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Ultrafast Dynamics of Rydberg Excitons and Their Optically Induced Charged Complexes in Encapsulated WSe2 Monolayers.

Armando Genco1, Chiara Trovatello1,2, Vanik A Shahnazaryan3,4

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Strong excitonic effects are observed in transition metal dichalcogenides (TMDs). Ultrafast microscopy reveals excited-state (2s) excitons and 2s trions in WSe2, detailing their unique dynamics and decay pathways.

Keywords:
Rydberg excitonssemiconducting monolayerstransition metal dichalcogenidestrionsultrafast spectroscopy

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Quantum Optics

Background:

  • Atomically thin transition metal dichalcogenides (TMDs) exhibit strong excitonic effects due to quantum confinement and reduced dielectric screening.
  • Encapsulation with hexagonal boron nitride (hBN) reveals excitonic Rydberg series below the bandgap in TMD monolayers.
  • The dynamics of higher-order exciton states and their multiparticle complexes in these materials are not well understood.

Purpose of the Study:

  • To investigate the dynamics of excited-state (2s) excitons in hBN-encapsulated monolayer WSe2 using ultrafast pump-probe optical microscopy.
  • To explore the formation and decay mechanisms of 2s excitons and light-induced 2s trions.
  • To understand the interactions between excited excitons and free carriers in TMDs.

Main Methods:

  • Ultrafast pump-probe optical microscopy.
  • Time-resolved spectroscopy.
  • Optical characterization of WSe2 monolayers encapsulated in hBN.

Main Results:

  • Excited-state (2s) excitons form via ultrafast relaxation from high-energy states in WSe2 monolayers.
  • 2s excitons exhibit longer decay dynamics than ground-state excitons due to their larger spatial extent.
  • Light-induced formation of 2s trions with significant oscillator strength and faster decay than 2s excitons was observed, attributed to an intra-excitonic Auger effect.

Conclusions:

  • The study elucidates the dynamics of excited-state excitons in TMDs.
  • It highlights the role of an intra-excitonic Auger effect in the decay of 2s trions.
  • The findings provide insights into exciton-carrier interactions in these advanced materials.