4.7 Article

Positively Charged Biexcitons in Monolayer WSe2 in Type-I GaSe/ WSe2 van der Waals Heterostructures: Implications for the Biexciton Laser

Journal

ACS APPLIED NANO MATERIALS
Volume 5, Issue 8, Pages 10628-10635

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.2c01957

Keywords

transition-metal dichalcogenide; van der Waals heterostructure; charge transfer process; type-I band alignment; positively charged biexciton

Funding

  1. National Key Ramp
  2. D Program of China [2018YFA0703700, 2017YFF0206106]
  3. Shanghai Municipal Science and Technology Commission [20ZR1403200, 18511110700, 20DZ2203600]
  4. National Natural Science Foundation of China [61774040, 61774042]
  5. Strategic Priority Research Program of Chinese Academy of Sciences [XDB30000000]
  6. National Young 1000 Talent Plan of China
  7. State Key Laboratory of ASIC & System, Fudan University [2018MS001]
  8. Innovation Program of Shanghai Municipal Education Commission [2021-01-07-00-07-E00077]
  9. First-Class Construction project of Fudan University [XM03170477]

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In this study, a five-particle positively charged biexciton in monolayer WSe2 is observed by achieving a high exciton density in the GaSe/WSe2 heterostructure with a type-I band alignment. The nature of this biexciton is confirmed through various photoluminescence measurements, and the mechanism of its formation is explained. The influence of charge transfer on the excitonic properties in the type-I band heterostructure is different from that in most TMDCs with type-II band alignments.
Monolayer two-dimensional transition metal dichalcogenides (TMDCs) exhibit strong Coulomb interactions, which provide an ideal platform for the fundamental studies of many body correlated excitonic states. As a typical representative of many-body problems, the neutral exciton and charged exciton have been widely studied. However, some high-order excitonic states involving more particles, such as four-body biexciton and five-body charged biexciton, remain elusive because of the requirement of a high exciton density. Herein, we present an observation of a five particle positively charged biexciton in monolayer WSe2, which is rarely reported to the best of our knowledge, by achieving a high exciton density in the GaSe/WSe2 heterostructure with a type-I band alignment. The nature of the positively charged biexciton in monolayer WSe2 is confirmed by the studies of the excitation-power-dependent and gate-voltage-dependent photoluminescence measurements. The mechanism of formation of the positively charged biexciton is also elaborated in the view of the band alignment of the GaSe/WSe2 heterostructure. In the GaSe/WSe2 heterostructure with type-I band alignment, the excessive hole carriers transfer into WSe2 and facilitate the formation of the positively charged exciton and further facilitate the formation of the positively charged biexciton in WSe2. The influence of charge transfer on the excitonic properties in the type-I band heterostructure by funneling excitons into one layer is very different from that in most TMDCs van der Waals heterostructures with type-II band alignments in which the electrons and holes are confined in two separate layers. These investigations provide a better understanding of the high-order excitonic states in monolayer TMDCs and offer some basis for exploration of the related phenomena of the many body effect and the biexciton laser based on van der Waals heterostructures.

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