arXiv subjects

Jaena Park

Publications and source records attributed to Jaena Park.

14 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

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↗

arXiv2025

Terahertz field-induced metastable magnetization near criticality in FePS3

Controlling the functional properties of quantum materials with light has emerged as a frontier of condensed-matter physics, leading to the discovery of various light-induced phases of matter, such as superconductivity, ferroelectricity, magnetism and charge density waves. However, in most cases, the photoinduced phases return to equilibrium on ultrafast timescales after the light is turned off, limiting their practical applications. Here we use intense terahertz pulses to induce a metastable magnetization with a remarkably long lifetime of more than 2.5 milliseconds in the van der Waals antiferromagnet FePS3. The metastable state becomes increasingly robust as the temperature approaches the antiferromagnetic transition point, suggesting that critical order parameter fluctuations play an important part in facilitating the extended lifetime. By combining first-principles calculations with classical Monte Carlo and spin dynamics simulations, we find that the displacement of a specific phonon mode modulates the exchange couplings in a manner that favours a ground state with finite magnetization near the N\'eel temperature. This analysis also clarifies how the critical fluctuations of the dominant antiferromagnetic order can amplify both the magnitude and the lifetime of the new magnetic state. Our discovery demonstrates the efficient manipulation of the magnetic ground state in layered magnets through non-thermal pathways using terahertz light and establishes regions near critical points with enhanced order parameter fluctuations as promising areas to search for metastable hidden quantum states.

cond-mat.mtrl-sci↗

arXiv2025

Two-stage evolution of magnetic correlations in spiral spin liquid material, Ca$_{10}$Cr$_{7}$O$_{28}$

We present an X-band and tunable high-frequency/high-field electron spin resonance (HF-ESR) study of single-crystalline Ca$_{10}$Cr$_{7}$O$_{28}$, which constitutes alternating antiferromagnetic and ferromagnetic kagome bilayers. At high temperatures, a phonon-assisted relaxation process is evoked to account for the pronounced increase of the linewidth in an exchange-narrowing regime ($k_{\rm B}T\gg J$). In contrast, at low temperatures ($k_{\rm B}T\lesssim J$), a power-law behavior in line narrowing is observed. Our data reveal two distinct power-law regimes for the linewidth which crossover at $T^*\approx 7.5$~K. Notably, the intriguing evolution of the ESR linewidth in this alternating kagome bilayer system with opposite sign of exchange interactions highlights distinct spin dynamics compared to those in a uniform kagome antiferromagnet.

cond-mat.str-el↗

arXiv2024

Spontaneous emergence of phonon angular momentum through hybridization with magnons

Chirality, the breaking of improper rotational symmetry, is a fundamental concept spanning diverse scientific domains. In condensed matter physics, chiral phonons, originating from circular atomic motions that carry angular momentum, have sparked intense interest due to their coupling to magnetic degrees of freedom, enabling potential phonon-controlled spintronics. However, modes and their counter-rotating counterparts are typically degenerate at the Brillouin zone center. Selective excitation of a single-handed circulating phonon requires external stimuli that break the degeneracy. Whether energetically nondegenerate circularly polarized phonons can appear spontaneously without structural or external symmetry breaking remains an open question. Here, we demonstrate that nondegenerate elliptically polarized phonon pairs can be induced by coupling to magnons with same helicity in the van der Waals antiferromagnet $\mathrm{FePSe_3}$. We confirm the presence of magnon-phonon hybrids, also known as magnon polarons, which exhibit inherent elliptical polarization with opposite helicities and distinct energies. This nondegeneracy enables their coherent excitation with linearly polarized terahertz pulses, which also endows these rotating modes with chirality. By tuning the polarization of the terahertz drive and measuring phase-resolved polarimetry of the resulting coherent oscillations, we determine the ellipticity and map the trajectory of these hybrid quasiparticles. Our findings establish a general approach to search for intrinsically nondegenerate phonons with angular momentum at the center of the Brillouin zone and introduce a new methodology for characterizing their ellipticity, outlining a roadmap towards chiral-phonon-controlled spintronic functionalities.

cond-mat.mtrl-sci↗

arXiv2024

Exchange striction induced thermal Hall effect in van der Waals antiferromagnet MnPS$_3$

