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Title: In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]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 [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.

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 Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1379893
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: 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. https://doi.org/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. 2017. "In situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4– cage nanoparticles". United States. https://doi.org/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},
url = {https://www.osti.gov/biblio/1379893}, journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 8,
place = {United States},
year = {Wed Jun 21 00:00:00 EDT 2017},
month = {Wed Jun 21 00:00:00 EDT 2017}
}

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Works referenced in this record:

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A Fast Deposition-Crystallization Procedure for Highly Efficient Lead Iodide Perovskite Thin-Film Solar Cells
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Additive Enhanced Crystallization of Solution-Processed Perovskite for Highly Efficient Planar-Heterojunction Solar Cells
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Fast Printing and In Situ Morphology Observation of Organic Photovoltaics Using Slot-Die Coating
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A Closer Look into Two-Step Perovskite Conversion with X-ray Scattering
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Microstructures of Organometal Trihalide Perovskites for Solar Cells: Their Evolution from Solutions and Characterization
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Formation Mechanism and Control of Perovskite Films from Solution to Crystalline Phase Studied by in Situ Synchrotron Scattering
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Crystallization Kinetics of Organic–Inorganic Trihalide Perovskites and the Role of the Lead Anion in Crystal Growth
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Hybrid Halide Perovskite Solar Cell Precursors: Colloidal Chemistry and Coordination Engineering behind Device Processing for High Efficiency
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Highly Reproducible Perovskite Solar Cells with Average Efficiency of 18.3% and Best Efficiency of 19.7% Fabricated via Lewis Base Adduct of Lead(II) Iodide
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Chemical Pathways Connecting Lead(II) Iodide and Perovskite via Polymeric Plumbate(II) Fiber
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Rhythmic Crystallization of Poly-L-alanine
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High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells
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Works referencing / citing this record:

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Improved Performance of Printable Perovskite Solar Cells with Bifunctional Conjugated Organic Molecule
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In Situ Real-Time Study of the Dynamic Formation and Conversion Processes of Metal Halide Perovskite Films
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Kinetic Stabilization of the Sol-Gel State in Perovskites Enables Facile Processing of High-Efficiency Solar Cells
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Manipulating the Mixed‐Perovskite Crystallization Pathway Unveiled by In Situ GIWAXS
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