arXiv subjects

Jonghwan Kim

Publications and source records attributed to Jonghwan Kim.

At least 19 recordsLinked to original sources

arXiv2026

Activated Migration of Localized Ligand-Field Excitons in Atomically Thin CrCl3

Two-dimensional crystals with densely packed atoms exhibit a range of emerging properties, particularly a wide variety of excitonic behaviors. Thickness-variable layered chromium trihalides with finite surface recombination sites provide an ideal system for understanding how excitons confined in octahedral ligand fields migrate on nanometer length scales, a regime that defies conventional transport probes. In this work, we demonstrate that Cr3+-derived photoluminescence in CrCl3 is spectrally thickness-independent, but its relaxation dynamics are strongly sensitive to thickness and temperature, thereby indicating significant activated migration. A diffusion-coupled surface recombination model reveals an effective out-of-plane diffusivity of 4.5 x 10-6 cm2/s for the ligand-field excitons and a diffusion activation energy of 130 meV. The latter is comparable to the reorganization energy independently estimated from optical Stokes shifts, suggesting that exciton transport is coupled to local lattice relaxation. Furthermore, we show that the relaxation dynamics can be systematically tuned by either enhancing or suppressing surface recombination through controlled surface reactions or encapsulation. This work not only reveals the nanoscopic transport of localized ligand-field excitons but also establishes a spectroscopic transport probe applicable to various 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Step-directed Epitaxy of Uni-directional Hexagonal Boron Nitride on Vicinal Ge(110)

Insulating hexagonal boron nitride (hBN) films with precisely controlled thickness are ideal dielectric components to modulate various interfaces in electronic devices. To achieve this, high-quality hBN with controlled atomic configurations must be able to form pristine interfaces with various materials in devices. However, previously reported large-scale hBN films with uniform thickness either are polycrystalline or are not suitable for atomically clean assembly via mechanical exfoliation, limiting their applications in device technology. Here, we report the large-scale growth of monolayer single crystalline hBN films on Ge(110) substrates by using chemical vapor deposition (CVD). Vicinal Ge(110) substrates are used for the step-directed epitaxial growth of hBN, where Ge atomic steps act as the hBN nucleation sites, guiding the uni-directional alignments of multiple hBN domains. Density functional theory (DFT) calculations reveal that the optimum hydrogen passivations on both hBN edges and Ge surfaces enable the epitaxial coupling between hBN and the Ge step edges and the single crystallinity of the final hBN films. Using epitaxially grown monolayer hBN films, we fabricate a few hBN films with controlled stacking orders and pristine interfaces through a layer-by-layer assembly process. These films function as high-quality dielectrics to enhance carrier transport in graphene and MoS 2 channels.

cond-mat.mtrl-sci↗

arXiv2025

Natural Hyperbolicity of Hexagonal Boron Nitride in the Deep Ultraviolet

Hyperbolic media enable unique optical phenomena including hyperlensing, negative refraction, enhanced photonic density of states (PDOS), and highly confined polaritons. While most hyperbolic media are artificially engineered metamaterials, certain natural materials with extreme anisotropy can exhibit hyperbolic dispersion. Here, we report the first observation of natural hyperbolic dispersion in hexagonal boron nitride (hBN) in the deep-ultraviolet (DUV) regime, induced by strong, anisotropic exciton resonances. Using imaging spectroscopic ellipsometry (ISE), we characterize the complex dielectric function along in-plane and out-of-plane directions down to 190 nm (6.53 eV), revealing a type-II hyperbolic window in the DUV regime. This hyperbolicity supports hyperbolic exciton polaritons (HEP) with high directionality and slow group velocity. Our findings establish hBN as a promising platform for nanophotonic applications in the technologically significant DUV spectral range.

physics.optics↗

arXiv2025

Quantum interference and occupation control in high harmonic generation from monolayer $WS_2$

