arXiv subjects

Suji Park

Publications and source records attributed to Suji Park.

At least 19 recordsLinked to original sources

arXiv2026

Quasiparticle phono-conversion: filming carriers coalescing into excitons

Condensed matter physics is replete with phenomena involving high-energy free particles coalescing into low-energy bound few-particle states. While the cooling of the individual particles is well understood, the crucial step by which cold free carriers form a bound state remains elusive, involving complex energy and momentum relaxation pathways. Here, by combining ultrafast time- and momentum-resolved photoemission spectroscopy on a monolayer WSe$_2$ with the first-principles excitonic-Bloch equations, we resolve the conversion of initially free electrons and holes at the bandedges into bound excitons. With unprecedented energy resolution, we observe the transient \textit{coexistence} of free-carrier and excitonic bands, accompanied by a transfer of spectral weight between the two. We establish the phononic origin of exciton formation and ascribe this coexistence to a sequential relaxation cascade toward the lowest-energy excitonic states, wherein intermediate states remain weakly populated. The efficiency of this process is controlled by valley multiplicity, large-momentum phonon emission and spin-flip processes. By elucidating how bound states emerge from their elementary constituents, our results point to strategies for engineering exciton formation, with direct implications for optical materials and devices that operate with excitons or free carriers.

cond-mat.mtrl-sci↗

arXiv2026

Proximity-induced charge transfer, strain and magnetic exchange in graphene/CrSBr heterostructure

Stacking van der Waals materials provides a powerful route to engineer emergent electronic and magnetic behaviors through proximity-driven interactions. The graphene/CrSBr heterostructure has emerged as a compelling platform in this frontier, exhibiting exotic macroscopic responses-- including uniaxial surface-plasmon-polariton propagation and an unconventional quantum Hall effect-- indicative of strong interfacial electronic and magnetic coupling. However, a microscopic electronic landscape governing these phenomena has remained elusive. Here, we provide a comprehensive spectroscopic characterization of the graphene/CrSBr interface using a combination of angle-resolved photoemission spectroscopy (ARPES), low-energy electron microscopy (LEEM), and density functional theory. We resolve a massive redistribution of interfacial charge that concurrently hole dopes graphene and populates the quasi-one-dimensional spin-polarized conduction band of CrSBr, resulting insulator-to-metal transition in the interfacial CrSBr layer. Furthermore, electronic structure of CrSBr exhibits strong momentum-dependent renormalization distinct from conventional charge doping, and theoretical modeling supported by Raman spectroscopy points to additional interfacial compressive strain. In addition, ARPES reveals a splitting-like feature in the graphene Dirac cone consistent with spin degeneracy lifting, providing possible evidence of magnetic proximity coupling. These findings provide crucial microscopic insight into the system's optical and transport responses and establish graphene/CrSBr as a versatile platform for charge-transfer control, strain-driven band engineering, magnetic-proximity coupling, and directionally confined excitations for next-generation spintronic and nanophotonic devices.

cond-mat.str-el↗

arXiv2026

Nanoscale Confinement Enhances Ultrafast Demagnetization

Nanoscale miniaturization has revolutionized the field of spintronics by enabling exponential growth in areal bit density. A similar leap is also expected in device speeds through successfully harnessing femtosecond magnetization dynamics. However, combining this with the miniaturization of realistic devices is challenging. To address this, we studied the effect of dimensional confinement on the femtosecond demagnetization of Fe. By gradually increasing the level of confinement while keeping excitation conditions constant, we found that Fe layers thinner than 10 nm exhibit enlarged demagnetization amplitudes, reaching a $\sim75\%$ increase at 2 nm. By combining ultrafast experiments sensitive to the spins, the charge carriers, and the phonons, we establish that this finite$\text{-}$size effect is magnetic in origin and is not phonon$\text{-}$driven. With the support of ab$\text{-}$initio calculations and atomistic spin dynamics simulations, we identify the enhancement effect as due to local weakening of spin order at the Fe$\text{'}$s interface, which becomes significant upon increased confinement.

