crystals

We report the intrinsic thermal and magnetic properties of the low-dimensional van der Waals (vdW) antiferromagnet NiPS$_3$ and explore its emergent magnetic phases by controlling crystallographic twinning. Using nearly twin-free crystals, we resolve intrinsic properties that are typically obscured by multidomain effects in bulk samples. Magnetization results reveal a highly anisotropic, sharp spin-flop transition, confirming the high domain purity of our crystals. Furthermore, high-precision thermodynamic and transport data reveal a broad fluctuation regime around the Néel temperature ($T_{\mathrm{N}}$ = 157.5 K), with a heat capacity anomaly and a concurrent suppression of thermal conductivity. Field-dependent thermal transport shows a small but distinct contribution from spin-lattice coupling, as evidenced by the dip at the spin-flop transition. We develop a theoretical model to explain these properties reported in this paper, with good agreement between experiment and theory. Our work establishes a definitive baseline for bulk properties of NiPS$_3$ and demonstrates the feasibility of resolving intrinsic anisotropies by addressing crystallographic twinning in vdW magnets.

cond-mat.mtrl-sci

Unconventional and Fragile Magnetic Exciton in a van der Waals Quantum Magnet

The recently discovered magnetic exciton in the van der Waals (vdW) antiferromagnet NiPS3 exemplifies these phenomena, exhibiting several distinctive characteristics. Despite extensive investigation, much of its physics remains unresolved, with key questions about why the NiPS3 magnetic exciton is so sharp and optically bright despite the nominally spin-forbidden transition, posing significant challenges to a proper understanding and practical manipulation of the exciton. An urgent question is to what extent it is due to chemical disorder, magnetic weakening, lattice modification, or intrinsic instability of the bright exciton itself: answers to which will put stringent constraints on possible theoretical models. Here we address these questions using hydrostatic pressure as a clean, continuous, reversible, and in-situ tuning parameter. We find that the sharp photoluminescence peak is drastically suppressed by as little as 0.4 GPa and completely quenched by 1.5 GPa, with demonstrating its reversibility. Crucially, this bright-to-dark conversion occurs without magnetic, crystallographic, or electronic reconstruction despite an increase in the Neel temperature, as established by Raman, X-ray absorption, nuclear magnetic resonance spectroscopy, and first-principles many-body calculations. Our results demonstrate that the optical brightness of the magnetic exciton is independent of chemical disorder, lattice expansion, and weakening of magnetic order, indicating that a higher-order correlated mechanism governs the bright exciton. We further propose experimentally constrained microscopic scenarios involving exciton pairing, crystal-field-controlled spin-orbit mixing, and symmetry breaking, providing a framework for future tests of entangled magnetic exciton in correlated quantum magnets.

cond-mat.mtrl-sci

Interfacial chirality-induced magnetic-field-free switching with high energy efficiency in all-vdW heterostructures

Chirality, a central concept across many scientific disciplines, continues to inspire the discovery of novel physical phenomena. In condensed matter physics, structural chirality - defined by the absence of mirror plane symmetries - has primarily been explored in bulk materials. However, new chiral phenomena can emerge uniquely at the interface, distinct from their bulk counterparts, when a chiral material forms a heterostructure. Here, we demonstrate that all van-der-Waals (vdW) heterostructure composed of the chiral Co1/3TaS2 and the achiral vdW ferromagnet Fe3GeTe2 exhibits two distinct and unconventional spin-orbit torques originating from the interfacial chirality. These torques enable magnetic-field-free switching of perpendicular magnetization with ultralow current density ~ 10^6 A/cm^2 and minimal power dissipation < 10^15 W/m^3. Moreover, by replacing Fe3GeTe2 with a similar vdW ferromagnet, Fe3GaTe2, but of higher Curie temperature, we achieved the magnetic-field-free switching at room temperature in the Fe3GaTe2/Co1/3TaS2 vdW heterostructure. Our findings establish interfacial chirality as a powerful new handle for spintronic control, opening a new pathway to explore chirality-induced phenomena beyond the bulk symmetry constraints - and paving the way toward highly efficient, low-power spintronic devices based on all-vdW heterostructures.

