arXiv subjects

Kyoung-Duck Park

Publications and source records attributed to Kyoung-Duck Park.

14 recordsLinked to original sources

arXiv2026

Polarization Engineering of Second-Harmonic Generation in 3R-MoS$_2$ Waveguides

Chip-scale nonlinear optics enables strong light-matter interactions within compact devices, serving as a fundamental platform for multifunctional integrated photonics from classical optical signal processing to quantum information technologies. Transition metal dichalcogenide (TMDC) waveguides have recently emerged as a highly promising platform owing to their giant material nonlinearity and extended interaction lengths. To date, however, research has predominantly focused on conversion efficiency, leaving the mechanisms governing the polarization state of nonlinear signal largely unexplored. Here, we establish a comprehensive framework for engineering the polarization of second-harmonic generation (SHG) in 3R-MoS$_2$ waveguides. By synergizing polarization-resolved measurements with theoretical modeling, we reveal that the SHG polarization is determined by guided-mode interactions constrained by waveguide geometry and crystal symmetry, and further reshaped during propagation. We demonstrate that thickness-dependent guided-mode confinement and in-plane crystal symmetry provide robust, static control over SHG polarization, while propagation length offers a dynamic tuning knob for continuously tailoring the nonlinear output. Our findings provide a deterministic approach for on-chip polarization engineering, opening opportunities for reconfigurable nonlinear light sources and quantum photonic circuits.

physics.optics↗

arXiv2025

Tip-enhanced quantum-sensing spectroscopy for bright and reconfigurable solid-state single-photon emitters

Atom-like defects in hexagonal boron nitride (hBN) provide room-temperature single-photon emission and coherent spin states, making them attractive for quantum-computing and -sensing applications. However, their random spatial and spectral characteristics hamper deterministic coupling with nano-optical cavities, limiting their use as bright single-photon sources and sensitive quantum sensors. Here, we present tip-enhanced quantum-sensing spectroscopy of single-photon emitters in hBN. Through precise spatial positioning of individual emitters within tip-cavities with different plasmon resonances, we adaptively control the enhancement rates of both excitation and emission, as well as the single-photon purity. In this way, optimal selection of their relative contributions can effectively reconfigure solid-state single-photon sources, with simultaneous nano-spectroscopic space- and time-resolved analyses. Furthermore, we demonstrate tip-enhanced quantum-sensing with single spin defects through optically detected magnetic resonance (ODMR) experiments in tip-coupled hBN nanoflakes. Our approach provides a unique pathway toward highly-sensitive and deterministic quantum-sensing with room-temperature single-photon emitters.

quant-ph↗

arXiv2022

Freeze-frame approach for robust single-molecule tip-enhnaced Raman spectroscopy at room temperature

A quantitative single-molecule tip-enhanced Raman spectroscopy (TERS) study at room temperature remained a challenge due to the rapid structural dynamics of molecules exposed to air. Here, we demonstrate the single-molecule level hyperspectral TERS imaging of brilliant cresyl blue (BCB) at room temperature for the first time, along with quantitative spectral analyses. Freeze-frame approach using a thin Al2O3 capping layer, which suppresses spectral diffusions and inhibits chemical reactions and contaminations in air, enabled reliable and robust chemical imaging. For the molecules resolved spatially in the TERS image, a clear Raman peak variation up to 7.5 cm-1 is observed, which cannot be found in molecular ensembles. From density functional theory-based quantitative analyses of the varied TERS peaks, we reveal the conformational heterogeneity at the single-molecule level. This work provides a facile way to investigate the single-molecule properties in interacting media, expanding the scope of single-molecule vibrational spectroscopy.

physics.chem-ph↗

arXiv2022

Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature

A quantitative single-molecule tip-enhanced Raman spectroscopy (TERS) study at room temperature remained a challenge due to the rapid structural dynamics of molecules exposed to air. Here, we demonstrate the hyperspectral TERS imaging of single or a few brilliant cresyl blue (BCB) molecules at room temperature, along with quantitative spectral analyses. Robust chemical imaging is enabled by the freeze-frame approach using a thin Al$_{2}$O$_{3}$ capping layer, which suppresses spectral diffusions and inhibits chemical reactions and contaminations in air. For the molecules resolved spatially in the TERS image, a clear Raman peak variation up to 7.5 cm$^{-1}$ is observed, which cannot be found in molecular ensembles. From density functional theory-based quantitative analyses of the varied TERS peaks, we reveal the conformational heterogeneity at the single-molecule level. This work provides a facile way to investigate the single-molecule properties in interacting media, expanding the scope of single-molecule vibrational spectroscopy studies.

