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Register a new userEnhanced trion emission in monolayer MoSe2 by constructing a type-I van der Waals heterostructure
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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.
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The atomic-level vdW heterostructures have been one of the most interesting quantum material systems, due to their exotic physical properties. The interlayer coupling in these systems plays a critical role to realize novel physical observation and enrich interface functionality. However, there is still lack of investigation on the tuning of interlayer coupling in a quantitative way. A prospective strategy to tune the interlayer coupling is to change the electronic structure and interlayer distance by high pressure, which is a well-established method to tune the physical properties. Here, we construct a high-quality WS2/MoSe2 heterostructure in a DAC and successfully tuned the interlayer coupling through hydrostatic pressure. Typical photoluminescence spectra of the monolayer MoSe2 (ML-MoSe2), monolayer WS2 (ML-WS2) and WS2/MoSe2 heterostructure have been observed and its intriguing that their photoluminescence peaks shift with respect to applied pressure in a quite different way. The intralayer exciton of ML-MoSe2 and ML-WS2 show blue shift under high pressure with a coefficient of 19.8 meV/GPa and 9.3 meV/GPa, respectively, while their interlayer exciton shows relative weak pressure dependence with a coefficient of 3.4 meV/GPa. Meanwhile, external pressure helps to drive stronger interlayer interaction and results in a higher ratio of interlayer/intralayer exciton intensity, indicating the enhanced interlayer exciton behavior. The first-principles calculation reveals the stronger interlayer interaction which leads to enhanced interlayer exciton behavior in WS2/MoSe2 heterostructure under external pressure and reveals the robust peak of interlayer exciton. This work provides an effective strategy to study the interlayer interaction in vdW heterostructures, which could be of great importance for the material and device design in various similar quantum systems.
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.
The optics of dangling-bond-free van der Waals heterostructures containing transition metal dichalcogenides are dominated by excitons. A crucial property of a confined exciton is the quantum confined Stark effect (QCSE). Here, such a heterostructure is used to probe the QCSE by applying a uniform vertical electric field across a molybdenum disulfide (MoS$_2$) monolayer. The photoluminescence emission energies of the neutral and charged excitons shift quadratically with the applied electric field provided the electron density remains constant, demonstrating that the exciton can be polarized. Stark shifts corresponding to about half the homogeneous linewidth were achieved. Neutral and charged exciton polarizabilities of $(7.8~pm~1.0)times 10^{-10}~tr{D~m~V}^{-1}$ and $(6.4~pm~0.9)times 10^{-10}~tr{D~m~V}^{-1}$ at relatively low electron density ($8 times 10^{11}~tr{cm}^{-2}$) have been extracted, respectively. These values are one order of magnitude lower than the previously reported values, but in line with theoretical calculations. The methodology presented here is versatile and can be applied to other semiconducting layered materials as well.
The promise of high-density and low-energy-consumption devices motivates the search for layered structures that stabilize chiral spin textures such as topologically protected skyrmions. At the same time, layered structures provide a new platform for the discovery of new physics and effects. Recently discovered long-range intrinsic magnetic orders in the two-dimensional van der Waals materials offer new opportunities. Here we demonstrate the Dzyaloshinskii-Moriya interaction and Neel-type skyrmions are induced at the WTe2/Fe3GeTe2 interface. Fe3GeTe2 is a ferromagnetic material with strong perpendicular magnetic anisotropy. We demonstrate that the strong spin orbit interaction in 1T-WTe2 does induce a large interfacial Dzyaloshinskii-Moriya interaction at the interface with Fe3GeTe2 due to the inversion symmetry breaking to stabilize skyrmions. Transport measurements show the topological Hall effect in this heterostructure for temperatures below 100 K. Furthermore, Lorentz transmission electron microscopy is used to directly image Neel-type skyrmions along with aligned and stripe-like domain structure. This interfacial coupling induced Dzyaloshinskii-Moriya interaction is estimated to have a large energy of 1.0 mJ/m^2, which can stabilize the Neel-type skyrmions in this heterostructure. This work paves a path towards the skyrmionic devices based on van der Waals heterostructures.
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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