Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots

Nikolay S. Makarov, Shaojun Guo, Oleksandr Isaienko, Wenyong Liu, István Robel, Victor I Klimov

Research output: Contribution to journalArticle

180 Citations (Scopus)

Abstract

Organic-inorganic lead-halide perovskites have been the subject of recent intense interest due to their unusually strong photovoltaic performance. A new addition to the perovskite family is all-inorganic Cs-Pb-halide perovskite nanocrystals, or quantum dots, fabricated via a moderate-temperature colloidal synthesis. While being only recently introduced to the research community, these nanomaterials have already shown promise for a range of applications from color-converting phosphors and light-emitting diodes to lasers, and even room-temperature single-photon sources. Knowledge of the optical properties of perovskite quantum dots still remains vastly incomplete. Here we apply various time-resolved spectroscopic techniques to conduct a comprehensive study of spectral and dynamical characteristics of single- and multiexciton states in CsPbX3 nanocrystals with X being either Br, I, or their mixture. Specifically, we measure exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton-exciton coupling. The overall conclusion of this work is that spectroscopic properties of Cs-Pb-halide quantum dots are largely similar to those of quantum dots of more traditional semiconductors such as CdSe and PbSe. At the same time, we observe some distinctions including, for example, an appreciable effect of the halide identity on radiative lifetimes, considerably shorter biexciton Auger lifetimes, and apparent deviation of their size dependence from the "universal volume scaling" previously observed for many traditional nanocrystal systems. The high efficiency of Auger decay in perovskite quantum dots is detrimental to their prospective applications in light-emitting devices and lasers. This points toward the need for the development of approaches for effective suppression of Auger recombination in these nanomaterials, using perhaps insights gained from previous studies of II-VI nanocrystals.

Original languageEnglish
Pages (from-to)2349-2362
Number of pages14
JournalNano Letters
Volume16
Issue number4
DOIs
Publication statusPublished - Apr 13 2016

Fingerprint

Cesium
cesium
Excitons
Perovskite
Semiconductor quantum dots
halides
Lead
Nanocrystals
quantum dots
excitons
nanocrystals
radiative lifetime
Nanostructured materials
Lasers
perovskites
electron states
Phosphors
absorption cross sections
phosphors
lasers

Keywords

  • absorption cross-section
  • Auger recombination
  • band-edge-state degeneracy
  • Cs-Pb-halide perovskites
  • exciton-exciton interaction
  • intraband cooling
  • nanocrystal
  • quantum dot
  • radiative recombination

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Mechanical Engineering

Cite this

Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots. / Makarov, Nikolay S.; Guo, Shaojun; Isaienko, Oleksandr; Liu, Wenyong; Robel, István; Klimov, Victor I.

In: Nano Letters, Vol. 16, No. 4, 13.04.2016, p. 2349-2362.

Research output: Contribution to journalArticle

Makarov, Nikolay S. ; Guo, Shaojun ; Isaienko, Oleksandr ; Liu, Wenyong ; Robel, István ; Klimov, Victor I. / Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots. In: Nano Letters. 2016 ; Vol. 16, No. 4. pp. 2349-2362.
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