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Super-Resolution Luminescence Microspectroscopy Reveals the Mechanism of Photoinduced Degradation in CH3NH3PbI3 Perovskite Nanocrystals

Merdasa, Aboma LU ; Bag, Monojit LU ; Tian, Yuxi LU ; Källman, Elin; Dobrovolsky, Alexander LU and Scheblykin, Ivan LU (2016) In Journal of Physical Chemistry C 120(19). p.10711-10719
Abstract
Photoinduced degradation of individual methylammonium lead triiodide (MAPbI3) perovskite nanocrystals was studied using super-resolution luminescence microspectroscopy under intense light excitation. The photoluminescence (PL) intensity decrease and blue-shift of the PL spectrum up to 60 nm together with spatial shifts in the emission localization position up to a few hundred nanometers were visualized in real time. PL blinking was found to temporarily suspend the degradation process, indicating that the degradation needs a high concentration of mobile photogenerated charges to occur. We propose that the mechanistic process of degradation occurs as the three-dimensional MAPbI3 crystal structure smoothly collapses to the two-dimensional... (More)
Photoinduced degradation of individual methylammonium lead triiodide (MAPbI3) perovskite nanocrystals was studied using super-resolution luminescence microspectroscopy under intense light excitation. The photoluminescence (PL) intensity decrease and blue-shift of the PL spectrum up to 60 nm together with spatial shifts in the emission localization position up to a few hundred nanometers were visualized in real time. PL blinking was found to temporarily suspend the degradation process, indicating that the degradation needs a high concentration of mobile photogenerated charges to occur. We propose that the mechanistic process of degradation occurs as the three-dimensional MAPbI3 crystal structure smoothly collapses to the two-dimensional layered PbI2 structure. The degradation starts locally and then spreads over the whole crystal. The structural collapse is primarily due to migration of methylammonium ions (MA+), which distorts the lattice structure causing alterations to the Pb–I–Pb bond angle and in turn changes the effective band gap. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
perovskite, photo-induced degradation, photophysics, blinking, super-resolution microscopy
in
Journal of Physical Chemistry C
volume
120
issue
19
pages
9 pages
publisher
The American Chemical Society
external identifiers
  • scopus:84971225635
  • wos:000376417500066
ISSN
1932-7447
DOI
10.1021/acs.jpcc.6b03512
language
English
LU publication?
yes
id
5938aa24-f515-4a85-89e1-a3e8bd633da0
date added to LUP
2017-01-10 12:16:11
date last changed
2017-10-01 05:28:35
@article{5938aa24-f515-4a85-89e1-a3e8bd633da0,
  abstract     = {Photoinduced degradation of individual methylammonium lead triiodide (MAPbI3) perovskite nanocrystals was studied using super-resolution luminescence microspectroscopy under intense light excitation. The photoluminescence (PL) intensity decrease and blue-shift of the PL spectrum up to 60 nm together with spatial shifts in the emission localization position up to a few hundred nanometers were visualized in real time. PL blinking was found to temporarily suspend the degradation process, indicating that the degradation needs a high concentration of mobile photogenerated charges to occur. We propose that the mechanistic process of degradation occurs as the three-dimensional MAPbI3 crystal structure smoothly collapses to the two-dimensional layered PbI2 structure. The degradation starts locally and then spreads over the whole crystal. The structural collapse is primarily due to migration of methylammonium ions (MA+), which distorts the lattice structure causing alterations to the Pb–I–Pb bond angle and in turn changes the effective band gap.},
  author       = {Merdasa, Aboma and Bag, Monojit and Tian, Yuxi and Källman, Elin and Dobrovolsky, Alexander and Scheblykin, Ivan},
  issn         = {1932-7447},
  keyword      = {perovskite,photo-induced degradation,photophysics,blinking,super-resolution microscopy},
  language     = {eng},
  month        = {04},
  number       = {19},
  pages        = {10711--10719},
  publisher    = {The American Chemical Society},
  series       = {Journal of Physical Chemistry C},
  title        = {Super-Resolution Luminescence Microspectroscopy Reveals the Mechanism of Photoinduced Degradation in CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> Perovskite Nanocrystals},
  url          = {http://dx.doi.org/10.1021/acs.jpcc.6b03512},
  volume       = {120},
  year         = {2016},
}