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

Journal Article · · Nature Communications
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [2];  [5];  [6];  [7];  [8]; ORCiD logo [8];  [9];  [6];  [7]; ORCiD logo [10];  [11]; ORCiD logo
  1. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Chemical and Biological Engineering; Shanghai Jiao Tong Univ. (China). School of Chemistry and Chemical Engineering
  2. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Chemical and Biological Engineering
  3. Cornell Univ., Ithaca, NY (United States). Kavli Inst. at Cornell for Nanoscale Science
  4. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab); Florida State Univ., Tallahassee, FL (United States). Dept. of Physics
  5. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Chemical and Biological Engineering; Nanjing Univ. (China). College of Physics
  6. Arizona State Univ., Tempe, AZ (United States). School for Engineering of Matter, Transport and Energy
  7. Washington Univ., St. Louis, MO (United States). Dept. of Physics
  8. National Inst. for Materials Science (NIMS), Tsukuba (Japan)
  9. Shanghai Jiao Tong Univ. (China). School of Chemistry and Chemical Engineering
  10. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  11. Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering

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.

Research Organization:
Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
Grant/Contract Number:
FG02-00ER41132
OSTI ID:
1624159
Journal Information:
Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (6)

Modulation of spin–valley splitting in a two-dimensional MnPSe 3 /CrBr 3 van der Waals heterostructure journal January 2020
Valley phonons and exciton complexes in a monolayer semiconductor journal January 2020
Advances in quantum light emission from 2D materials journal August 2019
Theory and Ab Initio Calculation of Optically Excited States—Recent Advances in 2D Materials journal December 2019
Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2 journal October 2019
Valley Phonons and Exciton Complexes in a Monolayer Semiconductor text January 2020