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Title: Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles

Abstract

Echoing the roaring success of their bulk coun-terparts, nano-objects built from organolead halide perov-skites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the pho-toinduced charge dynamics is essential for optimizing OLHP optoelectronic functionalities. However, mapping the carri-er-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorp-tion 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 net Coulombic field caused by the dis-placed inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L3 X-ray ab-sorption edge is well captured by a distortion with average bond elongation in the [PbBr6]2- motif. As a result, general implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.

Authors:
 [1];  [2];  [1];  [3];  [1];  [2];  [4];  [4];  [4];  [1];  [1];  [4];  [5];  [4];  [1];  [6]
  1. Lund Univ., Lund (Sweden)
  2. (Qatar)
  3. (Egypt)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Qatar Univ., Doha (Qatar)
  6. Univ. of Hamburg, Hamburg (Germany)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division; Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC)
OSTI Identifier:
1369031
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 22; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; CH3NH3PBI3; exciton binding-energy; lead-iodide perovskites; charge-carriers; molecules; solar-cells; trap states

Citation Formats

Zheng, Kaibo, Qatar Univ., Doha, Abdellah, Mohamed, South Valley Univ., Qena, Zhu, Qiushi, Qatar Univ., Doha, Kong, Qingyu, Jennings, Guy, Kurtz, Charles A., Messing, Maria E., Niu, Yuran, Gosztola, David J., Al-Marri, Mohammed J., Zhang, Xiaoyi, Pullerits, Tonu, and Canton, Sophie E.. Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles. United States: N. p., 2016. Web. https://doi.org/10.1021/acs.jpclett.6b02046.
Zheng, Kaibo, Qatar Univ., Doha, Abdellah, Mohamed, South Valley Univ., Qena, Zhu, Qiushi, Qatar Univ., Doha, Kong, Qingyu, Jennings, Guy, Kurtz, Charles A., Messing, Maria E., Niu, Yuran, Gosztola, David J., Al-Marri, Mohammed J., Zhang, Xiaoyi, Pullerits, Tonu, & Canton, Sophie E.. Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles. United States. https://doi.org/10.1021/acs.jpclett.6b02046
Zheng, Kaibo, Qatar Univ., Doha, Abdellah, Mohamed, South Valley Univ., Qena, Zhu, Qiushi, Qatar Univ., Doha, Kong, Qingyu, Jennings, Guy, Kurtz, Charles A., Messing, Maria E., Niu, Yuran, Gosztola, David J., Al-Marri, Mohammed J., Zhang, Xiaoyi, Pullerits, Tonu, and Canton, Sophie E.. Fri . "Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles". United States. https://doi.org/10.1021/acs.jpclett.6b02046. https://www.osti.gov/servlets/purl/1369031.
@article{osti_1369031,
title = {Direct experimental evidence for photoinduced strong-coupling polarons in organolead halide perovskite nanoparticles},
author = {Zheng, Kaibo and Qatar Univ., Doha and Abdellah, Mohamed and South Valley Univ., Qena and Zhu, Qiushi and Qatar Univ., Doha 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, Tonu and Canton, Sophie E.},
abstractNote = {Echoing the roaring success of their bulk coun-terparts, nano-objects built from organolead halide perov-skites (OLHP) present bright prospects for surpassing the performances of their conventional organic and inorganic analogues in photodriven technologies. Unraveling the pho-toinduced charge dynamics is essential for optimizing OLHP optoelectronic functionalities. However, mapping the carri-er-lattice interactions remains challenging, owing to their manifestations on multiple length scales and time scales. By correlating ultrafast time-resolved optical and X-ray absorp-tion 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 net Coulombic field caused by the dis-placed inorganic nuclei and the oriented organic cations. The transient structural change detected at the Pb L3 X-ray ab-sorption edge is well captured by a distortion with average bond elongation in the [PbBr6]2- motif. As a result, general implications for designing novel OLHP nanomaterials targeting the active utilization of these quasi-particles are outlined.},
doi = {10.1021/acs.jpclett.6b02046},
journal = {Journal of Physical Chemistry Letters},
number = 22,
volume = 7,
place = {United States},
year = {2016},
month = {10}
}

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