skip to main content

Title: Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice
Abstract Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states.  more » « less
Award ID(s):
2004701 1825594 1904716 1933214 1945420
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Nature Communications
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. 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 WSe2-WS2-WSe2trilayer 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 WSe2valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2layers 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 WSe2under 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.

    more » « less
  2. We develop a systematic theory for excitons subject to Fermi-Hubbard physics in moiré twisted transition metal dichalcogenides (TMDs). Specifically, we consider excitons from two moiré bands with a Mott-insulating valence band sustaining 120 spin order. These “Mott-moiré excitons,” which are achievable in twisted TMD heterobilayers, are bound states of a magnetic polaron in the valence band and a free electron in the conduction band. We find significantly narrower exciton bandwidths in the presence of Hubbard physics, serving as a potential experimental signature of strong correlations. We also demonstrate the high tunability of Mott-moiré excitons through the dependence of their binding energies, diameters, and bandwidths on the moiré period. In addition, we study bound states between charges outside of the strongly correlated moiré band and find that these as well exhibit signatures of spin correlation. Our work provides guidelines for future exploration of strongly correlated excitons in triangular Hubbard systems such as twisted TMD heterobilayers. 
    more » « less
  3. 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.

    more » « less
  4. Excitons in monolayer semiconductors have a large optical transition dipole for strong coupling with light. Interlayer excitons in heterobilayers feature a large electric dipole that enables strong coupling with an electric field and exciton-exciton interaction at the cost of a small optical dipole. We demonstrate the ability to create a new class of excitons in hetero- and homobilayers that combines advantages of monolayer and interlayer excitons, i.e., featuring both large optical and electric dipoles. These excitons consist of an electron confined in an individual layer, and a hole extended in both layers, where the carrier-species–dependent layer hybridization can be controlled through rotational, translational, band offset, and valley-spin degrees of freedom. We observe different species of layer-hybridized valley excitons, which can be used for realizing strongly interacting polaritonic gases and optical quantum controls of bidirectional interlayer carrier transfer. 
    more » « less
  5. Abstract

    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.

    more » « less