Ana P. M. Barboza | Searcharxiv

arXiv2026

Resonance-Enhanced Four-Wave Mixing Imaging for Mapping Defect Regions in Vanadium-Doped WS2 Monolayers

Defect engineering is crucial for tuning 2D transition metal dichalcogenide properties for quantum and optoelectronic applications. While conventional photoluminescence (PL) and Raman spectroscopies are important characterization tools, their mapping in large area samples can be time-consuming and lacks direct sensitivity for comprehensive defect characterization. Here, we introduce resonance-enhanced four-wave mixing (FWM) imaging for precise imaging and characterization of vanadium-induced defect states in WS2 monolayers. Our multi-modal investigation, integrating hyperspectral PL, Raman, and supported by density functional calculations, reveals nanoscale doping inhomogeneities, their influence on excitonic and vibrational properties. We observe resonance-enhanced FWM signals correlating with vanadium-induced defect regions, evidencing their unique nonlinear optical response. This work establishes FWM as an essential platform for high-resolution, defect-sensitive imaging, advancing defect-engineered excitonic devices and enabling novel nonlinear quantum photonics.

cond-mat.mes-hall↗

arXiv2024

Nano-optical investigation of grain boundaries, strain and edges in CVD grown MoS$_{2}$ monolayers

The role of defects in two-dimensional semiconductors and how they affect the intrinsic properties of these materials have been a wide researched topic over the past decades. Optical characterization such as photoluminescence and Raman spectroscopies are important tools to probe their physical properties and the impact of defects. However, conventional optical techniques present a spatial resolution limitation lying in a $μ$m-scale, which can be overcomed by the use of near-field optical measurements. Here, we use tip-enhanced photoluminescence and Raman spectroscopies to unveil nanoscale optical heterogeneities at grain boundaries, local strain fields and edges in grown MoS$_{2}$ monolayers. A noticeable enhancement of the exciton peak intensity corresponding to a trion emission quenching is observed at narrow regions down to 47 nm of width at grain boundaries related to doping effects. Besides, localized strain fields inside the sample lead to non-uniformities in the intensity and energy position of photoluminescence peaks. Finally, distinct samples present different nano-optical responses at their edges due to strain and passivation defects. The passivated defective edges show a photoluminescence intensity enhancement and energy blueshift as well as a frequency blueshift of the 2LA Raman mode. On the other hand, the strained edges display a photoluminescence energy redshift and frequency redshifts for E$_{2g}$ and 2LA Raman modes. Our work shows that different defect features can be only probed by using optical spectroscopies with a nanometric resolution, thus revealing hindered local impact of different nanoscale defects in two-dimensional materials.

cond-mat.mtrl-sci↗