Kyung-Duk Park

Many classes of two-dimensional (2D) materials have emerged as potential platforms for novel electronic and optical devices. However, their physical properties are strongly influenced by nanoscale heterogeneities in the form of edges, twin boundaries, and nucleation sites. Using combined tip-enhanced Raman scattering and photoluminescence (PL) nanospectroscopy and nanoimaging, we study the associated effects on the excitonic properties in monolayer WSe2 grown by physical vapor deposition. With ∼

Optical cavities can enhance and control light-matter interactions. This level of control has recently been extended to the nanoscale with single emitter strong coupling even at room temperature using plasmonic nanostructures. However, emitters in static geometries, limit the ability to tune the coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) with a nanocavity formed between a scanning plasmonic antenna tip and the substr

Abstract 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 to tune some of these properties, yet dynamic control at the nanoscale with real‐time and ‐space characterizations remains a challenge. Here, a dynamic nano‐mechanic

Structure, dynamics, and coupling involving single-molecules determine function in catalytic, electronic or biological systems. While vibrational spectroscopy provides insight into molecular structure, rapid fluctuations blur the molecular trajectory even in single-molecule spectroscopy, analogous to spatial averaging in measuring large ensembles. To gain insight into intramolecular coupling, substrate coupling, and dynamic processes, we use tip-enhanced Raman spectroscopy (TERS) at variable and

Abstract Photoluminescence (PL), a photo‐excited spontaneous emission process, provides a wealth of optical and electronic properties of materials, which enable microscopic and spectroscopic imaging, biomedical sensing and diagnosis, and a range of photonic device applications. However, conventional far‐field PL measurements have limitations in sensitivity and spatial resolution, especially to investigate single nano‐materials or nano‐scale dimension of them. In contrast, tip‐enhanced photolumin

Understanding and controlling the nanoscale transport of excitonic quasiparticles in atomically thin two-dimensional (2D) semiconductors are crucial to produce highly efficient nano-excitonic devices. Here, we present a nanogap device to selectively confine excitons or trions of 2D transition metal dichalcogenides at the nanoscale, facilitated by the drift-dominant exciton funneling into the strain-induced local spot. We investigate the spatiospectral characteristics of the funneled excitons in

Controlling the propagation and polarization vectors in linear and nonlinear optical spectroscopy enables us 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 nanoprobe in tip-enhanced near-field microscopy. This gives rise to a localized plasmonic antenna effect with significantly enhanced optical field vec

The bilayer grain boundaries (GBs) in chemical-vapor-deposition-grown large-area graphene are identified using multispectral tip-enhanced Raman imaging with 18 nm spatial resolution. The misorientation angle of the bilayer GBs is determined from a quantitative analysis of the phonon-scattering properties associated with the modified electronic structure.

Tip-enhanced nano-spectroscopy and -imaging have significantly advanced our understanding of low-dimensional quantum materials and their interactions with light, providing a rich insight into the underlying physics at their natural length scale. Recently, various functionalities of the plasmonic tip expand the capabilities of the nanoscopy, enabling dynamic manipulation of light-matter interactions at the nanoscale. In this review, we focus on a new paradigm of the nanoscopy, shifting from the c

Abstract In atomically thin semiconductors, localized exciton (X L ) coupled to light provides a new class of optical sources for potential applications in quantum communication. However, in most studies, 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. Hybrid‐modality of cavity‐spectroscopy to induce and probe the X L emissions at the nanoscale in atomically

Dark excitons in transition-metal dichalcogenides, with their long lifetimes and strong binding energies, provide potential platforms from photonic and optoelectronic applications to quantum information science even at room temperature. However, their spatial heterogeneity and sensitivity to strain is not yet understood. Here, we combine tip-enhanced photoluminescence spectroscopy with atomic force induced strain control to nanoimage dark excitons in WSe₂ and their response to local s

Abstract Emerging photo-induced excitonic processes in transition metal dichalcogenide (TMD) heterobilayers, e.g., interplay of intra- and inter-layer excitons and conversion of excitons to trions, allow new opportunities for ultrathin hybrid photonic devices. However, with the associated large degree of spatial heterogeneity, understanding and controlling their complex competing interactions in TMD heterobilayers at the nanoscale remains a challenge. Here, we present an all-round dynamic contro

Abstract The generation of high-purity localized trions, dynamic exciton–trion interconversion, and their spatial modulation in two-dimensional (2D) semiconductors are building blocks for the realization of trion-based optoelectronic devices. Here, we present a method for the all-optical control of the exciton-to-trion conversion process and its spatial distributions in a MoS 2 monolayer. We induce a nanoscale strain gradient in a 2D crystal transferred on a lateral metal–insulator–metal (MIM) w

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 the emission quantum yield of a single pQD. Single CsPbBr_<i>x</i>I_3-<i>x</i> pQDs are clearly resolved through hyperspectral TEPL imaging with ∼10 nm

Abstract 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 diffusio