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1. Tuning moiré excitons and correlated electronic states through layer degree of freedom

   https://doi.org/10.1038/s41467-022-32493-9  

   Chen, Dongxue ; Lian, Zhen ; Huang, Xiong ; Su, Ying ; Rashetnia, Mina ; Yan, Li ; Blei, Mark ; Taniguchi, Takashi ; Watanabe, Kenji ; Tongay, Sefaattin ; et al ( August 2022 , Nature Communications)

   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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2. Proximity-enhanced valley Zeeman splitting at the WS 2 /graphene interface

   https://doi.org/10.1088/2053-1583/acd5df  

   Faria Junior, Paulo E. ; Naimer, Thomas ; McCreary, Kathleen M. ; Jonker, Berend T. ; Finley, Jonathan J. ; Crooker, Scott A. ; Fabian, Jaroslav ; Stier, Andreas V. ( May 2023 , 2D Materials)

   The valley Zeeman physics of excitons in monolayer transition metal dichalcogenides provides valuable insight into the spin and orbital degrees of freedom inherent to these materials. Being atomically-thin materials, these degrees of freedom can be influenced by the presence of adjacent layers, due to proximity interactions that arise from wave function overlap across the 2D interface. Here, we report 60 T magnetoreflection spectroscopy of the A- and B- excitons in monolayer WS₂, systematically encapsulated in monolayer graphene. While the observed variations of the valley Zeeman effect for the A- exciton are qualitatively in accord with expectations from the bandgap reduction and modification of the exciton binding energy due to the graphene-induced dielectric screening, the valley Zeeman effect for the B- exciton behaves markedly different. We investigate prototypical WS₂/graphene stacks employing first-principles calculations and find that the lower conduction band of WS₂at the$K/K^{\mathrm{\prime }}$valleys (the${\mathrm{C}\mathrm{B}}^{-}$band) is strongly influenced by the graphene layer on the orbital level. Specifically, our detailed microscopic analysis reveals that the conduction band at theQpoint of WS₂mediates the coupling between${\mathrm{C}\mathrm{B}}^{-}$and graphene due to resonant energy conditions and strong coupling to the Dirac cone. This leads to variations in the valley Zeeman physics of the B- exciton, consistent with the experimental observations. Our results therefore expand the consequences of proximity effects in multilayer semiconductor stacks, showing that wave function hybridization can be a multi-step energetically resonant process, with different bands mediating the interlayer interactions. Such effects can be further exploited to resonantly engineer the spin-valley degrees of freedom in van der Waals and moiré heterostructures.

    

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3. Ultrathin WS 2 ‐on‐Glass Photonic Crystal for Self‐Resonant Exciton‐Polaritonics

   https://doi.org/10.1002/adom.201901988  

   Zhang, Xingwang ; Zhang, Xiaojie ; Huang, Wenzhuo ; Wu, Kedi ; Zhao, Mengqiang ; Charlie Johnson, A. T. ; Tongay, Sefaattin ; Cubukcu, Ertugrul ( February 2020 , Advanced Optical Materials)

   Room temperature stable excitons in layered two‐dimensional (2D) transition metal dichalcogenides (TMDs) offer a unique route for engineering light and matter interactions. Due to the strong optical dispersion near the excitonic transitions, a high refractive index arises in these ultrathin semiconductors.^[1,2]Utilizing this behavior, strongly confined Fano type optical resonances in an ultrathin (i.e., ≈12 nm) tungsten disulfide (WS₂) photonic crystal (PhC) directly fabricated on a TMD‐on‐glass platform are reported. In this approach, Fano‐type WS₂photonic resonances strongly couple to the WS₂excitonic dispersion engender self‐resonant exciton‐polaritons with an out‐of‐plane optical confinement exceeding that provided by surface plasmon polaritons in the visible. The large spatial light‐matter overlap endowed by this unique monolithic self‐coupling scheme is utilized for steering of enhanced 2D WSe₂excitonic photoluminescence in a truly TMD integrated system. It is envisioned that the strong light matter interaction on the TMD‐on‐glass platform will unfold the prospects of ultrathin exciton‐polaritonic resonators.

    

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4. Room‐Temperature Observation of Near‐Intrinsic Exciton Linewidth in Monolayer WS 2

   https://doi.org/10.1002/adma.202108721  

   Fang, Jie ; Yao, Kan ; Zhang, Tianyi ; Wang, Mingsong ; Jiang, Taizhi ; Huang, Suichu ; Korgel, Brian A. ; Terrones, Mauricio ; Alù, Andrea ; Zheng, Yuebing ( March 2022 , Advanced Materials)

   The homogeneous exciton linewidth, which captures the coherent quantum dynamics of an excitonic state, is a vital parameter in exploring light–matter interactions in 2D transition metal dichalcogenides (TMDs). An efficient control of the exciton linewidth is of great significance, and in particular of its intrinsic linewidth, which determines the minimum timescale for the coherent manipulation of excitons. However, such a control is rarely achieved in TMDs at room temperature (RT). While the intrinsic A exciton linewidth is down to 7 meV in monolayer WS₂, the reported RT linewidth is typically a few tens of meV due to inevitable homogeneous and inhomogeneous broadening effects. Here, it is shown that a 7.18 meV near‐intrinsic linewidth can be observed at RT when monolayer WS₂is coupled with a moderate‐refractive‐index hydrogenated silicon nanosphere in water. By boosting the dynamic competition between exciton and trion decay channels in WS₂through the nanosphere‐supported Mie resonances, the coherent linewidth can be tuned from 35 down to 7.18 meV. Such modulation of exciton linewidth and its associated mechanism are robust even in presence of defects, easing the sample quality requirement and providing new opportunities for TMD‐based nanophotonics and optoelectronics.

    

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5. Moiré excitons in defective van der Waals heterostructures

   https://doi.org/10.1073/pnas.2105468118  

   Guo, Hongli ; Zhang, Xu ; Lu, Gang ( August 2021 , Proceedings of the National Academy of Sciences)

   Excitons can be trapped by moiré potentials in van der Waals (vdW) heterostructures, forming ordered arrays of quantum dots. Excitons can also be trapped by defect potentials as single photon emitters. While the moiré and defect potentials in vdW heterostructures have been studied separately, their interplay remains largely unexplored. Here, we perform first-principles calculations to elucidate the interplay of the two potentials in determining the optoelectronic properties of twisted MoS 2 /WS 2 heterobilayers. The binding energy, charge density, localization, and hybridization of the moiré excitons can be modulated by the competition and cooperation of the two potentials. Their interplay can also be tuned by vertical electric fields, which can either de-trap the excitons or strongly localize them. One can further tailor the interplay of the two potentials via defect engineering to create one-dimensional exciton lattices with tunable orientations. Our work establishes defect engineering as a promising strategy to realize on-demand optoelectronic responses. 

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