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

Abstract

The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe${}_2$ crystals exhibit electric-field-driven coupling with the ground ($1s$) and excited states ($2s$) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to $0.73\pm 0.01$ enm), high energy tunability (up to $\sim$ 200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from -4 to +14). Further, we observe the bi- and tri-layer excited state ($2s$) interlayer excitons 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 explore exciton-exciton interactions with strong light-matter interactions.

References in corpus (49)

• Coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides
• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures
• The physics of dipolar bosonic quantum gases
• Tightly bound excitons in monolayer WSe2
• k.p theory for two-dimensional transition metal dichalcogenide semiconductors
• Magnetic Control of Valley Pseudospin in Monolayer WSe2
• Evolution of Interlayer Coupling in Twisted MoS2 Bilayers
• Evidence of high-temperature exciton condensation in 2D atomic double layers
• High-temperature superfluidity with indirect excitons in van der Waals heterostructures
• Observation of mesoscopic crystalline structures in a two-dimensional Rydberg gas
• Electrical control of interlayer exciton dynamics in atomically thin heterostructures
• Moiré superlattice in a MoSe${}_2$/hBN/MoSe${}_2$ heterostructure: from coherent coupling of inter- and intra-layer excitons to correlated Mott-like states of electrons
• Magnetoelectric effects and valley controlled spin quantum gates in transition metal dichalcogenide bilayers
• Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
• Spontaneous Coherence in a Cold Exciton Gas
• Control of interlayer excitons in two-dimensional van der Waals heterostructures
• Exciton diffusion and halo effects in monolayer semiconductors
• Magneto-Optics of Exciton Rydberg States in a Monolayer Semiconductor
• Quantum phase transition in a two-dimensional system of dipoles
• Exciton band structure in layered MoSe2: from a monolayer to the bulk limit
• Quantum correlations of confined exciton-polaritons
• Dipolar interactions between field-tuneable, localized emitters in van der Waals heterostructures
• Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe${}_2$/MoSe${}_2$ bilayers
• Electrical tuning of layer-polarized exciton gases in WSe2 bilayers
• Interlayer excitons in bilayer MoS2 with strong oscillator strength up to room temperature
• Giant Stark splitting of an exciton in bilayer MoS${}_2$
• Controlling interlayer excitons in MoS2 layers grown by chemical vapor deposition
• Discrete Interactions between a few Interlayer Excitons Trapped at a MoSe${}_2$-WSe${}_2$ Heterointerface
• Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
• Giant optical nonlinearities from Rydberg-excitons in semiconductor microcavities
• Highly nonlinear dipolar exciton-polaritons in bilayer MoS${}_2$
• Ab-initio studies of exciton $g$ factors: Monolayer transition metal dichalcogenides in magnetic fields
• Observation of Inter-layer Excitons in MoSe2 Single Crystals
• Dipolar and magnetic properties of strongly absorbing hybrid interlayer excitons in pristine bilayer MoS${}_2$
• Magnetooptics of layered two-dimensional semiconductors and heterostructures: progress and prospects
• Exciton landscape in van der Waals heterostructures
• Quantum phase transitions of tri-layer excitons in atomically thin heterostructures
• Electrical tuning of moiré excitons in MoSe${}_2$ bilayers
• Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe${}_2$, MoSe${}_2$ and MoTe${}_2$
• Every-other-layer Dipolar Excitons in a Spin-Valley locked Superlattice
• Key role of the moire potential for the quasi-condensation of interlayer excitons in van der Waals heterostructures
• Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity
• Quantum phase transition of a two-dimensional quadrupolar system
• Crystal Phases of Charged Interlayer Excitons in van der Waals Heterostructures
• Capacitively-coupled and inductively-coupled excitons in bilayer MoS${}_2$
• Analogy and dissimilarity of excitons in monolayer and bilayer of MoSe${}_2$
• Anomalous magneto-optical response and chiral interface of dipolar excitons at twisted valleys
• Interlayer excitons in semiconductor bilayers under a strong electric field

Cited by in corpus (7)

• Signatures of electric field and layer separation effects on the spin-valley physics of MoSe${}_2$/WSe${}_2$ heterobilayers: from energy bands to dipolar excitons
• Exciton Superposition across Moiré States in a Semiconducting Moiré Superlattice
• Quadrupolar Excitons in MoSe${}_2$ Bilayers
• Quadrupolar and Dipolar Excitons in Bilayer 2$H$-MoSe${}_2$
• Two dimensional semiconductors: optical and electronic properties
• Rydberg series of intralayer K-excitons in WSe${}_2$ multilayers
• Brightening interlayer excitons by electric-field-driven hole transfer in bilayer WSe2