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Title: Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization

Metastable structural polymorphs can have superior properties and applications to their thermodynamically stable phases, but the rational synthesis of metastable phases is a challenge. Here in this paper, a new strategy for stabilizing metastable phases using surface functionalization is demonstrated using the example of formamidinium lead iodide (FAPbI 3) perovskite, which is metastable at room temperature (RT) but holds great promises in solar and light-emitting applications. We show that, through surface ligand functionalization during direct solution growth at RT, pure FAPbI 3 in the cubic perovskite phase can be stabilized in nanostructures and thin films at RT without cation or anion alloying. Surface characterizations reveal that long-chain alkyl or aromatic ammonium (LA) cations bind to the surface of perovskite structure. Calculations show that such functionalization reduces the surface energy and plays a dominant role in stabilizing the metastable perovskite phase. Excellent photophysics and optically pumped lasing from the stabilized single-crystal FAPbI 3 nanoplates with low thresholds were demonstrated. High-performance solar cells can be fabricated with such directly synthesized stabilized phase-pure FAPbI3 with a lower bandgap. Our results offer new insights on the surface chemistry of perovskite materials and provide a new strategy for stabilizing metastable perovskites and metastable polymorphs ofmore » solid materials in general.« less
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [2] ;  [2] ; ORCiD logo [3] ; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry
  2. Nanjing Univ. of Technology (China). Dept. of Applied Physics
  3. Columbia Univ., New York, NY (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
SC0010692
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 7; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Columbia Univ., New York, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY; 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; lead halide perovskites; Metastable polymorphs; nanolasers; perovskite photovoltaics; photophysics; surface functionalization
OSTI Identifier:
1474062

Fu, Yongping, Wu, Tao, Wang, Jue, Zhai, Jianyuan, Shearer, Melinda J., Zhao, Yuzhou, Hamers, Robert J., Kan, Erjun, Deng, Kaiming, Zhu, X. -Y., and Jin, Song. Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization. United States: N. p., Web. doi:10.1021/acs.nanolett.7b01500.
Fu, Yongping, Wu, Tao, Wang, Jue, Zhai, Jianyuan, Shearer, Melinda J., Zhao, Yuzhou, Hamers, Robert J., Kan, Erjun, Deng, Kaiming, Zhu, X. -Y., & Jin, Song. Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization. United States. doi:10.1021/acs.nanolett.7b01500.
Fu, Yongping, Wu, Tao, Wang, Jue, Zhai, Jianyuan, Shearer, Melinda J., Zhao, Yuzhou, Hamers, Robert J., Kan, Erjun, Deng, Kaiming, Zhu, X. -Y., and Jin, Song. 2017. "Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization". United States. doi:10.1021/acs.nanolett.7b01500. https://www.osti.gov/servlets/purl/1474062.
@article{osti_1474062,
title = {Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization},
author = {Fu, Yongping and Wu, Tao and Wang, Jue and Zhai, Jianyuan and Shearer, Melinda J. and Zhao, Yuzhou and Hamers, Robert J. and Kan, Erjun and Deng, Kaiming and Zhu, X. -Y. and Jin, Song},
abstractNote = {Metastable structural polymorphs can have superior properties and applications to their thermodynamically stable phases, but the rational synthesis of metastable phases is a challenge. Here in this paper, a new strategy for stabilizing metastable phases using surface functionalization is demonstrated using the example of formamidinium lead iodide (FAPbI3) perovskite, which is metastable at room temperature (RT) but holds great promises in solar and light-emitting applications. We show that, through surface ligand functionalization during direct solution growth at RT, pure FAPbI3 in the cubic perovskite phase can be stabilized in nanostructures and thin films at RT without cation or anion alloying. Surface characterizations reveal that long-chain alkyl or aromatic ammonium (LA) cations bind to the surface of perovskite structure. Calculations show that such functionalization reduces the surface energy and plays a dominant role in stabilizing the metastable perovskite phase. Excellent photophysics and optically pumped lasing from the stabilized single-crystal FAPbI3 nanoplates with low thresholds were demonstrated. High-performance solar cells can be fabricated with such directly synthesized stabilized phase-pure FAPbI3 with a lower bandgap. Our results offer new insights on the surface chemistry of perovskite materials and provide a new strategy for stabilizing metastable perovskites and metastable polymorphs of solid materials in general.},
doi = {10.1021/acs.nanolett.7b01500},
journal = {Nano Letters},
number = 7,
volume = 17,
place = {United States},
year = {2017},
month = {6}
}