arXiv subjects

Timur O. Shegai

Publications and source records attributed to Timur O. Shegai.

13 recordsLinked to original sources

arXiv2026

Precise one-dimensional nanochannels in transition metal dichalcogenides as building blocks for advanced nanophotonics

Atomically sharp edges are essential for future high-index nanophotonic structures, yet conventional lithography and dry etching methods inevitably introduce edge roughness that limits optical confinement and reproducibility. Recently, anisotropic wet etching of multilayer van der Waals crystals, such as transition metal dichalcogenides (TMDs), has enabled crystallographically defined, atomically sharp zigzag edges, eliminating the edge-roughness problem. However, the process is intrinsically limited to confined geometries such as isolated triangular or hexagonal features dictated by crystal stacking symmetry. Here, we demonstrate a lithography-guided anisotropic etching framework that drives TMDs etching beyond isolated confined geometries by enforcing controlled interaction of neighboring etched nanoholes regions. In multilayer 2H-WS2, merging of anisotropic etch fronts enables sustained long-range propagation of zigzag facets, introducing a previously inaccessible 180-degree edge alignment and a crystallographically defined design space combining 120-degree and 180-degree junctions. Using this approach, we fabricate extended nanophotonic structures with ultrasharp sidewalls, including sub-100-nm-gap one-dimensional gratings, waveguides, defect-engineered photonic cavities, angle programmed photonic lattices, and diffractive zone plates. Back-focal-plane reflection spectroscopy of atomically sharp 1D periodic 2H-WS2 gratings demonstrates their photonic functionality, revealing symmetry-protected bound states in the continuum (SP-BICs) and strong exciton-photon coupling in multilayer WS2. Finally, we fabricate ultrathin, ultranarrow, and ultralong nanoribbons with record-high aspect ratios. Together, these results demonstrate edge merging as a generic route to fabricate edge-defined, atomically sharp nanophotonic and nanoelectronic architectures in layered van der Waals platforms.

physics.optics↗

arXiv2026

Raman scattering of phonon polaritons under nanoscale confinement: the role of structure and environment

Strong light-matter coupling gives rise to polaritons -- quasiparticles that combine both photonic and material characteristics. Here, we show that polar nanocrystals exhibit structure- and environment-dependent Raman scattering, enabled by their hybrid phonon polariton nature. Such dispersive behavior enables refractive index sensing in the mid-infrared range via visible-wavelength inelastic spectroscopy and draws parallels with molecular systems under vibrational strong coupling. Crucially, Raman scattering appears only under nanoscale confinement of phonon polaritons. For optimal structures, this leads to self-hybridization between localized phonon modes and surface phonon polaritons hosted by the same nanoparticle.

physics.optics↗

arXiv2025

Casimir-Lifshitz Theory for Cavity Modification of Ground-State Energy

A theory for ground-state modifications of matter embedded in a Fabry-Perot cavity and whose excitations are described as harmonic oscillators is presented. Based on Lifshitz's theory for vacuum energy and employing a Lorentz model for the material permittivity, a nonperturbative macroscopic QED model that accounts for the infinite number of cavity modes with a continuum of their wavevectors was built. Differences from the commonly used single-mode Hopfield Hamiltonian are revealed. The nonresonant role of polaritons in the ground-state energy shift is also demonstrated, showing that the cavity effect is mainly caused by static screening occurring at very low frequencies. The theory allows for a straightforward incorporation of losses and temperature effects.

quant-ph↗

arXiv2024

Humidity-enhanced NO$_2$ gas sensing using atomically sharp edges in multilayer MoS$_2$

Ambient humidity poses a significant challenge in the development of practical room temperature NO$_2$ gas sensors. Here, we employ atomically precise zigzag edges in multilayer MoS$_2$, fabricated using electron beam lithography and anisotropic wet etching, to achieve highly sensitive and selective gas sensing performance that is humidity-tolerant at elevated temperatures and humidity-enhanced at room temperature under ultraviolet illumination. Notably, exposure to 2.5 parts per billion (ppb) NO$_2$ at 70% relative humidity under ultraviolet illumination and at room-temperature resulted in a 33-fold increase in response and a 6-fold faster recovery compared to 0% relative humidity, leading to response values exceeding 1100%. The optimized samples demonstrated a theoretical detection limit ranging from 4 to 400 parts per trillion (ppt) NO$_2$. The enhanced NO$_2$ sensing capabilities of MoS$_2$ edges have been further confirmed through first-principles calculations. Our study expands the applications of nanostructured MoS$_2$ and highlights its potential for detecting NO$_2$ at sub-ppb levels in complex scenarios, such as high humidity conditions.

physics.app-ph↗

arXiv2024

Ultrathin 3R-MoS$_2$ metasurfaces with atomically precise edges for efficient nonlinear nanophotonics

