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The fundamental properties of an exciton are determined by the spin, valley,energy, and spatial wavefunctions of the Coulomb bound electron and hole. Invan der Waals materials, these attributes can be widely engineered throughlayer stacking configuration to create highly tunable interlayer excitons withstatic out-of-plane electric dipoles, at the expense of the strength of theoscillating in-plane dipole responsible for light-matter coupling. Here we showthat interlayer excitons in bi- and tri-layer 2H-MoSe$_2$ crystals exhibitelectric-field-driven coupling with the ground ($1s$) and excited states ($2s$)of the intralayer A excitons. We demonstrate that the hybrid states of thesedistinct exciton species provide strong oscillator strength, large permanentdipoles (up to $0.73 \pm 0.01$ enm), high energy tunability (up to $\sim$ 200meV), and full control of the spin and valley characteristics such that theexciton g-factor can be manipulated over a large range (from -4 to +14).Further, we observe the bi- and tri-layer excited state ($2s$) interlayerexcitons and their coupling with the intralayer excitons states ($1s$ and$2s$). Our results, in good agreement with a coupled oscillator model with spin(layer)-selectivity and beyond standard density functional theory calculations,promote multilayer 2H-MoSe$_2$ as a highly tunable platform to exploreexciton-exciton interactions with strong light-matter interactions.

Highly Tunable Ground and Excited State Excitonic Dipoles in Multilayer 2H-MoSe$_2$