Distinctive signatures of the spin- and momentum-forbidden dark exciton states in the photo-luminescences of strained WSe${}_2$ monolayers under thermalization

Abstract

With the both spin and valley degrees of freedom, the low-lying excitonic spectra of photo-excited transition-metal dichalcogenide monolayers (TMDC-MLs) are featured by rich fine structures, comprising the intra-valley bright exciton states as well as various intra- and inter-valley dark ones. The latter states can be classified as those of the spin- and momentum-forbidden dark excitons according to the violated optical selection rules. Because of the optical invisibility, the two types of the dark states are in general hardly observed and even distinguished in conventional spectroscopies although their impacts on the optical and dynamical properties of TMDC-MLs have been well noticed. In this Letter, we present a theoretical and computational investigation of the exciton fine structures and the temperature-dependent photo-luminescence spectra of strained tungsten diselenide monolayers (WSe${}_2$-MLs) where the intra-valley spin-forbidden dark exciton lies in the lowest exciton states and other momentum-forbidden states are in the higher energies that are tunable by external stress. The numerical computations are carried out by solving the Bethe-Salpeter equation for an exciton in a WSe${}_2$-ML under the stress-control in the tight-binding scheme established from the first principle computation in the density functional theory. According to the numerical computation and supportive model analysis, we reveal the distinctive signatures of the spin- and momentum-forbidden exciton states of strained WSe${}_2$-MLs in the temperature-dependent photo-luminescences and present the guiding principle to infer the relative energetic locations of the two types of DX's.

arXiv comment44 pages, 7 figures

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