Giant Stark splitting of an exciton in bilayer MoS$_2$

Abstract

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to the quantum confined Stark effect, here the electron is localised to one of the layers yet the hole is delocalised across the bilayer. We optically probe the interaction between intra- and interlayer excitons as they are energetically tuned into resonance. This allows studying their mixing supported by beyond standard density functional theory calculations including excitonic effects. In MoS2 trilayers our experiments uncover two types of interlayer excitons with and without in-built electric dipoles, respectively. Highly tunable excitonic transitions with large oscillator strength and in-built dipoles, that lead to considerable exciton-exciton interactions, hold great promise for non-linear optics with polaritons.