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Heterogeneities and Emissive Defects in MAPbI3 Perovskite Revealed by Spectrally Resolved Luminescence Blinking

Gerhard, Marina LU ; Louis, Boris LU ; Frantsuzov, Pavel A. LU ; Li, Jun LU ; Kiligaridis, Alexander LU ; Hofkens, Johan and Scheblykin, Ivan G. LU (2021) In Advanced Optical Materials
Abstract

The fate of excited charge carriers in metal halide perovskite semiconductors is influenced by energetic disorder and defects. Here, photoluminescence (PL) blinking is used to probe metastable nonradiative (NR) centers and the nanoscale energy landscape. Temporal activation of an NR center creates a local region with increased NR recombination. Activation and deactivation of this local PL quenching does not only lead to PL blinking, but also to fluctuations of the PL spectra, if the crystal is inhomogeneous in the sense that the PL emission spectrum is slightly different from one location to another. It resembles the spectral hole-burning technique; however, here the eliminated excited states are chosen by their spatial localization... (More)

The fate of excited charge carriers in metal halide perovskite semiconductors is influenced by energetic disorder and defects. Here, photoluminescence (PL) blinking is used to probe metastable nonradiative (NR) centers and the nanoscale energy landscape. Temporal activation of an NR center creates a local region with increased NR recombination. Activation and deactivation of this local PL quenching does not only lead to PL blinking, but also to fluctuations of the PL spectra, if the crystal is inhomogeneous in the sense that the PL emission spectrum is slightly different from one location to another. It resembles the spectral hole-burning technique; however, here the eliminated excited states are chosen by their spatial localization close to the quencher. In MAPbI3, PL spectral fluctuations at low temperature reveal energetic inhomogeneities on the order of 5 to 10 meV. Quenching of the main PL band is often found to correlate with an increase of the low-energetic tail of the PL spectra, which is attributed to partially radiative recombination of charges captured by the NR center. The transition energy of the NR center is found to be only ≈80 meV smaller than the bandgap, implying that the underlying defect cannot be a single mid-bandgap state.

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organization
publishing date
type
Contribution to journal
publication status
epub
subject
keywords
energetic disorder, hybrid perovskites, luminescence blinking, spectral hole burning
in
Advanced Optical Materials
publisher
John Wiley and Sons Inc.
external identifiers
  • scopus:85099248767
ISSN
2195-1071
DOI
10.1002/adom.202001380
language
English
LU publication?
yes
id
024fead9-adb5-4f9f-a305-fc3ce2e7706b
date added to LUP
2021-01-25 13:26:26
date last changed
2021-02-17 03:59:29
@article{024fead9-adb5-4f9f-a305-fc3ce2e7706b,
  abstract     = {<p>The fate of excited charge carriers in metal halide perovskite semiconductors is influenced by energetic disorder and defects. Here, photoluminescence (PL) blinking is used to probe metastable nonradiative (NR) centers and the nanoscale energy landscape. Temporal activation of an NR center creates a local region with increased NR recombination. Activation and deactivation of this local PL quenching does not only lead to PL blinking, but also to fluctuations of the PL spectra, if the crystal is inhomogeneous in the sense that the PL emission spectrum is slightly different from one location to another. It resembles the spectral hole-burning technique; however, here the eliminated excited states are chosen by their spatial localization close to the quencher. In MAPbI<sub>3</sub>, PL spectral fluctuations at low temperature reveal energetic inhomogeneities on the order of 5 to 10 meV. Quenching of the main PL band is often found to correlate with an increase of the low-energetic tail of the PL spectra, which is attributed to partially radiative recombination of charges captured by the NR center. The transition energy of the NR center is found to be only ≈80 meV smaller than the bandgap, implying that the underlying defect cannot be a single mid-bandgap state.</p>},
  author       = {Gerhard, Marina and Louis, Boris and Frantsuzov, Pavel A. and Li, Jun and Kiligaridis, Alexander and Hofkens, Johan and Scheblykin, Ivan G.},
  issn         = {2195-1071},
  language     = {eng},
  month        = {01},
  publisher    = {John Wiley and Sons Inc.},
  series       = {Advanced Optical Materials},
  title        = {Heterogeneities and Emissive Defects in MAPbI<sub>3</sub> Perovskite Revealed by Spectrally Resolved Luminescence Blinking},
  url          = {http://dx.doi.org/10.1002/adom.202001380},
  doi          = {10.1002/adom.202001380},
  year         = {2021},
}