Dielectric metasurfaces that combine high-index materials with optical nonlinearities are widely recognized for their potential in various quantum and classical nanophotonic applications. However, the fabrication of high-quality metasurfaces poses significant material-dependent challenges, as their designs are often susceptible to disorder, defects, and scattering losses, which are particularly prone to occur at the edges of nanostructured features. Additionally, the choice of the material platforms featuring second-order optical nonlinearities, $χ^{(2)}$, is limited to broken-inversion symmetry crystals such as GaAs, GaP, LiNbO$_3$, and various bulk van der Waals materials, including GaSe and NbOCl$_2$. Here, we use a combination of top-down lithography and anisotropic wet etching of a specially stacked van der Waals crystal -- 3R-MoS$_2$, which exhibits both a high refractive index and exceptional $χ^{(2)}$ nonlinearity, to produce metasurfaces consisting of perfect equilateral triangle nanoholes with atomically precise zigzag edges. Due to the geometry of the triangle, the etching process is accompanied by a transition from an in-plane $C_4$ symmetric structure to a broken-in-plane symmetry configuration, thereby allowing for the realization of the quasi-bound-state-in-the-continuum (q-BIC) concept. The resulting ultrathin metasurface ($\sim$ 20-25 nm) demonstrates a remarkable enhancement in second-harmonic generation (SHG) -- over three orders of magnitude at specific wavelengths and linear polarization directions compared to a host flake.

physics.optics↗

arXiv2024

Defect-assisted reversible phase transition in mono- and few-layer ReS$_2$

Transition metal dichalcogenide (TMD) materials have attracted substantial interest due to their remarkable excitonic, optical, electrical, and mechanical properties, which are highly dependent on their crystal structure. Controlling the crystal structure of these materials is essential for fine-tuning their performance, $\textit{e.g.}$, linear and nonlinear optical, as well as charge transport properties. While various phase-switching TMD materials, like molybdenum telluride (MoTe$_2$), are available, their transitions are often irreversible. Here, we investigate the mechanism of a light-induced reversible phase transition in mono- and bilayer flakes of rhenium disulfide (ReS$_2$). Our observations, based on scanning transmission electron microscopy, nonlinear spectroscopy, and density functional theory calculations, reveal a transition from the ground T$''$ (double distorted T) to the metastable H$'$ (distorted H) phase under femtosecond laser irradiation or influence of highly-energetic electrons. We show that the formation of sulfur vacancies facilitates this phenomenon. Our findings pave the way towards actively manipulating the crystal structure of ReS$_2$ and possibly its heterostructures.

physics.optics↗

arXiv2024

Quantum trapping and rotational self-alignment in triangular Casimir microcavities

Casimir torque -- a rotational motion caused by the minimization of the zero-point energy -- is a problem that attracts significant theoretical and experimental interest. Recently, it has been realized using liquid crystal phases and natural anisotropic substrates. However, for natural materials, the torque reaches substantial values only at van der Waals distances of ~10 nm. Here, we employ Casimir self-assembly using templated gold nanostructures of triangular symmetry for the purpose of rotational self-alignment at truly Casimir distances (100 -- 200 nm separation). The joint action of repulsive electrostatic and attractive Casimir potentials leads to the formation of a stable quantum trap, giving rise to a tunable Fabry-Perot microcavity. This cavity self aligns both laterally and rotationally to maximize the overlap area between the templated and floating triangular flakes. The rotational self-alignment is remarkably sensitive to the equilibrium distance between the two triangles as well as their area, which opens possibilities for active control through manipulating the electrostatic screening. Our self-assembled and self-aligned Casimir microcavities could find future use as a versatile and tunable platform for nanophotonic, polaritonic, and optomechanical applications.

cond-mat.mes-hall↗

arXiv2023

Self-hybridized vibrational-Mie polaritons in water droplets

We study the self-hybridization between Mie modes supported by water droplets with stretching and bending vibrations in water molecules. Droplets with radii $>2.7~μm$ are found to be polaritonic on the onset of the ultrastrong light-matter coupling regime. Similarly, the effect is observed in larger deuterated water droplets at lower frequencies. Our results indicate that polaritonic states are ubiquitous in nature and occur in water droplets in mists, fogs, and clouds. This finding may have implications not only for polaritonic physics but also for aerosol and atmospheric sciences.

