Lattice reconstruction and corresponding strain accumulation plays a key role in defining the electronic structure of two-dimensional moiré superlattices, including those of transition metal dichalcogenides (TMDs). Imaging of TMD moirés has so far provided a qualitative understanding of this relaxation process in terms of interlayer stacking energy, while models of the underlying deformation mechanisms have relied on simulations. Here, we use interferometric four-dimensional scanning transmission electron microscopy to quantitatively map the mechanical deformations through which reconstruction occurs in small-angle twisted bilayer MoS2and WSe2/MoS2heterobilayers. We provide direct evidence that local rotations govern relaxation for twisted homobilayers, while local dilations are prominent in heterobilayers possessing a sufficiently large lattice mismatch. Encapsulation of the moiré layers in hBN further localizes and enhances these in-plane reconstruction pathways by suppressing out-of-plane corrugation. We also find that extrinsic uniaxial heterostrain, which introduces a lattice constant difference in twisted homobilayers, leads to accumulation and redistribution of reconstruction strain, demonstrating another route to modify the moiré potential.
Interlayer excitons (IXs) in MoSe2–WSe2heterobilayers have generated interest as highly tunable light emitters in transition metal dichalcogenide (TMD) heterostructures. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. We show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2–WSe2region to those in a region separated by bilayer hBN. The doping, electric field, and temperature dependence of the narrow IX lines are similar for both regions, but their excitonic g-factors have opposite signs, indicating that the origin of narrow IX PL is not the moiré potential.
- Publication Date:
- NSF-PAR ID:
- 10371619
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Publisher:
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
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Abstract Transition metal dichalcogenide (TMD) semiconductor heterostructures are actively explored as a new platform for quantum optoelectronic systems. Most state of the art devices make use of insulating hexagonal boron nitride (hBN) that acts as a wide-bandgap dielectric encapsulating layer that also provides an atomically smooth and clean interface that is paramount for proper device operation. We report the observation of large, through-hBN photocurrents that are generated upon optical excitation of hBN encapsulated MoSe 2 and WSe 2 monolayer devices. We attribute these effects to Auger recombination in the TMDs, in combination with an asymmetric band offset between the TMD and the hBN. We present experimental investigation of these effects and compare our observations with detailed, ab-initio modeling. Our observations have important implications for the design of optoelectronic devices based on encapsulated TMD devices. In systems where precise charge-state control is desired, the out-of-plane current path presents both a challenge and an opportunity for optical doping control. Since the current directly depends on Auger recombination, it can act as a local, direct probe of both the efficiency of the Auger process as well as its dependence on the local density of states in integrated devices.
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Abstract Moiré coupling in transition metal dichalcogenides (TMDCs) superlattices introduces flat minibands that enable strong electronic correlation and fascinating correlated states, and it also modifies the strong Coulomb-interaction-driven excitons and gives rise to moiré excitons. Here, we introduce the layer degree of freedom to the WSe2/WS2moiré superlattice by changing WSe2from monolayer to bilayer and trilayer. We observe systematic changes of optical spectra of the moiré excitons, which directly confirm the highly interfacial nature of moiré coupling at the WSe2/WS2interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe2/monolayer WS2moiré superlattice. The additional WSe2layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe2layer(s). The layer dependence of both moiré excitons and correlated electronic states can be well described by our theoretical model. Our study presents a new method to tune the strong electronic correlation and moiré exciton bands in the TMDCs moiré superlattices, ushering in an exciting platform to engineer quantum phenomena stemming from strong correlation and Coulomb interaction.
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