Microscopic theory of cavity-confined monolayer semiconductors: Polariton-induced valley relaxation and the prospect of enhancing and controlling valley pseudospin by chiral strong coupling

Abstract

We apply a microscopic theory of exciton-polaritons in cavity-confined monolayer transition-metal dichalcogenides including both optical polarizations in the monolayer plane, allowing to describe how chiral cavity photons interact with the valley degrees of freedom of the active material. Upon polariton formation, the degenerate excitons inhabiting the two inequivalent valleys are shown to assume bonding and antibonding superpositions as a result of cavity-mediated intravalley interactions combined with intervalley Coulomb interactions. This is representative of a polariton-induced coherent mixing of the valley polarization. In combination with disorder, this mixing is prone to open a new valley relaxation channel which attains significance with increasing cavity coupling. Importantly, we show that optical cavities with an asymmetric reflectance of left- and right-handed circularly-polarized photons offer a considerably more robust platform to realize a conserved valley polarization, as the valley localization of excitons is reinstated by an asymmetric Rabi splitting which lifts their degeneracy. Moreover, we show this degeneracy lifting to allow for wavelength-selective access to the valley pseudospin by means of a polariton-induced chiral Stark effect, offering interesting opportunities for valleytronic applications.