Quadrupolar and Dipolar Excitons in Bilayer 2$H$-MoSe${}_2$

Abstract

We report the experimental observation of quadrupolar exciton states in the reflectance contrast spectrum of 2$H$-stacked bilayer MoSe${}_2$. The application of a vertical electric field results in a quadratic energy redshift of these quadrupolar excitons, in contrast to the linear energy splitting observed in the coexisting dipolar excitons within the bilayer MoSe${}_2$. We perform helicity-resolved reflectance contrast measurements to investigate the spin and valley configurations of the quadrupolar exciton states as a function of applied vertical electric and magnetic fields. Comparing our results with a phenomenological coupled-oscillator model indicates that the electric- and magnetic-field dependence of the quadrupolar exciton states can be attributed to the intravalley and intervalley hybridization of spin-triplet interlayer excitons with opposite permanent dipole moments, mediated by interlayer hole tunneling. These results position naturally stacked MoSe${}_2$ bilayers as a promising platform to explore electric-field-tunable many-body exciton phenomena.

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