Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2

Zhipeng Li, Tianmeng Wang, Chenhao Jin, Zhengguang Lu, Zhen Lian, Yuze Meng, Mark Blei, Shiyuan Gao, Takashi Taniguchi, Kenji Watanabe, Tianhui Ren (), Sefaattin Tongay, Li Yang, Dmitry Smirnov, Ting Cao () and Su-Fei Shi ()
Additional contact information
Zhipeng Li: Rensselaer Polytechnic Institute
Tianmeng Wang: Rensselaer Polytechnic Institute
Chenhao Jin: Kavli Institute at Cornell for Nanoscale Science
Zhengguang Lu: National High Magnetic Field Lab
Zhen Lian: Rensselaer Polytechnic Institute
Yuze Meng: Rensselaer Polytechnic Institute
Mark Blei: Arizona State University
Shiyuan Gao: Washington University in St. Louis
Takashi Taniguchi: National Institute for Materials Science
Kenji Watanabe: National Institute for Materials Science
Tianhui Ren: Shanghai Jiao Tong University
Sefaattin Tongay: Arizona State University
Li Yang: Washington University in St. Louis
Dmitry Smirnov: National High Magnetic Field Lab
Ting Cao: Stanford University
Su-Fei Shi: Rensselaer Polytechnic Institute

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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 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.

Date: 2019
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DOI: 10.1038/s41467-019-10477-6

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