Searcharxiv⌕ Search
Home/Archive/arXiv

arXiv · 2603.18230

Direct observation of ultrafast defect-bound and free exciton dynamics in defect-engineered WS$_2$ monolayers

Tae Gwan Park·Xufan Li·Kyungnam Kang·Austin Houston·Liam Collins·Gerd Duscher·David B. Geohegan·Christopher M. Rouleau·Kai Xiao·Alexander A. Puretzky
View original source ↗Read source document ↗Export metadata ↓

Abstract

Defects in two-dimensional transition metal dichalcogenides (TMDCs) broadly affect their optical and electronic properties. Directly capturing the ultrafast processes of exciton trapping and defect-bound exciton formation is crucial for understanding and advancing defect-mediated optoelectronics and quantum technologies. However, the weak transient optical absorption of defect-bound excitons has limited their experimental observation to date. Here, we report the direct observation of the ultrafast dynamics of defect-bound excitons in monolayer WS$_2$ crystals with a high density of mono-sulfur vacancies (V$_S$) and W-site defect complexes (S$_W$V$_S$) resulting from synthesis by alkali metal halide-assisted chemical vapor deposition. The dynamics of excitons bound to these defects, along with their coherent interactions with free excitons, are elucidated using ultrafast optical spectroscopy. Using above band-edge photoexcitation, we find that both free and defect-bound excitons simultaneously form within 300 fs from hot carrier relaxation. The defect-bound excitons exhibit shorter lifetimes than free excitons, leading to a population difference of the corresponding excitonic states and free exciton trapping within a 1--100 ps window. Band-edge photoexcitation of free and defect-bound exciton states reveals ultrafast interconversion within ~150 fs (comparable to our temporal resolution), indicating possible coherent coupling between these states. We further demonstrate efficient up-conversion of defect-bound excitons to free excitons with photon energies up to ~300 meV below the free exciton resonance. These findings provide insights into the ultrafast dynamics of defect-bound excitons in TMDCs and their coupling with free excitons, which are relevant to defect-engineered optoelectronic, quantum photonic, and valleytronic applications.

Explore related subjects

physics.opticscond-mat.mes-hallcond-mat.mtrl-sci

Keep this discovery

BibTeXRIS

Tae Gwan Park, Xufan Li, Kyungnam Kang, Austin Houston, Liam Collins, Gerd Duscher, David B. Geohegan, Christopher M. Rouleau, Kai Xiao, Alexander A. Puretzky. 2026-03-18. Direct observation of ultrafast defect-bound and free exciton dynamics in defect-engineered WS$_2$ monolayers. https://doi.org/10.1021/acsnano.5c18559

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

arXiv2026

Two-step high-accuracy microwave frequency measurement and time-frequency analysis based on optical frequency combs

Broadband microwave frequency measurement and time-frequency analysis are crucial for applications such as electronic warfare. However, when it comes to ultra wideband signal analysis, traditional electronic methods have high analysis accuracy, but intrinsic electronic bottlenecks limit their real-time analysis. Here, we propose and experimentally demonstrate a two-step microwave frequency measurement and time-frequency analysis method based on optical frequency combs. The system first performs coarse frequency localization over the 0-40 GHz range using stimulated-Brillouin-scattering-assisted frequency-to-time mapping (FTTM) and dual-comb channelized reception. The dual-comb is then reapplied for downconverting the signal under test, followed by digital signal processing to achieve high-accuracy unambiguous frequency extraction. Experimental results show that the system achieves mean single-tone frequency measurement errors of less than 10 kHz over 0-40 GHz. We further experimentally measure multi-tone, linearly frequency-modulated, and V-shaped frequency-modulated signals, demonstrating the proposed method's capability for analyzing complex signals.

physics.optics↗
arXiv2026

A Two-Mirror Faceted Projection System for EUV Lithography

We propose an all-reflective two-mirror projection system for extreme ultraviolet (EUV) lithography operating at exposure wavelengths of $13.5$~nm (Mo/Si) and $11.2$~nm (Ru/Be), delivering a fourfold ($4\times$) demagnification of the periodic mask pattern at a numerical aperture approaching unity ($\mathrm{NA}_{\max} \approx 0.993$). In contrast to conventional EUV projection objectives that incorporate 6--10 aspheric mirrors with an overall optical throughput of less than $15\%$, the proposed design redirects each accepted discrete spatial diffraction order scattered by the mask onto the wafer via a dedicated pair of planar mirror facets. The number of reflections is strictly fixed at two for all accepted orders, retaining $50$--$60\%$ of the power leaving the mask in each accepted order. We derive a spatial geometry providing rigorous optical path length equalization across all diffraction orders, thereby removing order-dependent propagation phase shifts. Individually optimized 30-bilayer Bragg multilayer coatings are designed for each facet using the transfer matrix method combined with global evolutionary optimization algorithms. The architecture is generalized to a three-dimensional vector formulation with a two-dimensionally periodic mask. Utilizing inverse lithography technology, Fourier parameterization, and a differentiable electromagnetic modal waveguide solver, we solve the synthesis problem for binary absorber masks (La absorber on a Ru/Be/Sr multilayer mirror). We demonstrate simulated aerial images of sub-10-nm features on the wafer (isolated peaks with a full width at half maximum (FWHM) of approximately $5.4$~nm and line pairs with a critical dimension of $6$~nm) and find that the two peaks remain resolved for the tested wafer defocus values from $0$ to $5$~nm along the $z$-axis.

physics.optics↗
arXiv2026

Antimony for broadband nanophotonics across the ultraviolet, visible and infrared

Semimetal elemental antimony (Sb) nanostructures show great potential for applications where nanophotonic properties play a key role, such as phase-change optical memories, non-linear optical elements, photothermal therapy agents, photodetectors and photocatalysts. However, designing advanced Sb-based photonic devices critically requires an accurate and reliable knowledge of the optical response of bulk and nanoscale Sb. Herein, we report for the first time a fully consistent and accurately measured dielectric function for Sb nanoscale films in a wide spectral range from the ultraviolet to the far infrared (4 - 0.04 eV, i.e. ~ 0.3 - 30 $\mu$m), surpassing previous reports that explored a limited spectral range. It is found that the Sb spectral response is driven exclusively by giant interband transitions in the visible up to mid infrared (4 - 0.4 eV, i.e. ~ 0.3 - 3 $\mu$m), and that their contribution dominates over that of free carriers down to 0.12 eV (i.e. ~ 10 $\mu$m). Such spectral response enables Sb nanostructures to display spectrally selective and tunable nanophotonic resonances. First, we showcase interband plasmonic resonances in the visible-to-near infrared for Sb nanogratings. Second, we report giant refractive index dielectric resonances in the mid infrared for nanostructured Sb/dielectric/metal resonant cavities. These findings open a pathway to optimized planar Sb nanoscale designs enabling a tailored light-matter interaction, which will be useful for integrated data, telecom, medical, optoelectronic and energy conversion devices operating in a broad spectral range.

physics.optics↗