The thermal Hall effect has emerged as an ideal probe for investigating topological phenomena of charge-neutral excitation. Notably, it reveals crucial aspects of spin-lattice couplings that have been difficult to access for decades. However, the exchange striction mechanism from a lattice-induced change in exchange interaction has often been ignored in thermal Hall experiments. MnPS3 can offer a platform to study exchange striction on the thermal Hall effect due to its significant spin-lattice coupling and field-induced non-collinear spin configuration. Our thermal transport data show distinct temperature and field dependence of longitudinal thermal conductivity ($\kappa_{xx}$) and thermal Hall effect ($\kappa_{xy}$). By using detailed theoretical calculation, we found that the inclusion of the exchange striction is essential for a better description of both $\kappa_{xx}$ and $\kappa_{xy}$. Our result demonstrates the importance of the exchange striction mechanism for a complete understanding of the magnon-phonon-driven thermal Hall effect.

cond-mat.str-el↗

arXiv2024

Terahertz Control of Linear and Nonlinear Magno-Phononics

Coherent manipulation of magnetism through the lattice provides unprecedented opportunities for controlling spintronic functionalities on the ultrafast timescale. Such nonthermal control conventionally involves nonlinear excitation of Raman-active phonons which are coupled to the magnetic order. Linear excitation, in contrast, holds potential for more efficient and selective modulation of magnetic properties. However, the linear channel remains uncharted, since it is conventionally considered forbidden in inversion symmetric quantum materials. Here, we harness strong coupling between magnons and Raman-active phonons to achieve both linear and quadratic excitation regimes of magnon-polarons, magnon-phonon hybrid quasiparticles. We demonstrate this by driving magnon-polarons with an intense terahertz pulse in the van der Waals antiferromagnet $\mathrm{FePS_3}$. Such excitation behavior enables a unique way to coherently control the amplitude of magnon-polaron oscillations by tuning the terahertz field strength and its polarization. The polarimetry of the resulting coherent oscillation amplitude breaks the crystallographic $C_2$ symmetry due to strong interference between different excitation channels. Our findings unlock a wide range of possibilities to manipulate material properties, including modulation of exchange interactions by phonon-Floquet engineering.

cond-mat.mtrl-sci↗

arXiv2024

Label-free correlative morpho-chemical tomography of 3D kidney mesangial cells

Label-free characterization of biological specimens seeks to supplement existing imaging techniques and avoid the need for contrast agents that can disturb the native state of living samples. Conventional label-free optical imaging techniques are compatible with living samples but face challenges such as poor sectioning capability, fragmentary morphology, and lack chemical specific information. Here, we combined simultaneous label-free autofluorescence multi-harmonic (SLAM) microscopy and gradient light interference microscopy (GLIM) to extract both chemical specific and morphological tomography of 3D cultured kidney mesangial cells. Imaging 3D in vitro kidney models is essential to understand kidney function and pathology. Our correlative approach enables imaging and quantification of these cells to extract both morphology and chemical-specific signals that is crucial for understanding kidney function. In our approach, SLAM offers a nonlinear imaging platform with a single-excitation source to simultaneously acquire autofluorescence (FAD and NAD(P)H), second, and third harmonic signal from the 3D cultured cells. Complementarily, GLIM acquires high-contrast quantitative phase information to quantify structural changes in samples with thickness of up to 250 micron. Our correlative imaging results demonstrate a versatile and hassle-free platform for morpho-chemical cellular tomography to investigate functions such as metabolism and matrix deposition of kidney mesangial cells in 3D under controlled physiological conditions.

physics.optics↗

arXiv2024

Giant Linear Dichroism Controlled by Magnetic Field in FePS$_3$

Magnetic-field control of fundamental optical properties is a crucial challenge in the engineering of multifunctional microdevices. Van der Waals (vdW) magnets retaining a magnetic order even in atomically thin layers, offer a promising platform for hosting exotic magneto-optical functionalities owing to their strong spin-charge coupling. Here, we demonstrate that a giant optical anisotropy can be controlled by magnetic fields in the vdW magnet FePS$_3$. The giant linear dichroism ($\sim$11%), observed below $T_{\text{N}}\!\sim\!120$ K, is nearly fully suppressed in a wide energy range from 1.6 to 2.0 eV, following the collapse of the zigzag magnetic order above 40 T. This remarkable phenomenon can be explained as a result of symmetry changes due to the spin order, enabling minority electrons of Fe$^{2+}$ to hop in a honeycomb lattice. The modification of spin-order symmetry by external fields provides a novel route for controllable anisotropic optical micro-devices.

cond-mat.mtrl-sci↗

arXiv2024

Distinct Optical Excitation Mechanisms of a Coherent Magnon in a van der Waals Antiferromagnet

