Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe<sub>2</sub>.

Li, Zhipeng; Wang, Tianmeng; Jin, Chenhao; Lu, Zhengguang; Lian, Zhen; Meng, Yuze; Blei, Mark; Gao, Shiyuan et al. · Nat Commun · 2019

basic_science · Level V

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Abstract

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 WSe<sub>2</sub>. 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.