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High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
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Exciton-Resolved Phonon Coupling and Energy Dissipation Pathways in CsPbBr3.

Pradeepa H L1, Sagnik Chatterjee1, Sayantan Patra1

  • 1Department of Physics, Indian Institute of Science Education and Research(IISER), Pune 411008, India.

ACS Nano
|June 27, 2026
PubMed
Summary

This study reveals distinct phonon replicas for high-energy and Rashba excitons in CsPbBr3, clarifying exciton-phonon coupling. These interactions evolve with temperature, impacting optoelectronic applications.

Keywords:
CsPbBr3Rashba excitonsexciton−phonon couplinglead halide perovskitesphonon replicasphotoluminescence spectroscopy

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Area of Science:

  • Solid State Physics
  • Materials Science
  • Quantum Optics

Background:

  • Exciton-phonon interactions are crucial for semiconductor optical properties.
  • Disentangling these interactions in lead halide perovskites is complex.
  • Understanding these couplings is key for advanced optoelectronic devices.

Purpose of the Study:

  • To investigate exciton-specific phonon coupling in CsPbBr3 microcrystals.
  • To differentiate coupling mechanisms for high-energy and Rashba excitons.
  • To explore temperature-dependent evolution of these interactions.

Main Methods:

  • Low-temperature photoluminescence, Raman, and reflectance spectroscopy.
  • Analysis of phonon replica series for different exciton types.
  • k-means clustering applied to photoluminescence data.

Main Results:

  • Identified distinct phonon replica series for high-energy (approx. 9 meV spacing) and Rashba (approx. 6 meV spacing) excitons.
  • Confirmed prevalence of these specific replica features using k-means clustering.
  • Observed broadening and merging of replicas with increasing temperature, leading to dominant LO phonon coupling.

Conclusions:

  • Provided direct spectroscopic evidence for concurrent, exciton-specific phonon coupling in CsPbBr3.
  • Demonstrated temperature-dependent evolution of exciton-phonon interactions.
  • Opened pathways for engineering light-matter interactions in optoelectronics and quantum devices.