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1. Shedding light on moiré excitons: A first-principles perspective

   https://doi.org/10.1126/sciadv.abc5638  

   Guo, Hongli; Zhang, Xu; Lu, Gang (October 2020, Science Advances)

   null (Ed.)

   Moiré superlattices in van der Waals (vdW) heterostructures could trap long-lived interlayer excitons. These moiré excitons could form ordered quantum dot arrays, paving the way for unprecedented optoelectronic and quantum information applications. Here, we perform first-principles simulations to shed light on moiré excitons in twisted MoS 2 /WS 2 heterostructures. We provide direct evidence of localized interlayer moiré excitons in vdW heterostructures. The interlayer and intralayer moiré potentials are mapped out based on spatial modulations of energy gaps. Nearly flat valence bands are observed in the heterostructures. The dependence of spatial localization and binding energy of the moiré excitons on the twist angle of the heterostructures is examined. We explore how vertical electric field can be tuned to control the position, polarity, emission energy, and hybridization strength of the moiré excitons. We predict that alternating electric fields could modulate the dipole moments of hybridized moiré excitons and suppress their diffusion in moiré lattices. 

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2. Predictions of moiré excitons in twisted two-dimensional organic–inorganic halide perovskites

   https://doi.org/10.1039/d1sc00359c  

   Zhang, Linghai; Zhang, Xu; Lu, Gang (January 2021, Chemical Science)

   null (Ed.)

   Recent breakthrough in synthesizing arbitrary vertical heterostructures of Ruddlesden–Popper (RP) perovskites opens doors to myriad quantum optoelectronic applications. However, it is not clear whether moiré excitons and flat bands can be formed in such heterostructures. Here, we predict from first principles that twisted homobilayers of RP perovskite, MA 2 PbI 4 , can host moiré excitons and yield flat energy bands. The moiré excitons exhibit unique and hybridized characteristics with electrons confined in a single layer of a striped distribution while holes localized in both layers. Nearly flat valence bands can be formed in the bilayers with relatively large twist angles, thanks to the presence of hydrogen bonds that strengthen the interlayer coupling. External pressures can further increase the interlayer coupling, yielding more localized moiré excitons and flatter valence bands. Finally, electrostatic gating is predicted to tune the degree of hybridization, energy, position and localization of moiré excitons in twisted MA 2 PbI 4 bilayers. 

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3. Tunable strain soliton networks confine electrons in van der Waals materials

   https://doi.org/10.1038/s41567-020-0953-2  

   Edelberg, Drew; Kumar, Hemant; Shenoy, Vivek; Ochoa, Héctor; Pasupathy, Abhay N. (July 2020, Nature Physics)

   Twisting or sliding two-dimensional crystals with respect to each other gives rise to moiré patterns determined by the difference in their periodicities. Such lattice mismatches can exist for several reasons: differences between the intrinsic lattice constants of the two layers, as is the case for graphene on BN; rotations between the two lattices, as is the case for twisted bilayer graphene; and strains between two identical layers in a bilayer. Moiré patterns are responsible for a number of new electronic phenomena observed in recent years in van der Waals heterostructures, including the observation of superlattice Dirac points for graphene on BN, collective electronic phases in twisted bilayers and twisted double bilayers, and trapping of excitons in the moiré potential. An open question is whether we can use moiré potentials to achieve strong trapping potentials for electrons. Here, we report a technique to achieve deep, deterministic trapping potentials via strain-based moiré engineering in van der Waals materials. We use strain engineering to create on-demand soliton networks in transition metal dichalcogenides. Intersecting solitons form a honeycomb-like network resulting from the three-fold symmetry of the adhesion potential between layers. The vertices of this network occur in bound pairs with different interlayer stacking arrangements. One vertex of the pair is found to be an efficient trap for electrons, displaying two states that are deeply confined within the semiconductor gap and have a spatial extent of 2 nm. Soliton networks thus provide a path to engineer deeply confined states with a strain-dependent tunable spatial separation, without the necessity of introducing chemical defects into the host materials. 

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4. Quadrupolar excitons and hybridized interlayer Mott insulator in a trilayer moiré superlattice

   https://doi.org/10.1038/s41467-023-40288-9  

   Lian, Zhen; Chen, Dongxue; Ma, Lei; Meng, Yuze; Su, Ying; Yan, Li; Huang, Xiong; Wu, Qiran; Chen, Xinyue; Blei, Mark; et al (December 2023, Nature Communications)

   Abstract Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe 2 -WS 2 -WSe 2 trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe 2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe 2 layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe 2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions. 

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5. Naturally occurring layered mineral franckeite with anisotropic Raman scattering and third-harmonic generation responses

   https://doi.org/10.1038/s41598-021-88143-5  

   Tripathi, Ravi P.; Gao, Jie; Yang, Xiaodong (December 2021, Scientific Reports)

   Abstract Vertically stacked van der Waals (vdW) heterostructures have introduced a unique way to engineer optical and electronic responses in multifunctional photonic and quantum devices. However, the technical challenges associated with the artificially fabricated vertical heterostructures have emerged as a bottleneck to restrict their proficient utilization, which emphasizes the necessity of exploring naturally occurring vdW heterostructures. As one type of naturally occurring vdW heterostructures, franckeite has recently attracted significant interest in optoelectronic applications, but the understanding of light–matter interactions in such layered mineral is still very limited especially in the nonlinear optical regime. Herein, the anisotropic Raman scattering and third-harmonic generation (THG) from mechanically exfoliated franckeite thin flakes are investigated. The observed highly anisotropic Raman modes and THG emission patterns originate from the low-symmetry crystal structure of franckeite induced by the lattice incommensurability between two constituent stacked layers. The thickness-dependent anisotropic THG response is further analyzed to retrieve the third-order nonlinear susceptibility for franckeite crystal. The results discussed herein not only provide new insights in engineering the nonlinear light–matter interactions in natural vdW heterostructures, but also develop a testbed for designing future miniaturized quantum photonics devices and circuits based on such heterostructures. 

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