The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS$_3$ under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a $d$-$d$ transition, we reveal a striking change in the coherent magnon's dependence on the pump polarization, indicating two distinct excitation mechanisms. Our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around sub-gap electronic states.

cond-mat.str-el↗

arXiv2023

Pixelation with concentration-encoded effective photons for molecular optical sectioning microscopy

Quality control in molecular optical sectioning microscopy is indispensable for transforming acquired digital images from qualitative descriptions to quantitative data. Although numerous tools, metrics, and phantoms have been developed, accurate quantitative comparisons of data from different microscopy systems with diverse acquisition conditions remains a challenge. Here, we develop a simple tool based on an absolute measurement of bulk fluorophore solutions with related Poisson photon statistics, to overcome this obstacle. Demonstrated in a prototypical multiphoton microscope, our tool unifies the unit of pixelated measurement to enable objective comparison of imaging performance across different modalities, microscopes, components/settings, and molecular targets. The application of this tool in live specimens identifies an attractive methodology for quantitative imaging, which rapidly acquires low signal-to-noise frames with either gentle illumination or low-concentration fluorescence labeling.

physics.optics↗

arXiv2023

Sizable suppression of magnon Hall effect by magnon damping in Cr$_2$Ge$_2$Te$_6$

Two-dimensional (2D) Heisenberg honeycomb ferromagnets are expected to have interesting topological magnon effects as their magnon dispersion can have Dirac points. The Dirac points are gapped with finite second nearest neighbor Dzyaloshinskii-Moriya interaction, providing nontrivial Berry curvature with finite magnon Hall effect. Yet, it is unknown how the topological properties are affected by magnon damping. We report the thermal Hall effect in Cr$_2$Ge$_2$Te$_6$, an insulating 2D honeycomb ferromagnet with a large Dirac magnon gap and significant magnon damping. Interestingly, the thermal Hall conductivity in Cr$_2$Ge$_2$Te$_6$ shows the coexisting phonon and magnon contributions. Using an empirical two-component model, we successfully estimate the magnon contribution separate from the phonon part, revealing that the magnon Hall conductivity was 20 times smaller than the theoretical calculation. Finally, we suggest that such considerable suppression in the magnon Hall conductivity is due to the magnon damping effect in Cr$_2$Ge$_2$Te$_6$.

cond-mat.str-el↗

arXiv2023

Coherent detection of hidden spin-lattice coupling in a van der Waals antiferromagnet

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin-lattice coupling in a vdW antiferromagnet FePS$_{3}$ that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS$_{3}$ selectively couples to the trigonal distortions through partially filled t$_{2g}$ orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin-lattice coupling in FePS$_3$, but also establish phase-resolved CPS as a tool to investigate hidden interactions.

cond-mat.str-el↗

arXiv2017

Anisotropy governed competition of magnetic phases in the honeycomb quantum magnet Na$_3$Ni$_2$SbO$_6$ studied by dilatometry and high-frequency ESR

Thermodynamic properties as well as low-energy magnon excitations of $S=1$ honeycomb-layered Na$_3$Ni$_2$SbO$_6$ have been investigated by high-resolution dilatometry, static magnetisation, and high-frequency electron spin resonance studies in magnetic fields up to 16 T. At $T_{\rm N}$ = 16.5 K, there is a tricritical point separating two distinct antiferromagnetic phases AF1 and AF2 from the paramagnetic regime. In addition, our data imply short-range antiferromagnetic correlations at least up to $\sim 5\cdot T_{\rm N}$. Well below $T_{\rm N}$, the magnetic field $B_{\rm C1}\approx$ 9.5 T is needed to stabilize AF2 against AF1. The thermal expansion and magnetostriction anomalies at $T_{\rm N}$ and $B_{\rm C1}$ imply significant magnetoelastic coupling, both of which associated with a sign change of $\partial L/\partial B$. The transition at $B_{\rm C1}$ is associated with softening of the antiferromagnetic resonance modes observed in the electron spin resonance spectra. The anisotropy gap $Δ= 360$ GHz implies considerable uniaxial anisotropy. We conclude the crucial role of axial anisotropy favoring the AF1 spin structure over the AF2 one. While the magnetostriction data disprove a simple spin-flop scenario at $B_{\rm C1}$, the nature of a second transition at $B_{\rm C2}\approx$ 13 T remains unclear. Both the sign of the magnetostriction and Grüneisen analysis suggest the short-range correlations at high temperatures to be of AF2-type.

cond-mat.str-el↗