physics.optics↗

arXiv2022

Dynamical Control of Interlayer Excitons and Trions in WSe$_2$/Mo$_{0.5}$W$_{0.5}$Se$_2$ Heterobilayer via Tunable Near-Field Cavity

Emerging photo-induced excitonic processes in transition metal dichalcogenide (TMD) heterobilayers, e.g., coupling, dephasing, and energy transfer of intra- and inter-layer excitons, allow new opportunities for ultrathin photonic devices. Yet, with the associated large degree of spatial heterogeneity, understanding and controlling their complex competing interactions at the nanoscale remains a challenge. Here, we present an all-round dynamic control of intra- and inter-layer excitonic processes in a WSe$_2$/Mo$_{0.5}$W$_{0.5}$Se$_2$ heterobilayer using multifunctional tip-enhanced photoluminescence (TEPL) spectroscopy. Specifically, we control the radiative recombination path and emission rate, electronic bandgap energy, and neutral to charged exciton conversion with <20 nm spatial resolution in a reversible manner. It is achieved through the tip-induced engineering of Au tip-heterobilayer distance and interlayer distance, GPa scale local pressure, and plasmonic hot-electron injection respectively, with simultaneous spectroscopic TEPL measurements. This unique nano-opto-electro-mechanical control approach provides new strategies for developing versatile nano-excitonic devices based on TMD heterobilayers.

cond-mat.mtrl-sci↗

arXiv2021

Low-threshold exciton transport and control in atomically thin semiconductors

Understanding and controlling the nanoscale transport of excitonic quasiparticles in atomically thin 2D semiconductors is crucial to produce highly efficient nano-excitonic devices. Here, we present a nano-gap device to selectively confine excitons or trions of 2D transition metal dichalcogenides at the nanoscale, facilitated by the drift-dominant exciton funnelling into the strain-induced local spot. We investigate the spatio-spectral characteristics of the funnelled excitons in a WSe2 monolayer (ML) and converted trions in a MoS2 ML using hyperspectral tip-enhanced photoluminescence (TEPL) imaging with <15 nm spatial resolution. In addition, we dynamically control the exciton funnelling and trion conversion rate by the GPa scale tip pressure engineering. Through a drift-diffusion model, we confirm an exciton funnelling efficiency of ~25 % with a significantly low strain threshold (~0.1 %) which sufficiently exceeds the efficiency of ~3 % in previous studies. This work provides a new strategy to facilitate efficient exciton transport and trion conversion of 2D semiconductor devices.

cond-mat.mes-hall↗

arXiv2021

Tip-induced strain, bandgap, and radiative decay engineering of a single metal halide perovskite quantum dot

Strain engineering of perovskite quantum dots (pQDs) enables widely-tunable photonic device applications. However, manipulation at the single-emitter level has never been attempted. Here, we present a tip-induced control approach combined with tip-enhanced photoluminescence (TEPL) spectroscopy to engineer strain, bandgap, and emission quantum yield of a single pQD. Single CsPbBr$_{x}$I$_{3-x}$ pQDs are clearly resolved through hyperspectral TEPL imaging with $\sim$10 nm spatial resolution. The plasmonic tip then directly applies pressure to a single pQD to facilitate a bandgap shift up to $\sim$62 meV with Purcell-enhanced PL quantum yield as high as $\sim$10$^5$ for the strain-induced pQD. Furthermore, by systematically modulating the tip-induced compressive strain of a single pQD, we achieve dynamical bandgap engineering in a reversible manner. In addition, we facilitate the quantum dot coupling for a pQD ensemble with $\sim$0.8 GPa tip pressure at the nanoscale. Our approach presents a new strategy to tune the nano-opto-electro-mechanical properties of pQDs at the single-crystal level.

physics.app-ph↗

arXiv2020

Tip-induced nano-engineering of strain, bandgap, and exciton dynamics in 2D semiconductors

