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  • Li, Zhipeng; Wang, Tianmeng; Jin, Chenhao; Lu, Zhengguang; Lian, Zhen; Meng, Yuze; Blei, Mark; Gao, Shiyuan; Taniguchi, Takashi; Watanabe, Kenji; Ren, Tianhui; Tongay, Sefaattin; Yang, Li; Smirnov, Dmitry; Cao, Ting; Su-Fei, Shi

    arXiv.org, 05/2019
    Paper, Journal Article

    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.