arXiv subjects

Chun-Chieh Yu

Publications and source records attributed to Chun-Chieh Yu.

3 recordsLinked to original sources

arXiv2026

Subwavelength Coherent Scaling of High-Order Nonlinear Light Generation in Bulk Monolayer MoS2 Thin Films

Monolayer transition metal dichalcogenides (e.g., MoS2) exhibit exceptionally large optical nonlinearities for high-order nonlinear light generation (NLG), yet their inherent atomic thickness fundamentally limits light-matter interactions and thus conversion efficiency. Here, we overcome this intrinsic trade-off using a solution-processed bulk monolayer MoS2 (BM-MoS2) architecture composed of electronically decoupled MoS2 monolayers separated by organic interlayers. This layered superstructure preserves the exceptional intrinsic nonlinear susceptibility of monolayer MoS2 while enabling scalable interaction length. In the subwavelength regime, the NLG scales nearly quadratically with layer number (N1.8), confirming the constructive buildup of nonlinear fields across stacked monolayers. As a result, a 100-nm-thick BM-MoS2 thin film exhibits colossal high-order NLG, including four-wave mixing and high-harmonic generation. The generated nonlinear beam is directly visible to the naked eye and exhibits broad spectral tunability spanning approximately 1000 nm in the mid-IR, enabling mid-IR-to-visible upconversion spectroscopy for resolving molecular vibrational fingerprints. By uniting monolayer-scale nonlinear susceptibility with bulk interaction length and coherent field buildup, BM-MoS2 establishes a thin-film platform for ultra-compact and substrate-agnostic nonlinear photonic systems beyond the constraints of conventional single crystals.

physics.optics↗

arXiv2023

Interfaces Govern Structure of Angstrom-scale Confined Water

Water plays a crucial role in geological, biological, and technological processes. Nanoscale water confinement occurs in many of these settings, including sedimentary rocks, water channel proteins, and applications like desalination and water purification membranes. The structure and properties of water in nanoconfinement can differ significantly from bulk water, exhibiting, for instance, modified hydrogen bonds, dielectric constant, and phase transitions. Despite the importance of strongly nanoconfined water, experimentally elucidating the nanoconfinement effect on water, such as its orientation and hydrogen bond (H-bond) network, has remained challenging. Here, we study two-dimensionally nanoconfined aqueous electrolyte solutions with tunable confinement from nanoscale to angstrom-scale sandwiched between a graphene sheet and CaF2. We employ heterodyne-detection sum-frequency generation (HD-SFG) spectroscopy, a surface-specific vibrational spectroscopy capable of directly and selective probing water orientation and H-bond environment at interfaces and under confinement. Remarkably, the vibrational spectra of the nanoscale confined water can be described quantitatively by the sum of the individual water surface signals from the CaF2/water and water/graphene interfaces until the confinement reduces to angstrom-scale (< ~8 {\AA}). Ab initio molecular dynamics simulations confirm our experimental observation. These results manifest that interfacial, rather than nanoconfinement effects, dominate the water structure until angstrom-level confinement.

physics.chem-ph↗

arXiv2022

Surface-specific vibrational spectroscopy of interfacial water reveals large pH change near graphene electrode at low current densities

Molecular-level insight into interfacial water at buried electrode interfaces is essential in elucidating many phenomena of electrochemistry, but spectroscopic probing of the buried interfaces remains challenging. Here, using surface-specific vibrational spectroscopy, we probe and identify the interfacial water orientation and interfacial electric field at the calcium fluoride (CaF2)-supported electrified graphene/water interface under applied potentials. Our data shows that the water orientation changes drastically at negative potentials (<-0.03 V vs. Pd/H2), from O-H group pointing down towards bulk solution to pointing up away from the bulk solution, which arises from charging/discharging not of the graphene but of the CaF2 substrate. The potential-dependent spectra are nearly identical to the pH-dependent spectra, evidencing that the applied potentials change the local pH (more than five pH units) near the graphene electrode even at a current density below 1 microamp per square centimeter. Our work provides molecular-level insights into the dissociation and reorganization of interfacial water on an electrode/electrolyte interface.

physics.chem-ph↗