cond-mat.mtrl-sci

Microscopic evidence for a Zhang-Rice triplet state in the van der Waals antiferromagnet, NiPS$_3$

Quantum-entangled states underpin many emergent phenomena in quantum materials, yet their direct experimental identification remains a challenge. NiPS$_3$, a van der Waals antiferromagnet exhibiting a resolution-limited magnetic exciton in its ordered phase, has been proposed to host a many-body entangled Zhang-Rice triplet state. Here, using $^{33}$S nuclear magnetic resonance (NMR) on $^{33}$S-enriched NiPS$_3$ single crystals, we provide microscopic evidence for this charge-transfer state. The $^{33}$S and $^{31}$P Knight shifts as a function of temperature reveal a unified spin-triplet configuration arising from strong hybridization between a self-doped hole in the S $3p$ orbitals and a hole in Ni $3d$ orbitals. Furthermore, the $^{33}$S nuclear spin-lattice relaxation rate exhibits a power-law divergence as it approaches the Néel temperature $T_N=155$ K, indicating critical slowing down of collective charge fluctuations consistent with spin-nematic correlations. These results reveal a spin-charge-intertwined ground state and establish the microscopic foundation for the exceptional coherence of the magnetic exciton in NiPS$_3$.

cond-mat.str-el

Coherent terahertz control of metastable magnetization in FePS3

The crystal lattice governs the emergent electronic, magnetic, and optical properties of quantum materials, making structural tuning through strain, pressure, or chemical substitution a key approach for discovering and controlling novel quantum phases. Beyond static modifications, driving specific lattice modes with ultrafast stimuli offers a dynamic route for tailoring material properties out of equilibrium. However, achieving dynamic coherent control of the nonequilibrium phases via resonant excitation of lattice coherences remains largely unexplored. Such manipulation enables non-volatile, on demand amplification and suppression of order parameters on femtosecond timescales, necessary for next generation optoelectronic ultrafast computation. In this study, we demonstrate coherent phononic control of a newly discovered, light-induced metastable magnetization in the van der Waals antiferromagnet FePS3. By using a sequence of terahertz (THz) pulses, we modulate the magnetization amplitude at the frequencies of phonon coherences, whose infrared-active nature and symmetries are further revealed by polarization- and field-strength-dependent measurements. Furthermore, our two-dimensional THz spectroscopy, in tandem with first-principles numerical simulations, shows that these phonons nonlinearly displace a Raman active phonon, which induces the metastable net magnetization. These findings not only clarify the microscopic mechanism underlying the metastable state in FePS3 but also establish vibrational coherences in solids as a powerful tool for ultrafast quantum phase control, enabling manipulation of material functionalities far from equilibrium.

cond-mat.mtrl-sci

Emergent giant topological Hall effect in twisted Fe3GeTe2 metallic system

The topological Hall effect, driven by the exchange interaction between conduction electrons and topological magnetic textures such as skyrmions, is a powerful probe for investigating the topological properties of magnetic materials. Typically, this phenomenon arises in systems with broken global inversion symmetry, where Dzyaloshinskii-Moriya interactions stabilize such textures. Here, we report the discovery of an emergent giant topological Hall effect in the twisted Fe3GeTe2 metallic system, which notably preserves the general global inversion symmetry. This effect manifests exclusively within a narrow window of "magic" twist angles ranging from 0.45° to 0.75°, while it is absent identically outside of that range, highlighting its unique and emergent nature. Micromagnetic simulations reveal that this topological Hall effect originates from a skyrmion lattice induced by alternating in-plane and layer-contrasting Dzyaloshinskii-Moriya interactions that result from local inversion symmetry breaking. Our findings underscore twisted Fe3GeTe2 as a versatile platform for engineering and controlling topological magnetic textures in metallic twisted van der Waals magnets, thereby opening up new avenues for next-generation spintronic devices.