The tunability of the bandgap, absorption and emission energies, photoluminescence (PL) quantum yield, exciton transport, and energy transfer in transition metal dichalcogenide (TMD) monolayers provides a new class of functions for a wide range of ultrathin photonic devices. Recent strain-engineering approaches have enabled us to tune some of these properties, yet dynamic control at the nanoscale with real-time and -space characterizations remains a challenge. Here, we demonstrate a dynamic nano-mechanical strain-engineering of naturally-formed wrinkles in a WSe2 monolayer, with real-time investigation of nano-spectroscopic properties using hyperspectral adaptive tip-enhanced PL (a-TEPL) spectroscopy. First, we characterize nanoscale wrinkles through hyperspectral a-TEPL nano-imaging with <15 nm spatial resolution which reveals the modified nano-excitonic properties by the induced tensile strain at the wrinkle apex, e.g., an increase in the quantum yield due to the exciton funneling, decrease in PL energy up to ~10 meV, and a symmetry change in the TEPL spectra caused by the reconfigured electronic bandstructure. We then dynamically engineer the local strain by pressing and releasing the wrinkle apex through an atomic force tip control. This nano-mechanical strain-engineering allows us to tune the exciton dynamics and emission properties at the nanoscale in a reversible fashion. In addition, we demonstrate a systematic switching and modulation platform of the wrinkle emission, which provides a new strategy for robust, tunable, and ultracompact nano-optical sources in atomically thin semiconductors.

cond-mat.mtrl-sci↗

arXiv2020

Adaptive tip-enhanced nano-spectroscopy

Tip-enhanced nano-spectroscopy and -imaging, such as tip-enhanced photoluminescence (TEPL), tip-enhanced Raman spectroscopy (TERS), and others, have become indispensable from materials science to single molecule studies. However, the techniques suffer from inconsistent performance due to lack of nanoscale control of tip apex structure, which often leads to irreproducible spectral, spatial, and polarization resolved imaging. Instead of refining tip-fabrication to resolve this problem, we pursue the inverse approach of optimizing the nano-optical vector-field at the tip apex via adaptive optics. Specifically, we demonstrate dynamic wavefront shaping of the excitation field to effectively couple light to the tip and adaptively control for enhanced sensitivity and polarization-controlled TEPL and TERS, with performance exceeding what can be achieved by conventional tip-fabrication and optimal excitation polarization. Employing a sequence feedback algorithm, we achieve 4.4$\times$10$^4$-fold TEPL enhancement of a WSe$_2$ monolayer which is >2$\times$ larger than the normal TEPL intensity without wavefront shaping, as well as the largest plasmon-enhanced PL intensity of a transition metal dichalcogenide (TMD) monolayer reported to date. In addition, with dynamical near-field polarization control in TERS, we demonstrate the investigation of conformational heterogeneity of brilliant cresyl blue (BCB) molecules as well as the controllable observation of IR-active modes due to a large gradient field effect. Adaptive tip-enhanced spectroscopy and imaging thus provides for a new systematic approach towards computational nanoscopy making optical nano-imaging more robust, versatile, and widely deployable.

physics.optics↗

arXiv2020

Radiative control of localized excitons at room temperature with an ultracompact tip-enhanced plasmonic nano-cavity

In atomically thin semiconductors, localized exciton (X$_L$) coupled to light shows single quantum emitting behaviors through radiative relaxation processes providing a new class of optical sources for potential applications in quantum communication. In most studies, however, X$_L$ photoluminescence (PL) from crystal defects has mainly been observed in cryogenic conditions because of their sub-wavelength emission region and low quantum yield at room temperature. Furthermore, engineering the radiative relaxation properties, e.g., emission region, intensity, and energy, remained challenging. Here, we present a plasmonic antenna with a triple-sharp-tips geometry to induce and control the X$_L$ emission of a WSe$_2$ monolayer (ML) at room temperature. By placing a ML crystal on the two sharp Au tips in a bowtie antenna fabricated through cascade domino lithography with a radius of curvature of <1 nm, we effectively induce tensile strain in the nanoscale region to create robust X$_L$ states. An Au tip with tip-enhanced photoluminescence (TEPL) spectroscopy is then added to the strained region to probe and control the X$_L$ emission. With TEPL enhancement of X$_L$ as high as ~10$^6$ in the triple-sharp-tips device, experimental results demonstrate the controllable X$_L$ emission in <30 nm area with a PL energy shift up to 40 meV, resolved by tip-enhanced PL and Raman imaging with <15 nm spatial resolution. Our approach provides a systematic way to control localized quantum light in 2D semiconductors offering new strategies for active quantum nano-optical devices.

physics.optics↗

arXiv2019

Tip-enhanced strong coupling spectroscopy, imaging, and control of a single quantum emitter

