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Register a new userNano-optical imaging of monolayer MoSe2-WSe2 lateral heterostructure
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Near-field optical microscopy can be used as a viable route to understand the nanoscale material properties below the diffraction limit. On the other hand, atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDs) are the materials of recent interest to study the spatial confinement of charge carriers, photon, and phonons. Heterostructures based on Mo or W based monolayer TMDs form type-II band alignment, and hence the optically excited carriers can be easily separated for applications pertaining to photonics and electronics. Mapping these spatially confined carriers or photons in a heterostructure with nanoscale resolution as well as their recombination behavior at the interfaces are necessary for the effective use of these materials in future high performance optoelectronics. We performed tip-enhanced photoluminescence (TEPL) imaging to increase the spatial resolution on multi-junction monolayer MoSe2-WSe2 lateral heterostructures grown by chemical vapor deposition (CVD) method. The near-field nano-PL emission map was used to distinguish the presence of distinct crystalline boundaries and the heterogeneities across the interfaces. This method significantly improves the nanoscale resolution of 2D materials, especially for understanding the PL emission properties at the vicinity of hetero-interfaces.
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An emerging class of semiconductor heterostructures involves stacking discrete monolayers such as the transition metal dichalcogenides (TMDs) to form van der Waals heterostructures. In these structures, it is possible to create interlayer excitons (ILEs), spatially indirect, bound electron-hole pairs with the electron in one TMD layer and the hole in an adjacent layer. We are able to clearly resolve two distinct emission peaks separated by 24 meV from an ILE in a MoSe2/WSe2 heterostructure fabricated using state-of-the-art preparation techniques. These peaks have nearly equal intensity, indicating they are of common character, and have opposite circular polarizations when excited with circularly polarized light. Ab initio calculations successfully account for these observations - they show that both emission features originate from excitonic transitions that are indirect in momentum space, are split by spin-orbit coupling, and that including interlayer hybridization is essential in correctly describing the ILE transition. Although well separated in momentum space, we find that in real space the electron has significant weight in both the MoSe2 and WSe2 layers, contrary to the commonly assumed model. This is a significant consideration for understanding the static and dynamic properties of TMD heterostructures.
In this work, we show how domain engineered lithium niobate can be used to selectively dope monolayer MoSe2 and WSe2 and demonstrate that these ferroelectric domains can significantly enhance or inhibit photoluminescence (PL) with the most dramatic modulation occurring at the heterojunction interface between two domains. A micro-PL and Raman system is used to obtain spatially resolved images of the differently doped transition metal dichalcogenides (TMDs). The domain inverted lithium niobate causes changes in the TMDs due to electrostatic doping as a result of the remnant polarization from the substrate. Moreover, the differently doped TMDs (n-type MoSe2 and p-type WSe2) exhibit opposite PL modulation. Distinct oppositely charged domains were obtained with a 9-fold PL enhancement for the same single MoSe2 sheet when adhered to the positive (P+) and negative (P-) domains. This sharp PL modulation on the ferroelectric domain results from different free electron or hole concentrations in the materials conduction band or valence band. Moreover, excitons dissociate rapidly at the interface between the P+ and P- domains due to the built-in electric field. We are able to adjust the charge on the P+ and P- domains using temperature via the pyroelectric effect and observe rapid PL quenching over a narrow temperature range illustrating the observed PL modulation is electronic in nature. This observation creates an opportunity to harness the direct bandgap TMD 2D materials as an active optical component for the lithium niobate platform using domain engineering of the lithium niobate substrate to create optically active heterostructures that could be used for photodetectors or even electrically driven optical sources on-chip.
Trions, quasi-particles consisting of two electrons combined with one hole or of two holes with one electron, have recently been observed in transition metal dichalcogenides (TMDCs) and drawn increasing attention due to potential applications of these materials in light-emitting diodes, valleytronic devices as well as for being a testbed for understanding many-body phenomena. Therefore, it is important to enhance the trion emission and its stability. In this study, we construct a MoSe2/FePS3 van der Waals heterostructure (vdWH) with type-I band alignment, which allows for carriers injection from FePS3 to MoSe2. At low temperatures, the neutral exciton (X0) emission in this vdWH is almost completely suppressed. The ITrion/Ix0 intensity ratio increases from 0.44 in a single MoSe2 monolayer to 20 in this heterostructure with the trion charging state changing from negative in the monolayer to positive in the heterostructure. The optical pumping with circularly polarized light shows a 14% polarization for the trion emission in MoSe2/FePS3. Moreover, forming such type-I vdWH also gives rise to a 20-fold enhancement of the room temperature photoluminescence from monolayer MoSe2. Our results demonstrate a novel approach to convert excitons to trions in monolayer 2D TMDCs via interlayer doping effect using type-I band alignment in vdWH.
We report on nano-optical imaging study of WSe2 thin flakes with the scanning near-field optical microscopy (NSOM). The NSOM technique allows us to visualize in real space various waveguide photon modes inside WSe2. By tuning the excitation laser energy, we are able to map the entire dispersion of these waveguide modes both above and below the A exciton energy of WSe2. We found that all the modes interact strongly with WSe2 excitons. The outcome of the interaction is that the observed waveguide modes shift to higher momenta right below the A exciton energy. At higher energies, on the other hand, these modes are strongly damped due to adjacent B excitons or band edge absorptions. The mode-shifting phenomena are consistent with polariton formation in WSe2.
We report first-principles calculations of the structural and vibrational properties of the synthesized two-dimensional van der Waals heterostructures formed by single-layers dichalcogenides MoSe2 and WSe2. We show that, when combining these systems in a periodic two-dimensional heterostructures, the intrinsic phonon characteristics of the free-standing constituents are to a large extent preserved but, furthermore, exhibit shear and breathing phonon modes that are not present in the individual building blocks. These peculiar modes depend strongly on the weak vdW forces and has a great contibution to the thermal properties of the layered materials. Besides these features, the departure of flexural modes of heterobilayer from the ones of its monolayer parents are also found.
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