physics.optics↗

arXiv2023

Probing optical anapoles with fast electron beams

Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far. Here, we theoretically and experimentally analyze the excitation of optical anapoles in tungsten disulfide (WS$_2$) nanodisks using Electron Energy Loss Spectroscopy (EELS) in Scanning Transmission Electron Microscopy (STEM). We observe prominent dips in the electron energy loss spectra and associate them with the excitation of optical anapoles and anapole-exciton hybrids. We are able to map the anapoles excited in the WS$_2$ nanodisks with subnanometer resolution and find that their excitation can be controlled by placing the electron beam at different positions on the nanodisk. Considering current research on the anapole phenomenon, we envision EELS in STEM to become a useful tool for accessing optical anapoles appearing in a variety of dielectric nanoresonators.

physics.optics↗

arXiv2022

Nanostructured transition metal dichalcogenide multilayers for advanced nanophotonics

Transition metal dichalcogenides (TMDs) attract significant attention due to their exceptional optical, excitonic, mechanical, and electronic properties. Nanostructured multilayer TMDs were recently shown to be highly promising for nanophotonic applications, as motivated by their exceptionally high refractive indexes and optical anisotropy. Here, we extend this vision to more sophisticated structures, such as periodic arrays of nanodisks and nanoholes, as well as proof-of-concept waveguides and resonators. We specifically focus on various advanced nanofabrication strategies, including careful selection of resists for electron beam lithography and etching methods. The specific materials studied here include semiconducting WS$_2$, in-plane anisotropic ReS$_2$, and metallic TaSe$_2$, TaS$_2$ and NbSe$_2$. The resulting nanostructures can potentially impact several nanophotonic and optoelectronic areas, including high-index nanophotonics, plasmonics and on-chip optical circuits. The knowledge of TMD material-dependent nanofabrication parameters developed here will help broaden the scope of future applications of these materials in all-TMD nanophotonics.

physics.optics↗

arXiv2020

Enhancing vibrational light-matter coupling strength beyond the molecular concentration limit using plasmonic arrays

Vibrational strong coupling is emerging as a promising tool to modify molecular properties, by making use of hybrid light-matter states known as polaritons. Fabry-Perot cavities filled with organic molecules are typically used, and the molecular concentration limits the maximum reachable coupling strength. Developing methods to increase the coupling strength beyond the molecular concentration limit are highly desirable. In this letter, we investigate the effect of adding a gold nanorod array into a cavity containing pure organic molecules, using FT-IR microscopy and numerical modeling. Incorporation of the plasmonic nanorod array, that acts as artificial molecules, leads to an order of magnitude increase in the total coupling strength for the cavity filled with organic molecules. Additionally, we observe a significant narrowing of the plasmon linewidth inside the cavity. We anticipate that these results will be a step forward in exploring vibropolaritonic chemistry and may be used in plasmon based bio-sensors.

physics.optics↗

arXiv2020

Transition metal dichalcogenide metamaterials with atomic precision

The ability to extract materials just a few atoms thick has led to discovery of graphene, monolayer transition metal dichalcogenides (TMDs), and other important two-dimensional materials. The next step in promoting understanding and utility of the flatland physics beyond the state-of-the-art is to study one-dimensional edges of such two-dimensional materials as well as to control the edge-plane ratio. Edges typically exhibit properties that are unique and distinctly different from those of planes and bulk. Thus, controlling them allows to design principally new materials with synthetic edge-plane-bulk characteristics, that is, TMD metamaterials. However, the enabling technology to study such metamaterials experimentally in a precise and systematic way has not yet been developed. Here we report a facile and controllable anisotropic wet etching method that allows scalable fabrication of TMD metamaterials with atomic precision. We show that TMDs can be etched along certain crystallographic axes, such that the obtained edges are atomically sharp and exclusively zigzag-terminated. This results in hexagonal nanostructures of predefined order and complexity, including few nanometer thin nanoribbons and nanojunctions. The method thus enables future studies of a broad range of TMD metamaterials with tailored functionality through atomically precise control of the structure.

physics.app-ph↗

arXiv2019

Single-particle Mie-resonant all-dielectric nanolasers

All-dielectric subwavelength structures utilizing Mie resonances provide a novel paradigm in nanophotonics for controlling and manipulating light. So far, only spontaneous emission enhancement was demonstrated with single dielectric nanoantennas, whereas stimulated emission was achieved only in large lattices supporting collective modes. Here, we demonstrate the first single-particle all-dielectric monolithic nanolaser driven by Mie resonances in visible and near-IR frequency range. We employ halide perovskite CsPbBr$_3$ as both gain and resonator material that provides high optical gain (up to $\sim 10^4$ cm$^{-1}$) and allows simple chemical synthesis of nanocubes with nearly epitaxial quality. Our smallest non-plasmonic Mie-resonant single-mode nanolaser with the size of 420 nm operates at room temperatures and wavelength 535 nm with linewidth $\sim 3.5$ meV. These novel lasing nanoantennas can pave the way to multifunctional photonic designs for active control of light at the nanoscale.

physics.optics↗