Optical cavities can enhance and control light-matter interactions. This has recently been extended to the nanoscale, and with single emitter strong coupling regime even at room temperature using plasmonic nano-cavities with deep sub-diffraction-limited mode volumes. However, with emitters in static nano-cavities, this limits the ability to tune coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) spectroscopy, imaging, and control. Based on a nano-cavity formed between a scanning plasmonic antenna-tip and the substrate, by reversibly and dynamically addressing single quantum dots (QDs) we observe mode splitting > 160 meV and anticrossing over a detuning range of ~100 meV, and with sub-nm precision control over the mode volume in the ~1000 nm^3 regime. Our approach, as a new paradigm of nano-cavity quantum-electrodynamics near-field microscopy to induce, probe, and control single-emitter plasmon hybrid quantum states, opens new pathways from opto-electronics to quantum information science.

physics.optics↗

arXiv2018

Polarization control with plasmonic antenna-tips: A universal approach for optical nano-crystallography and vector-field imaging

Controlling the propagation and polarization vectors in linear and nonlinear optical spectroscopy enables to probe the anisotropy of optical responses providing structural symmetry selective contrast in optical imaging. Here we present a novel tilted antenna-tip approach to control the optical vector-field by breaking the axial symmetry of the nano-probe in tip-enhanced near-field microscopy. This gives rise to a localized plasmonic antenna effect with significantly enhanced optical field vectors with control of both \textit{in-plane} and \textit{out-of-plane} components. We use the resulting vector-field specificity in the symmetry selective nonlinear optical response of second-harmonic generation (SHG) for a generalized approach to optical nano-crystallography and -imaging. In tip-enhanced SHG imaging of monolayer MoS$_2$ films and single-crystalline ferroelectric YMnO$_3$, we reveal nano-crystallographic details of domain boundaries and domain topology with enhanced sensitivity and nanoscale spatial resolution. The approach is applicable to any anisotropic linear and nonlinear optical response, and provides for optical nano-crystallographic imaging of molecular or quantum materials.

physics.optics↗

arXiv2017

Radiative control of dark excitons at room temperature by nano-optical antenna-tip induced Purcell effect

Excitons, Coulomb-bound electron and hole pairs, are elementary photo-excitations in semiconductors, that can couple directly to light through radiative relaxation. In contrast to these bright excitons, dark excitons X$\rm{_D}$ with anti-parallel electron spin polarization exist, with generally forbidden radiative emission. Because of their associated long lifetimes, these dark excitons are appealing candidates for quantum computing and opto-electronic devices. However, optical read-out and control of X$\rm{_D}$ states have remained a major challenge due to their decoupling from light. Here, we present a novel tip-enhanced nano-optical approach to precisely switch and programmably modulate the X$\rm{_D}$ emission even at room temperature. Using monolayer two-dimensional transition metal dichalcogenide (TMD) WSe$\rm{_2}$ on a gold film as model system, we demonstrate ${\sim} 6 \times 10^5$-fold enhancement in dark exciton photoluminescence quantum yield. This is achieved by the unique coupling of the nano-optical antenna-tip to the dark exciton \textit{out-of-plane} optical dipole moment, with an extraordinary Purcell factor of $\ge 2 \times 10^3$ of the tip-sample nano-cavity. Compared to the necessity of cryogenic temperatures and high magnetic fields in conventional approaches, our work provides a new way to harness excitonic properties in low-dimensional semiconductors and new strategies for quantum opto-electronic devices.

cond-mat.mtrl-sci↗

arXiv2016

Hybrid tip-enhanced nano-spectroscopy and -imaging of monolayer WSe2 with local strain control

Many classes of two-dimensional (2D) materials have emerged as potential platforms for novel electronic and optical devices. However, the physical properties are strongly influenced by nanoscale heterogeneities in the form of edges, grain boundaries, and nucleation sites. Using combined tip-enhanced Raman scattering (TERS) and photoluminescence (TEPL) nano-spectroscopy and -imaging, we study the associated effects on the excitonic properties in monolayer WSe2 grown by physical vapor deposition (PVD). With <15 nm spatial resolution we resolve nonlocal nanoscale correlations of PL spectral intensity and shifts with crystal edges and internal twin boundaries associated with the expected exciton diffusion length. Through an active atomic force tip interaction we can control the crystal strain on the nanoscale, and tune the local bandgap in reversible (up to 24 meV shift) and irreversible (up to 48 meV shift) fashion. This allows us to distinguish the effect of strain from the dominant influence of defects on the PL modification at the different structural heterogeneities. Hybrid nano-optical and nano-mechanical imaging and spectroscopy thus enables the systematic study of the coupling of structural and mechanical degrees of freedom to the nanoscale electronic and optical properties in layered 2D materials.

physics.optics↗