Intrinsic exciton states mixing and non-linear optical properties in transition metal dichalcogenide monolayers

Abstract

Optical properties of transition metal dichalcogenides monolayers are controlled by the Wannier-Mott excitons forming a series of $1s$, $2s$, $2p$,... hydrogen-like states. We develop the theory of the excited excitonic states energy spectrum fine structure. We predict that $p$- and $s$-shell excitons are mixed due to the specific $D_{3h}$ point symmetry of the transition metal dichalcogenide monolayers. Hence, both $s$- and $p$-shell excitons are active in both single- and two-photon processes providing an efficient mechanism of second harmonic generation. The corresponding contribution to the nonlinear susceptibility is calculated.