Giant Spin-Selective Bandgap Renormalization in CsPbBr3 Colloidal Nanocrystals

Megha Shrivastava, Abhijit Hazarika, J. Aneesh, Dipendranath Mandal, Matthew Beard, K. Adarsh

Research output: Contribution to journalArticlepeer-review

4 Scopus Citations

Abstract

The spin-dependence of the strongly correlated phenomena and many-body interactions play an important role in quantum information science. In particular, it is quite interesting but unclear how the spin degree of freedom ramifies the bandgap renormalization, one of the fundamental many-body phenomena. We report the first room-temperature observation of giant spin-selective bandgap renormalization (SS-BGR) in CsPbBr3 colloidal nanocrystals using time-resolved circularly polarized femtosecond pump-probe spectroscopy. The SS-BGR results from many-body interactions among carriers with the same spin that renormalize their joint density of states by 57± 1 meV, visualized here as photoinduced absorption (PIA) below band-edge transition energy when the pump and probe are co-polarized. The hallmark result of spectrally resolved SS-BGR is in stark contrast to the usually submerged signal in II-VI and III-V semiconductors and is 3 orders of magnitude larger than that observed in Ge/SiGe quantum wells, highlighting the unique and beneficial band structure of the metal-halide semiconductors. We propose that the PIA, due to SS-BGR, can be used to describe the spin-polarization and spin-relaxation dynamics. The experimental and theoretical findings open up new possibilities for optical manipulation of spin degrees of freedom and their many-body interactions in metal-halide perovskite nanocrystals for potential room-temperature applications.

Original languageAmerican English
Article numberArticle No. L041404
Number of pages7
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume106
Issue number4
DOIs
StatePublished - 15 Jul 2022

Bibliographical note

Publisher Copyright:
© 2022 American Physical Society.

NREL Publication Number

  • NREL/JA-5900-82268

Keywords

  • bandgap renormalization
  • CsPbBr3
  • spin polarization

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