We report a novel optical property in WS2 monolayer. The monolayer naturally exhibits beautiful in-plane periodical and lateral homojunctions by way of alternate dark and bright band in the fluorescence images of these monolayers. The interface between different fluorescence species within the sample is distinct and sharp. This gives rise to intriguing concentric triangular fluorescence patterns in the monolayer. The novel optical property of this special WS2 monolayer is facilitated by chemical heterogeneity. The photoluminescence of the bright band is dominated by emissions from trion and biexciton while the emission from defect-bound exciton dominates the photoluminescence at the dark band. The discovery of such concentric fluorescence patterns represents a potentially new form of optoelectronic or photonic functionality.
Using wide spectral range in situ spectroscopic ellipsometry with systematic ultra high vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS2 isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A (1.92 eV) and B (2.02 eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the bandstructure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This work unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS2.
We clarify that the chemisorption of oxygen atoms at the edges is a key contributor to the frequently observed edge enhancement and spatial non-uniformities of photoluminescence (PL) in WS2 monolayers. Here we have investigated with momentum- and real-space nanoimaging of the chemical and electronic density inhomogeneity of WS2 flakes. Our finding from a large panoply of techniques together with density functional theory calculation confirms that the oxygen chemisorption leads to the electron accumulation at the edges. This facilitates the trion dominance of PL at the edges of WS2 flakes. Our results highlight and unravel the significance of chemisorbed oxygen at the edges in the PL emission and electronic structure of WS2, providing a viable path to enhance the performance of transition-metal-dichalcogenide-based devices.
Platinum dichalcogenide (PtX 2 ), an emergent group-10 transition metal dichalcogenide (TMD) has shown great potential in infrared photonic and optoelectronic applications due to its layer-dependent electronic structure with potentially suitable bandgap. However, a scalable synthesis of PtSe 2 and PtTe 2 atomic layers with controlled thickness still represents a major challenge in this field because of the strong interlayer interactions. Herein, we develop a facile cathodic exfoliation approach for the synthesis of solution-processable high-quality PtSe 2 and PtTe 2 atomic layers for high-performance infrared (IR) photodetection. As-exfoliated PtSe 2 and PtTe 2 bilayer exhibit an excellent photoresponsivity of 72 and 1620 mA W −1 at zero gate voltage under a 1540 nm laser illumination, respectively, approximately several orders of magnitude higher than that of the majority of IR photodetectors based on graphene, TMDs, and black phosphorus. In addition, our PtSe 2 and PtTe 2 bilayer device also shows a decent specific detectivity of beyond 10 9 Jones with remarkable airstability (>several months), outperforming the mechanically exfoliated counterparts under the laser illumination with a similar wavelength. Moreover, a high yield of PtSe 2 and PtTe 2 atomic layers dispersed in solution also allows for a facile fabrication of airstable wafer-scale IR photodetector. This work demonstrates a new route for the synthesis of solution-processable layered materials with the narrow bandgap for the infrared optoelectronic applications.
We present scanning focused laser beam as a multipurpose tool to engineer the physical and chemical properties of WS microflakes. For monolayers, the laser modification integrates oxygen into the WS microflake, resulting in ∼9 times enhancement in the intensity of the fluorescence emission. This modification does not cause any morphology change, allowing "micro-encryption" of information that is only observable as fluorescence under excitation. The same focused laser also facilitates on demand thinning down of WS multilayers into monolayers, turning them into fluorescence active components. With a scanning focused laser beam, micropatterns are readily created on WS multilayers through selective thinning of specific regions on the flake.
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