Two-dimensional hexagonal materials such as transition metal dichalcogenides exhibit valley degrees of freedom, offering fascinating potential for valley-based quantum computing and optoelectronics. In nonlinear optics, the K and K' valleys provide excitation resonances that can be used for ultrafast control of excitons, Bloch oscillations, and Floquet physics. Under intense laser fields, however, the role of coherent carrier dynamics away from the K/K' valleys is largely unexplored. In this study, we observe quantum interferences in high harmonic generation from monolayer $WS_2$ as laser fields drive electrons from the valleys across the full Brillouin zone. In the perturbative regime, interband resonances at the valleys enhance high harmonic generation through multi-photon excitations. In the strong-field regime, the high harmonic spectrum is sensitively controlled by light-driven quantum interferences between the interband valley resonances and intraband currents originating from electrons occupying various points in the Brillouin zone, also away from K/K' valleys such as $\Gamma$ and M. Our experimental observations are in strong agreement with quantum simulations, validating their interpretation. This work proposes new routes for harnessing laser-driven quantum interference in two-dimensional hexagonal systems and all-optical techniques to occupy and read-out electronic structures in the full Brillouin zone via strong-field nonlinear optics, advancing quantum technologies.

physics.optics↗

arXiv2025

Electrical Generation of Colour Centres in Hexagonal Boron Nitride

Defects in wide band gap crystals have emerged as a promising platform for hosting colour centres that enable quantum photonic applications. Among these, hexagonal boron nitride (hBN), a van der Waals material, stands out for its ability to be integrated into heterostructures, enabling unconventional charge injection mechanisms that bypass the need for p-n junctions. This advancement allows for the electrical excitation of hBN colour centres deep inside the large hBN bandgap, which has seen rapid progress in recent developments. Here, we fabricate hBN electroluminescence (EL) devices that generate narrowband colour centres suitable for electrical excitation. The colour centres are localised to tunnelling current hotspots within the hBN flake, which are designed during device fabrication. We outline the optimal conditions for device operation and colour centre stability, focusing on minimising background emission and ensuring prolonged operation. Our findings follow up on the existing literature and mark a step forward towards the integration of hBN based colour centres into quantum photonic technologies.

physics.optics↗

arXiv2023

Quantum spin nematic phase in a square-lattice iridate

Spin nematic (SN) is a magnetic analog of classical liquid crystals, a fourth state of matter exhibiting characteristics of both liquid and solid. Particularly intriguing is a valence-bond SN, in which spins are quantum entangled to form a multi-polar order without breaking time-reversal symmetry, but its unambiguous experimental realization remains elusive. Here, we establish a SN phase in the square-lattice iridate Sr$_2$IrO$_4$, which approximately realizes a pseudospin one-half Heisenberg antiferromagnet (AF) in the strong spin-orbit coupling limit. Upon cooling, the transition into the SN phase at T$_C$ $\approx$ 263 K is marked by a divergence in the static spin quadrupole susceptibility extracted from our Raman spectra, and concomitant emergence of a collective mode associated with the spontaneous breaking of rotational symmetries. The quadrupolar order persists in the antiferromagnetic (AF) phase below T$_N$ $\approx$ 230 K, and becomes directly observable through its interference with the AF order in resonant x-ray diffraction, which allows us to uniquely determine its spatial structure. Further, we find using resonant inelastic x-ray scattering a complete breakdown of coherent magnon excitations at short-wavelength scales, suggesting a resonating-valence-bond-like quantum entanglement in the AF state. Taken together, our results reveal a quantum order underlying the Néel AF that is widely believed to be intimately connected to the mechanism of high temperature superconductivity (HTSC).

cond-mat.str-el↗

arXiv2023

Room temperature electroluminescence from isolated colour centres in van der Waals semiconductors

Defects in wide bandgap semiconductors have recently emerged as promising candidates for solid-state quantum optical technologies. Electrical excitation of emitters may pave the way to scalable on-chip devices, and therefore is highly sought after. However, most wide band gap materials are not amenable to efficient doping, which in turn poses challenges on efficient electrical excitation and on-chip integration. Here, we demonstrate for the first time room temperature electroluminescence from isolated colour centres in hexagonal boron nitride (hBN). We harness the van der Waals (vdW) structure of two-dimensional materials, and engineer nanoscale devices comprised of graphene - hBN - graphene tunnel junctions. Under an applied bias, charge carriers are injected into hBN, and result in a localised light emission from the hBN colour centres. Remarkably, our devices operate at room temperature and produce robust, narrowband emission spanning a wide spectral range - from the visible to the near infrared. Our work marks an important milestone in van der Waals materials and their promising attributes for integrated quantum technologies and on-chip photonic circuits.

cond-mat.mes-hall↗

arXiv2022

Dimensional crossover of charge order in IrTe$_2$ with strong interlayer coupling

