4.8 Article

Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon

Journal

ACS NANO
Volume 13, Issue 12, Pages 14107-14113

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b06682

Keywords

intervalley exciton; chiral phonon; magneto-PL; time-resolved PL; tungsten diselenide

Funding

  1. AFSOR [FA9550-18-1-0312]
  2. Shanghai Sailing Program [19YF1425200]
  3. National Natural Science Foundation for Young Scientists Fund of China [51902196]
  4. National Natural Science Foundation of China [11890703, 11574154]
  5. NSF [DMR-1552220, DMR 1838443, NSF/DMR-1644779]
  6. Kavli Postdoctoral Fellowship
  7. Elemental Strategy Initiative by the MEXT, Japan
  8. CREST, JST [JPMJCR15F3]
  9. US Department of Energy [DE-FG02-07ER46451]
  10. State of Florida
  11. ACS PRF [59957-DNI10]
  12. New York State Empire State Development's Division of Science, Technology, and Innovation (NYSTAR) through Focus Center-NY-RPI Contract [C150117]
  13. KIP grant from RPI
  14. VSP grant from NHMFL

Ask authors/readers for more resources

Inversion symmetry breaking and 3-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition-metal dichalco-genides, which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, the 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 spectra. Interest-ingly, 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 of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be similar to 23 meV, based on the experimentally extracted exchange interaction (similar to 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.

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