cond-mat.mes-hall↗

arXiv2026

Equilibrium Stabilization of a Hidden Phase Like Metallic State in 1T-TaS2

Electronic phases that lie outside the equilibrium ground state offer a route to explore competing configurations in correlated materials. In 1T-TaS2, ultrafast excitation accesses a metallic hidden phase that is distinct from the commensurate insulating ground state. Here we use angle-resolved photoemission spectroscopy to show that an equivalent electronic configuration is stabilized in exfoliated intermediate-thickness 1T-TaS2 flakes, where it persists up to room temperature before evolving through a different sequence of electronic transitions. This equilibrium hidden-phase-like state hosts a metallic band with finite Fermi-level spectral weight while retaining the characteristic hybridization gaps associated with the star-of-David band folding. These results establish a platform for controlling competing electronic states in layered materials, with implications for both quantum science and phase change technologies.

cond-mat.str-el↗

arXiv2025

Wigner polarons reveal Wigner crystal dynamics in a monolayer semiconductor

Wigner crystals, lattices made purely of electrons, are a quintessential paradigm of studying correlation-driven quantum phase transitions. Despite decades of research, the internal dynamics of Wigner crystals has remained extremely challenging to access, with most experiments probing only static order or collective motion. Here, we establish monolayer WSe2 as a new materials platform to host zero-field Wigner crystals and then demonstrate that exciton spectroscopy provides a direct means to probe both static and dynamic properties of these electron lattices. We uncover striking optical resonances that we identify as Wigner polarons, quasiparticles formed when the electron lattice is locally distorted by exciton-Wigner crystal coupling. We further achieve all-optical control of spins in the Wigner crystal, directly probing valley-dependent Wigner polaron scattering well above the magnetic ordering temperature and in the absence of any external magnetic field. Finally, we demonstrate optical melting of the Wigner crystal and observe intriguingly different responses of the umklapp (static) and Wigner polaron (dynamic) resonances to optical excitation. Our results open up exciting new avenues for elucidating electron dynamics and achieving ultrafast optical control of interaction-driven quantum phase transitions in strongly correlated electron systems.

cond-mat.mes-hall↗

arXiv2025

Probing Quantum Anomalous Hall States in Twisted Bilayer WSe2 via Attractive Polaron Spectroscopy

Moir\'e superlattices in semiconductors exhibit a rich variety of interaction-induced topological states, including quantum anomalous Hall (QAH) effects. A recent study hinted that twisted WSe2 homobilayer (tWSe2) could host a QAH state but lacked direct evidence of ferromagnetism, a key hallmark of this phase. Here, we report the first direct evidence of QAH states in tWSe2 with spontaneous ferromagnetism. Specifically, we employ polarization-resolved attractive polaron spectroscopy on a dual-gated, 2 degree tWSe2 and observe direct signatures of spontaneous time-reversal symmetry breaking at hole filling \nu = 1. Together with a Chern number measurement via Streda formula analysis, we identify this magnetized state as a topological state, characterized by C = 1. Furthermore, we demonstrate that these topological and magnetic properties are tunable via a finite displacement field, between a QAH ferromagnetic state and an antiferromagnetic state. Our findings position tWSe2 as a highly versatile, stable, and optically addressable platform for investigating topological order and strong correlations in two-dimensional landscapes.

cond-mat.str-el↗

arXiv2025

Quantum confining excitons with electrostatic moir\'e superlattice

Quantum confining excitons has been a persistent challenge in the pursuit of strong exciton interactions and quantum light generation. Unlike electrons, which can be readily controlled via electric fields, imposing strong nanoscale potentials on excitons to enable quantum confinement has proven challenging. In this study, we utilize piezoresponse force microscopy to image the domain structures of twisted hexagonal boron nitride (hBN), revealing evidence of strong in-plane electric fields at the domain boundaries. By placing a monolayer MoSe2 only one to two nanometers away from the twisted hBN interface, we observe energy splitting of neutral excitons and Fermi polarons by several millielectronvolts at the moir\'e domain boundaries. By directly correlating local structural and optical properties, we attribute such observations to excitons confined in a nanoscale one-dimensional electrostatic potential created by the strong in-plane electric fields at the moir\'e domain boundaries. Intriguingly, this 1D quantum confinement results in pronounced polarization anisotropy in the excitons' reflection and emission, persistent to temperatures as high as ~80 Kelvins. These findings open new avenues for exploring and controlling strongly interacting excitons for classical and quantum optoelectronics.