Tuning dimensionality in van der Waals materials with finite interlayer coupling has introduced various electronic phase transitions by conventional mechanical exfoliation. Particularly when the electronic order is tied to the modulation of the interlayer coupling, such dimensional tunability has a strong impact on its stability and properties, which has rarely been investigated experimentally. Here, we demonstrate a dimensional crossover of charge order in IrTe$_2$ from genuine two- to quasi-three-dimension using low-temperature scanning tunneling microscopy and spectroscopy. Employing atomically thin IrTe$_2$ flakes ranging from monolayer to multilayer, we observe a gradual phase transition of charge order and exponential decay of Coulomb gap with increasing thickness. Moreover, we find a suppression of the density of states emerging at an abrupt lateral interface between two- and three-dimension. These findings are attributed to the interplay between the strongly coupled layers and substrate-driven perturbation, which can provide a new insight into the dimensional crossover of strongly coupled layered materials with hidden electronic phases.

cond-mat.str-el↗

arXiv2022

Gate-tunable quantum pathways of high harmonic generation in graphene

Under strong laser fields, electrons in solids radiate high-harmonic fields by travelling through quantum pathways in Bloch bands in the sub-laser-cycle timescales. Understanding these pathways in the momentum space through the high-harmonic radiation can enable an all-optical ultrafast probe to observe coherent lightwave-driven processes and measure electronic structures as recently demonstrated for semiconductors. However, such demonstration has been largely limited for semimetals because the absence of the bandgap hinders an experimental characterization of the exact pathways. In this study, by combining electrostatic control of chemical potentials with HHG measurement, we resolve quantum pathways of massless Dirac fermions in graphene under strong laser fields. Electrical modulation of HHG reveals quantum interference between the multi-photon interband excitation channels. As the light-matter interaction deviates beyond the perturbative regime, elliptically polarized laser fields efficiently drive massless Dirac fermions via an intricate coupling between the interband and intraband transitions, which is corroborated by our theoretical calculations. Our findings pave the way for strong-laser-field tomography of Dirac electrons in various quantum semimetals and their ultrafast electronics with a gate control.

cond-mat.mes-hall↗

arXiv2022

Photoluminescence Path Bifurcations by Spin Flip in Two-Dimensional CrPS4

Ultrathin layered crystals of coordinated chromium(III) are promising not only as two-dimensional (2D) magnets but also as 2D near-infrared (NIR) emitters owing to long-range spin correlation and efficient transition between high and low-spin excited states of Cr3+ ions. In this study, we report on dual-band NIR photoluminescence (PL) of CrPS4 and show that its excitonic emission bifurcates into fluorescence and phosphorescence depending on thickness, temperature and defect density. In addition to the spectral branching, the biexponential decay of PL transients, also affected by the three factors, could be well described within a three-level kinetic model for Cr(III). In essence, the PL bifurcations are governed by activated reverse intersystem crossing from the low to high-spin states, and the transition barrier becomes lower for thinner 2D samples because of surface-localized defects. Our findings can be generalized to 2D solids of coordinated metals and will be valuable in realizing novel magneto-optic functions and devices.

cond-mat.mtrl-sci↗

arXiv2022

Customising radiative decay dynamics of two-dimensional excitons via position- and polarisation-dependent vacuum-field interference

Embodying bosonic and electrically interactive characteristics in two-dimensional space, excitons in transition-metal dichalcogenides (TMDCs) have garnered considerable attention. The realisation and application of strong-correlation effects, long-range transport, and valley-dependent optoelectronic properties require customising exciton decay dynamics. Strains, defects, and electrostatic doping effectively control the decay dynamics but significantly disturb the intrinsic properties of TMDCs, such as electron band structure and exciton binding energy. Meanwhile, vacuum-field manipulation provides an optical alternative for engineering radiative decay dynamics. Planar mirrors and cavities have been employed to manage the light-matter interactions of two-dimensional excitons. However, the conventional flat platforms cannot customise the radiative decay landscape in the horizontal TMDC plane or independently control vacuum field interference at different pumping and emission frequencies. Here, we present a meta-mirror resolving the issues with more optical freedom. For neutral excitons of the monolayer MoSe2, the meta-mirror manipulated the radiative decay rate by two orders of magnitude, depending on its geometry. Moreover, we experimentally identified the correlation between emission intensity and spectral linewidth. The anisotropic meta-mirror demonstrated polarisation-dependent radiative decay control. We expect that the meta-mirror platform will be promising to tailor the two-dimensional distributions of lifetime, density, and diffusion of TMDC excitons in advanced opto-excitonic applications.