cond-mat.mtrl-sci

Current Switching of Topological Spin Chirality in the van der Waals Antiferromagnet Co1/3TaS2

Magnetic topology is central to modern quantum magnet, where spin chirality governs exotic spin winding, real-space Berry phase, and topological Hall effect. A key unresolved challenge is how to electrically switch topological spin chirality and its associated gauge flux, an essential requirement for manipulating its topological quantum properties. In this work, we propose and experimentally demonstrate the concept of current-switching spin chirality. We identify the new vdW antiferromagnet Co1/3TaS2 as an ideal platform, hosting a topological 3Q state with a minimum chirality cell, an ultrahigh skyrmion density, a non-centrosymmetric geometry, and a strong Berry curvature. We discover intrinsic self-torque-induced chirality switching within Co1/3TaS2, driven purely by current, without the need of heavy metals or a magnetic field, and with high energy efficiency. Our results establish a promising framework for electrically generating and controlling topological spin chirality, and demonstrate a practical route toward chiral spintronics. They can be naturally generalised to other skyrmion systems, offering new opportunities in symmetry control, topological manipulation, and spin-chirality-based quantum functionalities.

cond-mat.mtrl-sci

Van der Waals Antiferromagnets: From Early Discoveries to Future Directions in the 2D Limit

The emergence of a long-range magnetic order in the atomically thin, two-dimensional (2D) limit has long remained a fundamental question in condensed matter physics. The advent of exfoliable van der Waals (vdW) materials, particularly transition-metal phosphorus trisulfides (T MPS3; T M = Fe, Ni, and Mn), provided the first experimental access to this regime and established a foundational platform for investigating 2D magnetism. The 2016 experimental demonstrations of intrinsic magnetism in monolayer FePS3 provided a platform to test key aspects of 2D Ising criticality in the true 2D limit. It was followed by a rapid growth resulting in a wealth of emergent phenomena arising from the interplay of low-dimensional magnetism and quantum materials. We begin this review with the historical development of vdW antiferromagnets and highlight the key physical insights gained over the past decade. We finish with emerging opportunities in which vdW antiferromagnets can serve as versatile platforms for exploring low-dimensional magnetism and its interplay with other quantum degrees of freedom.

cond-mat.mtrl-sci

Emergent Polar Metal Phase in a Van der Waals Mott Magnet

We report the emergence of a two-dimensional (2D) polar metal phase in van der Waals compound FePSe$_3$ under moderate pressures. This layered material is a Mott insulator with antiferromagnetic order under ambient conditions. We show that FePSe$_3$ uniquely allows tuning a 2D correlated insulator into an exotic metal state where a loss of inversion symmetry leads to periodic polar displacements of ions, within a conducting phase - a polar metal. Our combined synchrotron and neutron diffraction data allow us to present a long-sought, unambiguous high-pressure structural model and show the polar displacements of this new phase. We also observe the suppression of magnetic ordering at the insulator-to-metal transition correspondent with this structural change. Our work outlines a comprehensive temperature-pressure phase diagram of FePSe$_3$, combining detailed structural, magnetic and transport data. The high-pressure phase exhibits activated semiconductor behavior at high temperatures, a $T^2$-dependence in its resistivity at lower temperatures - despite the conditions required for a `good metal' Fermi-Liquid description not being met in this case - and a low-temperature resistivity upturn which is suppressed as the system is tuned away from the concomitant transitions. The realisation of a tunable 2D polar metal state in FePSe$_3$ due to the loss of its inversion symmetry combined with pressure-induced metallicity offers a promising new platform to investigate this exotic phase at accessible pressures.

cond-mat.str-el

Viewpoint: On the Emergence of van der Waals Magnets: A Personal Reflection

The observation of magnetism in atomically thin van der Waals (vdW) antiferromagnets (FePS$_3$, NiPS$_3$, and MnPS$_3$) in 2016 marked an important moment in the development of two-dimensional (2D) physics. In this personal reflection, I describe how a simple question, posed in the early 2010s, motivated experimental efforts that culminated in the demonstration of antiferromagnetic order in monolayer FePS$_3$. Alongside subsequent reports of vdW ferromagnets in 2017, these developments helped establish intrinsic magnetism as a viable degree of freedom in atomically thin materials. I close with personal lessons drawn from this period and a perspective on the opportunities that now shape the field's second decade and beyond.

