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Direct Experimental Evidence for Photoinduced Strong-Coupling Polarons in Organolead Halide Perovskite Nanoparticles

Zheng, Kaibo LU ; Abdellah, Mohamed LU ; Zhu, Qiushi LU ; Kong, Qingyu; Jennings, Guy; Kurtz, Charles A.; Messing, Maria E. LU ; Niu, Yuran LU ; Gosztola, David J. and Al-Marri, Mohammed J., et al. (2016) In The Journal of Physical Chemistry Letters 7(22). p.4535-4539
Abstract

Echoing the roaring success of their bulk counterparts, nano-objects built from organolead halide perovskites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the photoinduced charge dynamics is essential for optimizing the optoelectronic functionalities. However, mapping the carrier-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorption measurements, this work reveals the photoinduced formation of strong-coupling polarons in CH3NH3PbBr3 nanoparticles. Such polarons... (More)

Echoing the roaring success of their bulk counterparts, nano-objects built from organolead halide perovskites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the photoinduced charge dynamics is essential for optimizing the optoelectronic functionalities. However, mapping the carrier-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorption measurements, this work reveals the photoinduced formation of strong-coupling polarons in CH3NH3PbBr3 nanoparticles. Such polarons originate from the self-trapping of electrons in the Coulombic field caused by the displaced inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L3 X-ray absorption edge is well-captured by a distortion with average bond elongation in the [PbBr6]2- motif. General implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.

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The Journal of Physical Chemistry Letters
volume
7
issue
22
pages
5 pages
publisher
The American Chemical Society
external identifiers
  • scopus:84996490775
  • wos:000388433200018
ISSN
1948-7185
DOI
10.1021/acs.jpclett.6b02046
language
English
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yes
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3df8fbea-06a3-412e-bb78-d0bbf4a79a6f
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2016-12-12 09:57:44
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2017-09-18 11:31:01
@article{3df8fbea-06a3-412e-bb78-d0bbf4a79a6f,
  abstract     = {<p>Echoing the roaring success of their bulk counterparts, nano-objects built from organolead halide perovskites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the photoinduced charge dynamics is essential for optimizing the optoelectronic functionalities. However, mapping the carrier-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorption measurements, this work reveals the photoinduced formation of strong-coupling polarons in CH<sub>3</sub>NH<sub>3</sub>PbBr<sub>3</sub> nanoparticles. Such polarons originate from the self-trapping of electrons in the Coulombic field caused by the displaced inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L<sub>3</sub> X-ray absorption edge is well-captured by a distortion with average bond elongation in the [PbBr<sub>6</sub>]<sup>2-</sup> motif. General implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.</p>},
  author       = {Zheng, Kaibo and Abdellah, Mohamed and Zhu, Qiushi and Kong, Qingyu and Jennings, Guy and Kurtz, Charles A. and Messing, Maria E. and Niu, Yuran and Gosztola, David J. and Al-Marri, Mohammed J. and Zhang, Xiaoyi and Pullerits, Tönu and Canton, Sophie E.},
  issn         = {1948-7185},
  language     = {eng},
  month        = {11},
  number       = {22},
  pages        = {4535--4539},
  publisher    = {The American Chemical Society},
  series       = {The Journal of Physical Chemistry Letters},
  title        = {Direct Experimental Evidence for Photoinduced Strong-Coupling Polarons in Organolead Halide Perovskite Nanoparticles},
  url          = {http://dx.doi.org/10.1021/acs.jpclett.6b02046},
  volume       = {7},
  year         = {2016},
}