arXiv subjects

Jeong Hyun Han

Publications and source records attributed to Jeong Hyun Han.

4 recordsLinked to original sources

arXiv2026

Broadband Single-Particle Absorption Circular Dichroism Reveals Chiroptical Heterogeneity in Gold Helicoids

Quantitative measurements of absorption circular dichroism (CD) at the single-particle level are essential for understanding how individual chiral nanostructures dissipate optical energy, yet broadband absorptance measurements remain experimentally challenging. Here, we introduce a wavelength-tunable integrating-sphere microscope that determines the absorptance of individual nanoparticles under right- and left-circularly polarized illumination through direct optical energy balance, enabling broadband measurement of the absorption dissymmetry factor, gabs. Measurements of achiral gold nanospheres and strongly anisotropic gold nanorods establish the apparent absorption CD baseline and demonstrate minimal detectable linear-dichroism-to-circular-dichroism (LD-to-CD) leakage under the experimental conditions. Applying this approach to 87 chiral gold helicoids synthesized using L-glutathione (L-helicoids) and 96 synthesized using D-glutathione (D-helicoids) reveals mean particle-level gabs values of opposite sign, with a statistically significant difference between the two populations. Individual particles nevertheless exhibit pronounced heterogeneity in response sign, magnitude, spectral position, and line shape. More than one-third of the particles in each population display opposite-sign absorption CD responses relative to their population-average tendency. Correlative SEM analysis of the L-helicoid population further shows that opposite-sign responses persist among isolated particles exhibiting the characteristic projected helicoid morphology, indicating that aggregation and gross differences in projected morphology are insufficient to explain the observed heterogeneity. These results establish broadband single-particle absorption CD spectroscopy as a direct probe of absorptive chiroptical heterogeneity and reveal particle-specific responses obscured by ensemble averaging.

physics.optics↗

arXiv2026

Helicity-Resolved Spatiotemporal Mapping of Chiral Plexcitons in Helicoids

Plasmon-exciton hybrids, or plexcitons, offer deeply subwavelength light-matter interactions with versatile pathways for energy redistribution. Incorporating chirality into such systems is particularly compelling, enabling spin-sensitive optical functionality that can operate on ultrafast timescales and within ultracompact volumes. Despite recent progress in chiral plexcitonic systems, how structural chirality and plasmon-exciton coupling determine chiroptical spectra and ultrafast energy flow remains elusive. Here we realize chiral plexcitons by functionalizing intrinsically chiral gold helicoid nanoparticles with molecular J-aggregates. Within a non-Hermitian framework, we trace the microscopic origin of the helicoid chiroptical response and its coupling to the excitonic transition, revealing how the helicity of light selectively addresses distinct hybrid responses. At the spatiotemporal extreme, we find that the gap-localized response not only enhances polarization-sensitive contrast but also strengthens the local hybrid interaction, leading to accelerated ultrafast relaxation. Together, these space-, time-, and polarization-resolved measurements provide a physically grounded and experimentally benchmarked picture of chiral plexcitonic coupling, identifying chirality as a practical control parameter for selectively steering nanoscale energy pathways and dynamics.

physics.optics↗

arXiv2025

Broadband ultrafast self-heterodyned chiro-optical spectroscopy

Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 $μ$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics.

physics.optics↗

arXiv2022

Strain and Crystallographic Identification of the Helically Concaved Surfaces of Nanoparticles

Identifying the three-dimensional (3D) crystal-plane and strain-field distributions of nanocrystals is essential for optical, catalytic, and electronic applications. Here, we developed a methodology for visualizing the 3D information of chiral gold nanoparticles with concave gap structures by Bragg coherent X-ray diffraction imaging. The distribution of the high-Miller-index planes constituting the concave chiral gap was precisely determined. The highly strained region adjacent to the chiral gaps was resolved, which was correlated to the 432-symmetric morphology of the nanoparticles and its corresponding plasmonic properties were numerically predicted from the atomically defined structures. This approach can serve as a general characterization platform for visualizing the 3D crystallographic and strain distributions of nanoparticles, especially for applications where structural complexity and local heterogeneity are major determinants, as exemplified in plasmonics.

cond-mat.mtrl-sci↗