physics.hist-ph

Dominant Kitaev Interaction and Field-induced Quantum Disordered Phase in the Cobaltate Na$_2$Co$_2$TeO$_6$

The identification of quantum spin liquid phases in Kitaev candidate materials remains a major experimental challenge. Since most Kitaev candidates develop antiferromagnetic (AFM) order at low temperatures, currently there are great interest on the field-induced magnetic disordered phase in these compounds, that are distinct from (partially) polarized states. Recently, a cobaltate Na$_2$Co$_2$TeO$_6$ has emerged as a promising Kitaev candidate with high-spin $t^{5}_{2g}e^2_g$ configuration and spin-orbit entangled $J_{\rm eff} = 1/2$ honeycomb lattice system. There are intensive studies on field-induced magnetic states and phase transitions under in-plane magnetic fields. In this study, we propose an intermediate disordered phase induced by an out-of-plane field along the $c$-axis, through high-field magnetization and magnetocaloric effect measurements. To explain the high-field behavior of Na$_2$Co$_2$TeO$_6$, we develop an effective $K$-$J$-$Γ$-$Γ^{\prime}$ spin model featuring a dominant AFM Kitaev interaction. This framework uncovers an intermediate quantum spin liquid phase, establishing the material as a unique platform for exploring Kitaev physics and field-induced quantum-disordered states.

cond-mat.str-el

AC magnetometry of van der Waals magnets using ultrasensitive Graphene Hall sensors

Probing the dynamical magnetic properties of two-dimensional (2D) materials requires sensitive techniques capable of detecting small magnetic fields from nanoscale samples. We demonstrate quantitative AC and DC magnetometry of a ferromagnetic Fe3-xGeTe2 nanoflakes using ultrasensitive graphene Hall sensors. These devices achieve record-low magnetic field detection noise at both cryogenic and room temperature, enabled by hBN encapsulation, low-resistance fluorographene contacts, and a novel fabrication process. We perform quantitative AC susceptibility measurements up to 1 kHz, resolving both real and imaginary components with nanotesla-scale sensitivity and milliradian phase accuracy, the first such measurement in a van der Waals magnet. Our results establish graphene Hall sensors as a powerful and broadly applicable platform for studying magnetic and superconducting phases near the 2D limit.

cond-mat.mtrl-sci

Magneto-Optical Study of Chiral Magnetic Modes in NiI$_{2}$: Direct Evidence for Kitaev Interactions

Bond-dependent magnetic interactions, particularly those described by the Kitaev model, have emerged as a key pathway toward realizing unconventional magnetic states such as quantum spin liquids and topologically nontrivial excitations, including skyrmions. These interactions frustrate conventional magnetic order and give rise to rich collective behavior that continues to challenge both theory and experiment. While Kitaev physics has been extensively explored in the context of honeycomb magnets, direct evidence for its role in real materials remains scarce. Magnetic van der Waals (vdW) materials have emerged as a versatile platform for exploring low-dimensional electrical, magnetic, and correlated electronic phenomena, and provide a fertile ground for potential applications ranging from spintronics to multiferroic devices and quantum information technologies. Here, we demonstrate, through magneto-transmission, Faraday angle rotation, and magnetic circular dichroism measurements, that the magnetic excitation spectrum of NiI$_2$, a van der Waals multiferroic material, is more accurately captured by a Kitaev-based spin model than by the previously invoked helical spin framework.

cond-mat.str-el

Electrical control of topological 3Q state in intercalated van der Waals antiferromagnet Cox-TaS2

