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Title: In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI 6] 4– cage nanoparticles

Abstract

Hybrid lead halide perovskites have emerged as high-performance photovoltaic materials with their extraordinary optoelectronic properties. In particular, the remarkable device efficiency is strongly influenced by the perovskite crystallinity and the film morphology. Here, we investigate the perovskites crystallisation kinetics and growth mechanism in real time from liquid precursor continually to the final uniform film. We utilize some advanced in situ characterisation techniques including synchrotron-based grazing incident X-ray diffraction to observe crystal structure and chemical transition of perovskites. The nano-assemble model from perovskite intermediated [PbI 6] 4– cage nanoparticles to bulk polycrystals is proposed to understand perovskites formation at a molecular- or nano-level. A crystallisation-depletion mechanism is developed to elucidate the periodic crystallisation and the kinetically trapped morphology at a mesoscopic level. Based on these in situ dynamics studies, the whole process of the perovskites formation and transformation from the molecular to the microstructure over relevant temperature and time scales is successfully demonstrated.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3];  [4];  [4];  [4];  [4];  [4]; ORCiD logo [4];  [4];  [5];  [6];  [7];  [8]; ORCiD logo [9];  [9]
  1. Peking Univ., Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Peking Univ., Beijing (China); Ecole Polytechnique Federale de Lausanne, Lausanne (Switzerland)
  3. Peking Univ., Beijing (China)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Univ. of Surrey, Surrey (United Kingdom)
  6. Ecole Polytechnique Federale de Lausanne, Lausanne (Switzerland)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Shanghai Jiaotong Univ., Shanghai (China)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Massachusetts, Amherst, MA (United States)
  9. Peking Univ., Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China); Shanxi Univ. Shanxi (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1379893
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Energy; Materials chemistry; Materials for energy and catalysis

Citation Formats

Hu, Qin, Zhao, Lichen, Wu, Jiang, Gao, Ke, Luo, Deying, Jiang, Yufeng, Zhang, Ziyi, Zhu, Chenhui, Schaible, Eric, Hexemer, Alexander, Wang, Cheng, Liu, Yi, Zhang, Wei, Gratzel, Michael, Liu, Feng, Russell, Thomas P., Zhu, Rui, and Gong, Qihuang. In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4– cage nanoparticles. United States: N. p., 2017. Web. doi:10.1038/ncomms15688.
Hu, Qin, Zhao, Lichen, Wu, Jiang, Gao, Ke, Luo, Deying, Jiang, Yufeng, Zhang, Ziyi, Zhu, Chenhui, Schaible, Eric, Hexemer, Alexander, Wang, Cheng, Liu, Yi, Zhang, Wei, Gratzel, Michael, Liu, Feng, Russell, Thomas P., Zhu, Rui, & Gong, Qihuang. In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4– cage nanoparticles. United States. doi:10.1038/ncomms15688.
Hu, Qin, Zhao, Lichen, Wu, Jiang, Gao, Ke, Luo, Deying, Jiang, Yufeng, Zhang, Ziyi, Zhu, Chenhui, Schaible, Eric, Hexemer, Alexander, Wang, Cheng, Liu, Yi, Zhang, Wei, Gratzel, Michael, Liu, Feng, Russell, Thomas P., Zhu, Rui, and Gong, Qihuang. Wed . "In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4– cage nanoparticles". United States. doi:10.1038/ncomms15688. https://www.osti.gov/servlets/purl/1379893.
@article{osti_1379893,
title = {In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4– cage nanoparticles},
author = {Hu, Qin and Zhao, Lichen and Wu, Jiang and Gao, Ke and Luo, Deying and Jiang, Yufeng and Zhang, Ziyi and Zhu, Chenhui and Schaible, Eric and Hexemer, Alexander and Wang, Cheng and Liu, Yi and Zhang, Wei and Gratzel, Michael and Liu, Feng and Russell, Thomas P. and Zhu, Rui and Gong, Qihuang},
abstractNote = {Hybrid lead halide perovskites have emerged as high-performance photovoltaic materials with their extraordinary optoelectronic properties. In particular, the remarkable device efficiency is strongly influenced by the perovskite crystallinity and the film morphology. Here, we investigate the perovskites crystallisation kinetics and growth mechanism in real time from liquid precursor continually to the final uniform film. We utilize some advanced in situ characterisation techniques including synchrotron-based grazing incident X-ray diffraction to observe crystal structure and chemical transition of perovskites. The nano-assemble model from perovskite intermediated [PbI6]4– cage nanoparticles to bulk polycrystals is proposed to understand perovskites formation at a molecular- or nano-level. A crystallisation-depletion mechanism is developed to elucidate the periodic crystallisation and the kinetically trapped morphology at a mesoscopic level. Based on these in situ dynamics studies, the whole process of the perovskites formation and transformation from the molecular to the microstructure over relevant temperature and time scales is successfully demonstrated.},
doi = {10.1038/ncomms15688},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {6}
}

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