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Title: Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating

Abstract

Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [2];  [2]; ORCiD logo [2];  [2]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [6]
  1. Technische Univ. München, Garching (Germany); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); École Polytechnique Fédérale de Lausanne (Switzerland)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Pennsylvania State Univ., University Park, PA (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  6. Technische Univ. München, Garching (Germany)
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1829026
Alternate Identifier(s):
OSTI ID: 1829215
Report Number(s):
LLNL-JRNL-826733
Journal ID: ISSN 2041-1723; 1041529; TRN: US2216344
Grant/Contract Number:  
AC52-07NA27344; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Solar cells; Structural properties

Citation Formats

Pratap, Shambhavi, Babbe, Finn, Barchi, Nicola S., Yuan, Zhenghao, Luong, Tina, Haber, Zach, Song, Tze-Bin, Slack, Jonathan L., Stan, Camelia V., Tamura, Nobumichi, Sutter-Fella, Carolin M., and Müller-Buschbaum, Peter. Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating. United States: N. p., 2021. Web. doi:10.1038/s41467-021-25898-5.
Pratap, Shambhavi, Babbe, Finn, Barchi, Nicola S., Yuan, Zhenghao, Luong, Tina, Haber, Zach, Song, Tze-Bin, Slack, Jonathan L., Stan, Camelia V., Tamura, Nobumichi, Sutter-Fella, Carolin M., & Müller-Buschbaum, Peter. Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating. United States. https://doi.org/10.1038/s41467-021-25898-5
Pratap, Shambhavi, Babbe, Finn, Barchi, Nicola S., Yuan, Zhenghao, Luong, Tina, Haber, Zach, Song, Tze-Bin, Slack, Jonathan L., Stan, Camelia V., Tamura, Nobumichi, Sutter-Fella, Carolin M., and Müller-Buschbaum, Peter. Fri . "Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating". United States. https://doi.org/10.1038/s41467-021-25898-5. https://www.osti.gov/servlets/purl/1829026.
@article{osti_1829026,
title = {Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating},
author = {Pratap, Shambhavi and Babbe, Finn and Barchi, Nicola S. and Yuan, Zhenghao and Luong, Tina and Haber, Zach and Song, Tze-Bin and Slack, Jonathan L. and Stan, Camelia V. and Tamura, Nobumichi and Sutter-Fella, Carolin M. and Müller-Buschbaum, Peter},
abstractNote = {Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.},
doi = {10.1038/s41467-021-25898-5},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Fri Sep 24 00:00:00 EDT 2021},
month = {Fri Sep 24 00:00:00 EDT 2021}
}

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