cond-mat.mes-hall↗

arXiv2024

Sub-wavelength optical lattice in 2D materials

Recently, light-matter interaction has been vastly expanded as a control tool for inducing and enhancing many emergent non-equilibrium phenomena. However, conventional schemes for exploring such light-induced phenomena rely on uniform and diffraction-limited free-space optics, which limits the spatial resolution and the efficiency of light-matter interaction. Here, we overcome these challenges using metasurface plasmon polaritons (MPPs) to form a sub-wavelength optical lattice. Specifically, we report a ``non-local" pump-probe scheme where MPPs are excited to induce a spatially modulated AC Stark shift for excitons in a monolayer of MoSe$_2$, several microns away from the illumination spot. Remarkably, we identify nearly two orders of magnitude reduction for the required modulation power compared to the free-space optical illumination counterpart. Moreover, we demonstrate a broadening of the excitons' linewidth as a robust signature of MPP-induced periodic sub-diffraction modulation. Our results will allow exploring power-efficient light-induced lattice phenomena below the diffraction limit in active chip-compatible MPP architectures.

cond-mat.mes-hall↗

arXiv2024

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light-matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean-square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

cond-mat.mtrl-sci↗

arXiv2023

Electrical control and transport of tightly bound interlayer excitons in a MoSe2/hBN/MoSe2 heterostructure

Controlling interlayer excitons in van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe2/hBN/MoSe2 heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ~180 meV through the Stark effect, and exhibit a sizable binding energy of ~81 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding ten micrometers, which can be attributed, in part, to their dipolar repulsive interactions. Spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. The formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.

cond-mat.mes-hall↗

arXiv2023

Chiral Flat-Band Optical Cavity with Atomically Thin Mirrors

A fundamental requirement for photonic technologies is the ability to control the confinement and propagation of light. Widely utilized platforms include two-dimensional (2D) optical microcavities in which electromagnetic waves are confined between either metallic or distributed Bragg reflectors. Recently, transition metal dichalcogenides hosting tightly bound excitons with high optical quality have emerged as promising atomically thin mirrors. In this work, we propose and experimentally demonstrate a sub-wavelength 2D nano-cavity using two atomically thin mirrors with degenerate resonances. Angle-resolved measurements show a flat band, which sets this system apart from conventional photonic cavities. Remarkably, we demonstrate how the excitonic nature of the mirrors enables the formation of chiral and tunable optical modes upon the application of an external magnetic field. Moreover, we show the electrical tunability of the confined mode. Our work demonstrates a mechanism for confining light with high-quality excitonic materials, opening perspectives for spin-photon interfaces, and chiral cavity electrodynamics.

physics.optics↗

arXiv2023

Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

Realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently significant efforts have focused on exploring excitons in solids as a pathway to achieving nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light-matter interactions require large oscillator strength and short radiative lifetime of the excitons, which limits their interaction strength and nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses by exploiting the coupling between excitons and carriers in an atomically thin semiconductor of trilayer tungsten diselenide. By controlling the electric field and electrostatic doping of the trilayer, we observe the hybridization between intralayer and interlayer excitons along with the formation of Fermi polarons due to the interactions between excitons and free carriers. We find substantial optical nonlinearity can be achieved under both continuous wave and pulsed laser excitation, where the resonance of the hole-doped Fermi polaron blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the strong interactions between excitons and free charges with optically induced valley polarization. Our results establish that atomically thin heterostructures are a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics, and open avenues for exploring many-body physics in hybrid Fermionic-Bosonic systems.

cond-mat.mes-hall↗

arXiv2023

Excitation-Dependent High-Lying Excitonic Exchange via Interlayer Energy Transfer from Lower-to-Higher Bandgap 2D Material

High light absorption (~15%) and strong photoluminescence (PL) emission in monolayer (1L) transition metal dichalcogenide (TMD) make it an ideal candidate for optoelectronic applications. Competing interlayer charge (CT) and energy transfer (ET) processes control the photocarrier relaxation pathways in TMD heterostructures (HSs). In TMDs, long-distance ET can survive up to several tens of nm, unlike the CT process. Our experiment shows that an efficient ET occurs from the 1Ls WSe2-to-MoS2 with an interlayer hBN, due to the resonant overlapping of the high-lying excitonic states between the two TMDs, resulting in enhanced HS MoS2 PL emission. This type of unconventional ET from the lower-to-higher optical bandgap material is not typical in the TMD HSs. With increasing temperature, the ET process becomes weaker due to the increased electron-phonon scattering, destroying the enhanced MoS2 emission. Our work provides new insight into the long-distance ET process and its effect on the photocarrier relaxation pathways.