Van der Waals (vdW) magnets have opened a new avenue of opportunities encompassing various interesting phases. Co1/3TaS2-an intercalated metallic vdW antiferromagnet-is one of the latest additions to this growing list of materials due to its unique topologically nontrivial triple-Q (3Q) ground state. This 3Q tetrahedral structure, which critically depends on the Co content, yields the highest-density Skyrmion lattice with scalar spin chirality, resulting in a noticeable anomalous Hall effect. In this work, we demonstrate control of this topological phase via ionic gating. Using four CoxTaS2 devices with different Co compositions, we show that ionic gating can cover the entire 3Q topological phase and reveal the nature of the thermodynamically inaccessible phase space. Another striking finding in our data is the existence of an adiabatic discontinuity in the phase boundary between the 3Q and 1Q phases. Our work constitutes one of the first examples of electrical control of scalar spin chirality using an antiferromagnetic metal.

cond-mat.mtrl-sci

Spin dynamics of triple-Q magnetic orderings in a triangular lattice: Implications for multi-Q orderings in general two-dimensional lattices

Multi-Q magnetic structures on two-dimensional (2D) lattices provide a key route to realizing topological physics in 2D magnetism. A major experimental challenge is to unambiguously confirm their formation by excluding the possibility of topologically trivial multi-domain single- or double-Q magnetic orders, which cannot be distinguished using conventional diffraction techniques. Here, we propose that long-wavelength spin dynamics offers a universal diagnostic for triangular lattices: triple-Q orders that preserve rotational symmetry and single- or double-Q orders that break it exhibit qualitatively distinct anisotropies in their Goldstone mode velocities, stemming from fundamental differences in their underlying spin configurations. We validate this concept using the metallic triangular lattice antiferromagnet Co$_{0.325}$TaS$_{2}$, which hosts both a stripe-type single-Q state and a triple-Q tetrahedral ordering at different temperatures. Using inelastic neutron scattering (INS) and spin dynamics simulations, we first refine the spin Hamiltonian by fitting the paramagnetic excitation spectra, allowing us to develop an unbiased model independent of magnetic ordering. We then show that the observed velocity profiles of the Goldstone modes agree with the high-temperature model's predictions: markedly anisotropic for the single-Q phase and near isotropic for the triple-Q phase. Importantly, this contrast persists across various exchange parameters, highlighting its model-independent nature and suggesting potential applicability to other 2D lattice systems. This work provides universal insight into the dynamical properties of topological multi-Q magnetic orderings in 2D lattice structures, offering a broadly applicable diagnostic to distinguishing them from topologically trivial single- or double-Q counterparts. (For the full abstract, please refer to the manuscript)

cond-mat.str-el

Tunable chiral and nematic states in the triple-Q antiferromagnet Co$_{1/3}$TaS$_2$

Complex spin configurations in magnetic materials, ranging from collinear single-Q to noncoplanar multi-Q states, exhibit rich symmetry and chiral properties. However, their detailed characterization is often hindered by the limited spatial resolution of neutron diffraction techniques. Here we employ magnetic circular dichroism (MCD) and magnetic linear dichroism (MLD) to investigate the triangular lattice antiferromagnet Co$_{1/3}$TaS$_2$, revealing three-state (Z3) nematicity and also spin chirality across its multi-Q magnetic phases. At intermediate temperatures, the presence of MLD identifies nematicity arising from a single-Q stripe phase, while at high magnetic fields and low temperatures, a phase characterized solely by MCD emerges, signifying a purely chiral non-coplanar triple-Q state. Notably, at low temperatures and small fields, we discover a unique phase where both chirality and nematicity coexist. A theoretical analysis based on a continuous multi-Q manifold captures the emergence of these distinct magnetic phases, as a result of the interplay between four-spin interactions and weak magnetic anisotropy. Additionally, MCD and MLD microscopy spatially resolves the chiral and nematic domains. Our findings establish Co$_{1/3}$TaS$_2$ as a rare platform hosting diverse multi-Q states with distinct combinations of spin chirality and nematicity while demonstrating the effectiveness of polarized optical techniques in characterizing complex magnetic textures.

cond-mat.str-el