Stacked atomically thin transition metal dichalcogenides (TMDs) exhibit fundamentally new physical properties compared to those of the individual layers. The twist angle between the layers plays a crucial role in tuning these properties. Having a tool that provides high-resolution, large area mapping of the twist angle, would be of great importance in the characterization of such 2D structures. Here we use polarization-resolved second harmonic generation (P-SHG) imaging microscopy to rapidly map the twist angle in large areas of overlapping WS2 stacked layers. The robustness of our methodology lies in the combination of both intensity and polarization measurements of SHG in the overlapping region. This allows the accurate measurement and consequent pixel-by-pixel mapping of the twist angle in this area. For the specific case of 30° twist angle, P-SHG enables imaging of individual layers.
Degenerate minima in momentum space—valleys—provide an additional degree of freedom that can be used for information transport and storage. Notably, such minima naturally exist in the band structure of transition metal dichalcogenides (TMDs). When these atomically thin crystals interact with intense laser light, the second harmonic generated (SHG) field inherits special characteristics that reflect not only the broken inversion symmetry in real space but also the valley anisotropy in reciprocal space. The latter is present whenever there exists a valley population imbalance (VPI) between the two valleys and affects the polarization state of the detected SHG. In this work, it is shown that the temperature-induced change of the SHG intensity dependence on the excitation field polarization is a fingerprint of VPI in TMDs. In particular, pixel-by-pixel VPI mapping based on polarization-resolved raster-scanning imaging microscopy was performed inside a cryostat to generate the SHG contrast in the presence of VPI from every point of a TMD flake. The generated contrast is marked by rotation of the SHG intensity polar diagrams at low temperatures and is attributed to the VPI-induced SHG.
The sufficient control of the carrier density of a single layer WS2 (1L-WS2) has been realized by the pulsed laser irradiation doping technique. Chlorine atoms are incorporated on the surface of the atomically thin lattice in a precursor gas atmosphere. In this work, we demonstrate spin-valley polarization tunability by more than 40% in 1L-WS2 on hBN via photochlorination. Polarization photoluminescence spectroscopy was performed in the temperature range from 4 K to 300 K. The decrease in circular polarization after the photochlorination treatment is attributed to the significant reduction of the active defect sites in 1L-WS2 and, consequently, to the increase in the non-radiative exciton lifetime. Ultrafast time-resolved transient absorption spectroscopy measurements support our findings. The above results indicate a useful approach of controlling the density of the active defect sites and the valley polarized light emission in doped monolayer crystal lattices.
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