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

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/WS₂ moiré superlattice by changing WSe₂ from 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/WS₂ interface. In addition, the energy resonances of moiré excitons are strongly modified, with their separation significantly increased in multilayer WSe₂/monolayer WS₂ moiré superlattice. The additional WSe₂ layers also modulate the strong electronic correlation strength, evidenced by the reduced Mott transition temperature with added WSe₂ layer(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.