cond-mat.mtrl-sci↗

arXiv2022

Large Itinerant Electron Exchange Coupling in the Magnetic Topological Insulator MnBi2Te4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with applications in spintronics and quantum information. The emergence of such phases relies on strong interaction between localized spins and itinerant states comprising the topological bands, and the subsequent formation of an exchange gap. However, this interaction has never been measured in any intrinsic magnetic topological material. Using a multimodal approach, this exchange interaction is measured in MnBi2Te4, the first realized intrinsic magnetic topological insulator. Interrogating nonequilibrium spin dynamics, itinerant bands are found to exhibit a strong exchange coupling to localized Mn spins. Momentum-resolved ultrafast electron scattering and magneto-optic measurements reveal that itinerant spins disorder via electron-phonon scattering at picosecond timescales. Localized Mn spins, probed by resonant X-ray scattering, disorder concurrently with itinerant spins, despite being energetically decoupled from the initial excitation. Modeling the results using atomistic simulations, the exchange coupling between localized and itinerant spins is estimated to be >100 times larger than superexchange interactions. This implies an exchange gap of >25 meV should occur in the topological surface states. By directly quantifying local-itinerant exchange coupling, this work validates the materials-by-design strategy of utilizing localized magnetic order to create and manipulate magnetic topological phases, from static to ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2021

SGEITL: Scene Graph Enhanced Image-Text Learning for Visual Commonsense Reasoning

Answering complex questions about images is an ambitious goal for machine intelligence, which requires a joint understanding of images, text, and commonsense knowledge, as well as a strong reasoning ability. Recently, multimodal Transformers have made great progress in the task of Visual Commonsense Reasoning (VCR), by jointly understanding visual objects and text tokens through layers of cross-modality attention. However, these approaches do not utilize the rich structure of the scene and the interactions between objects which are essential in answering complex commonsense questions. We propose a Scene Graph Enhanced Image-Text Learning (SGEITL) framework to incorporate visual scene graphs in commonsense reasoning. To exploit the scene graph structure, at the model structure level, we propose a multihop graph transformer for regularizing attention interaction among hops. As for pre-training, a scene-graph-aware pre-training method is proposed to leverage structure knowledge extracted in the visual scene graph. Moreover, we introduce a method to train and generate domain-relevant visual scene graphs using textual annotations in a weakly-supervised manner. Extensive experiments on VCR and other tasks show a significant performance boost compared with the state-of-the-art methods and prove the efficacy of each proposed component.

cs.CV↗

arXiv2021

Role of equilibrium fluctuations in light-induced order

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.

cond-mat.mtrl-sci↗

arXiv2021

Subterahertz collective dynamics of polar vortices

The collective dynamics of topological structures have been of great interest from both fundamental and applied perspectives. For example, the studies of dynamical properties of magnetic vortices and skyrmions not only deepened the understanding of many-body physics but also led to potential applications in data processing and storage. Topological structures constructed from electrical polarization rather than spin have recently been realized in ferroelectric superlattices, promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics of such complex extended nanostructures which in turn underlies their functionalities. Using terahertz-field excitation and femtosecond x-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders of magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices. A previously unseen soft mode, hereafter referred to as a vortexon, emerges as transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond time scales. Its frequency is significantly reduced at a critical strain, indicating a condensation of structural dynamics. First-principles-based atomistic calculations and phase-field modeling reveal the microscopic atomic arrangements and frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens up opportunities for applications of electric-field driven data processing in topological structures with ultrahigh speed and density.

cond-mat.mes-hall↗

arXiv2021

Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in nanocrystals are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in semiconductor nanocrystals. Investigation of the excitation energy dependence shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap result in transient lattice heating that occurs on a much longer 200 ps timescale, governed by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

cond-mat.mes-hall↗