cond-mat.mes-hall↗

arXiv2022

Sr$_2$IrO$_4$/Sr$_3$Ir$_2$O$_7$ superlattice for a model 2D quantum Heisenberg antiferromagnet

Spin-orbit entangled pseudospins hold promise for a wide array of exotic magnetism ranging from a Heisenberg antiferromagnet to a Kitaev spin liquid depending on the lattice and bonding geometry, but many of the host materials suffer from lattice distortions and deviate from idealized models in part due to inherent strong pseudospin-lattice coupling. Here, we report on the synthesis of a magnetic superlattice comprising the single ($n$=1) and the double ($n$=2) layer members of the Ruddlesden-Popper series iridates Sr$_{n+1}$Ir$_{n}$O$_{3n+1}$ alternating along the $c$-axis, and provide a comprehensive study of its lattice and magnetic structures using scanning transmission electron microscopy, resonant elastic and inelastic x-ray scattering, third harmonic generation measurements and Raman spectroscopy. The superlattice is free of the structural distortions reported for the parent phases and has a higher point group symmetry, while preserving the magnetic orders and pseudospin dynamics inherited from the parent phases, featuring two magnetic transitions with two symmetry-distinct orders. We infer weaker pseudospin-lattice coupling from the analysis of Raman spectra and attribute it to frustrated magnetic-elastic couplings. Thus, the superlattice expresses a near ideal network of effective spin-one-half moments on a square lattice.

cond-mat.str-el↗

arXiv2021

Deep-ultraviolet electroluminescence and photocurrent generation in graphene/hBN/graphene heterostructures

Hexagonal boron nitride (hBN) is a van der Waals semiconductor with a wide bandgap of ~ 5.96 eV. Despite the indirect bandgap characteristics of hBN, charge carriers excited by high energy electrons or photons efficiently emit luminescence at deep-ultraviolet (DUV) frequencies via strong electron-phonon interaction, suggesting potential DUV light emitting device applications. However, electroluminescence from hBN has not been demonstrated at DUV frequencies so far. In this study, we report DUV electroluminescence and photocurrent generation in graphene/hBN/graphene heterostructures at room temperature. Tunneling carrier injection from graphene electrodes into the band edges of hBN enables prominent electroluminescence at DUV frequencies. On the other hand, under DUV laser illumination and external bias voltage, graphene electrodes efficiently collect photo-excited carriers in hBN, which generates high photocurrent. Laser excitation micro-spectroscopy shows that the radiative recombination and photocarrier excitation processes in the heterostructures mainly originate from the pristine structure and the stacking faults in hBN. Our work provides a pathway toward efficient DUV light emitting and detection devices based on hBN.

cond-mat.mtrl-sci↗

arXiv2021

Direct observation of excitonic instability in Ta2NiSe5

Coulomb attraction between electrons and holes in a narrow-gap semiconductor or a semimetal is predicted to lead to an elusive phase of matter dubbed 'excitonic insulator'. However, direct observation of such electronic instability remains extremely rare. Here, we report the observation of incipient divergence in the static excitonic susceptibility of the candidate material Ta2NiSe5 using Raman spectroscopy. Critical fluctuations of the excitonic order parameter give rise to quasi-elastic scattering of B2g symmetry, whose intensity grows inversely with temperature toward the Weiss temperature of Tw ~241 K, which is arrested by a structural phase transition driven by an acoustic phonon of the same symmetry at Tc =325 K. Concurrently, a B2g optical phonon becomes heavily damped to the extent that its trace is almost invisible around Tc, which manifests a strong electron-phonon coupling that has obscured the identification of the low-temperature phase as an excitonic insulator for more than a decade. Our result unambiguously reveals the electronic origin of the phase transition.

cond-mat.str-el↗

arXiv2021

γ-GeSe:a new hexagonal polymorph from group IV-VI monochalcogenides

The family of group IV-VI monochalcogenides has an atomically puckered layered structure, and their atomic bond configuration suggests the possibility for the realization of various polymorphs. Here, we report the synthesis of the first hexagonal polymorph from the family of group IV-VI monochalcogenides, which is conventionally orthorhombic. Recently predicted four-atomic-thick hexagonal GeSe, so-called γ-GeSe, is synthesized and clearly identified by complementary structural characterizations, including elemental analysis, electron diffraction, high-resolution transmission electron microscopy imaging, and polarized Raman spectroscopy. The electrical and optical measurements indicate that synthesized γ-GeSe exhibits high electrical conductivity of 3x10^5 S/m, which is comparable to those of other two-dimensional layered semimetallic crystals. Moreover, γ-GeSe can be directly grown on h-BN substrates, demonstrating a bottom-up approach for constructing vertical van der Waals heterostructures incorporating γ-GeSe. The newly identified crystal symmetry of γ-GeSe warrants further studies on various physical properties of γ-GeSe.

