Inversion symmetry breaking and three-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition metal dichalcogenides (TMDCs), which can be exploited for ...valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, dark exciton could be long-lived but does not necessarily possess the valley degree of freedom. In this work, we report the identification of the momentum-dark, intervalley exciton in monolayer WSe2 through low-temperature magneto-photoluminescence (PL) spectra. Interestingly, the intervalley exciton is brightened through the emission of a chiral phonon at the corners of the Brillouin zone (K point), and the pseudoangular momentum (PAM) of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be ~ 23 meV, based on the experimentally extracted exchange interaction (~ 7 meV), in excellent agreement with the theoretical expectation of 24.6 meV. The long-lived intervalley exciton with valley degree of freedom adds an exciting quasiparticle for valleytronics, and the coupling between the chiral phonon and intervalley exciton furnishes a venue for valley spin manipulation.
Tungsten-based monolayer transition metal dichalcogenides host a long-lived dark exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the ...dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E" phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin.