cond-mat.mes-hall↗

arXiv2020

Strongly-bound excitons and trions in anisotropic 2D semiconductors

Monolayer and few-layer phosphorene are anisotropic quasi-two-dimensional (quasi-2D) van der Waals (vdW) semiconductors with a linear-dichroic light-matter interaction and a widely-tunable direct-band gap in the infrared frequency range. Despite recent theoretical predictions of strongly-bound excitons with unique properties, it remains experimentally challenging to probe the excitonic quasiparticles due to the severe oxidation during device fabrication. In this study, we report observation of strongly-bound excitons and trions with highly-anisotropic optical properties in intrinsic bilayer phosphorene, which are protected from oxidation by encapsulation with hexagonal boron nitride (hBN), in a field-effect transistor (FET) geometry. Reflection contrast and photoluminescence spectroscopy clearly reveal the linear-dichroic optical spectra from anisotropic excitons and trions in the hBN-encapsulated bilayer phosphorene. The optical resonances from the exciton Rydberg series indicate that the neutral exciton binding energy is over 100 meV even with the dielectric screening from hBN. The electrostatic injection of free holes enables an additional optical resonance from a positive trion (charged exciton) ~ 30 meV below the optical bandgap of the charge-neutral system. Our work shows exciting possibilities for monolayer and few-layer phosphorene as a platform to explore many-body physics and novel photonics and optoelectronics based on strongly-bound excitons with two-fold anisotropy.

cond-mat.mes-hall↗

arXiv2020

Superconductivity emerging from a stripe charge order in IrTe2 nanoflakes

Superconductivity in the vicinity of a competing electronic order often manifests itself with a superconducting dome, centred at a presumed quantum critical point in the phase diagram. This common feature, found in many unconventional superconductors, has supported a prevalent scenario that fluctuations or partial melting of a parent order are essential for inducing or enhancing superconductivity. Here we present a contrary example, found in IrTe2 nanoflakes of which the superconducting dome is identified well inside the parent stripe charge ordering phase in the thickness-dependent phase diagram. The coexisting stripe charge order in IrTe2 nanoflakes significantly increases the out-of-plane coherence length and the coupling strength of superconductivity, in contrast to the doped bulk IrTe2. These findings clarify that the inherent instabilities of the parent stripe phaseare sufficient to induce superconductivity in IrTe2 without its complete or partial melting. Our study highlights the thickness control as an effective means to unveil intrinsic phase diagrams of correlated vdW materials.

cond-mat.supr-con↗

arXiv2018

Rethinking Misalignment to Raise the Bar for Heap Pointer Corruption

Heap layout randomization renders a good portion of heap vulnerabilities unexploitable. However, some remnants of the vulnerabilities are still exploitable even under the randomized layout. According to our analysis, such heap exploits often abuse pointer-width allocation granularity to spray crafted pointers. To address this problem, we explore the efficacy of byte-granularity (the most fine-grained) heap randomization. Heap randomization, in general, has been a well-trodden area; however, the efficacy of byte-granularity randomization has never been fully explored as \emph{misalignment} raises various concerns. This paper unravels the pros and cons of byte-granularity heap randomization by conducting comprehensive analysis in three folds: (i) security effectiveness, (ii) performance impact, and (iii) compatibility analysis to measure deployment cost. Security discussion based on 20 CVE case studies suggests that byte-granularity heap randomization raises the bar against heap exploits more than we initially expected; as pointer spraying approach is becoming prevalent in modern heap exploits. Afterward, to demystify the skeptical concerns regarding misalignment, we conduct cycle-level microbenchmarks and report that the performance cost is highly concentrated to edge cases depending on L1-cache line. Based on such observations, we design and implement an allocator suited to optimize the performance cost of byte-granularity heap randomization; then evaluate the performance with the memory-intensive benchmark (SPEC2006). Finally, we discuss compatibility issues using Coreutils, Nginx, and ChakraCore.

cs.CR↗