Halide perovskite materials have attracted great interest for applications in low-cost, solution-processed solar cells and other optoelectronics applications. The role of moisture in perovskite device degradation and crystal formation processes remains poorly understood. Here, we use a data-driven approach to discover the influence of trace amounts of water on perovskite crystal formation by analyzing a comprehensive dataset of 8470 inverse-temperature crystallization lead iodide perovskite synthesis reactions, performed over 20 months using a robotic system. We identified discrepancies between the empirical crystal formation rates in batches of experiments conducted under different ambient relative humidity conditions for each organoammonium cation. We prioritized these using a statistical model and then used the robotic system to conduct 1296 controlled interventional experiments, in which small amounts of water were deliberately introduced to the reactions. The addition of trace amounts of water promotes crystal formation for 4-methoxyphenylammonium lead iodide and iso-propylammonium lead iodide and inhibits crystal formation for dimethylammonium lead iodide and acetamidinium lead iodide. We also performed thin-film syntheses of these four materials and determined the grain size distributions using scanning electron microscopy. The addition of water results in smaller grain sizes for dimethylammonium and larger grain sizes for iso-propylammonium, consistent with earlier or delayed nucleation, respectively. The agreement between the inverse temperature crystallization and thin film results indicates that this is a feature of the organoammonium-water interaction that persists despite differences in the synthesis method.
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26 July 2021
Research Article|
July 29 2021
Using automated serendipity to discover how trace water promotes and inhibits lead halide perovskite crystal formation
Philip W. Nega;
Philip W. Nega
1
The Molecular Foundry, Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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Zhi Li
;
Zhi Li
1
The Molecular Foundry, Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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Victor Ghosh;
Victor Ghosh
2
Bronx High School of Science
, 75 W 205th Street, The Bronx, New York 10468, USA
3
Department of Chemistry, Fordham University
, 441 E. Fordham Road, The Bronx, New York 10458, USA
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Janak Thapa;
Janak Thapa
4
Massachusetts Institute of Technology
, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
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Shijing Sun
;
Shijing Sun
4
Massachusetts Institute of Technology
, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
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Noor Titan Putri Hartono
;
Noor Titan Putri Hartono
4
Massachusetts Institute of Technology
, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
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Mansoor Ani Najeeb Nellikkal
;
Mansoor Ani Najeeb Nellikkal
5
Department of Chemistry, Haverford College
, 370 Lancaster Avenue, Haverford, Pennsylvania 19041, USA
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Alexander J. Norquist
;
Alexander J. Norquist
5
Department of Chemistry, Haverford College
, 370 Lancaster Avenue, Haverford, Pennsylvania 19041, USA
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Tonio Buonassisi
;
Tonio Buonassisi
4
Massachusetts Institute of Technology
, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
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Emory M. Chan
;
Emory M. Chan
1
The Molecular Foundry, Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
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Joshua Schrier
Joshua Schrier
a)
3
Department of Chemistry, Fordham University
, 441 E. Fordham Road, The Bronx, New York 10458, USA
a)Author to whom correspondence should be addressed: [email protected]
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Philip W. Nega
1
Victor Ghosh
2,3
Janak Thapa
4
Shijing Sun
4
Noor Titan Putri Hartono
4
Mansoor Ani Najeeb Nellikkal
5
Alexander J. Norquist
5
Tonio Buonassisi
4
Emory M. Chan
1
Joshua Schrier
3,a)
1
The Molecular Foundry, Lawrence Berkeley National Laboratory
, 1 Cyclotron Road, Berkeley, California 94720, USA
2
Bronx High School of Science
, 75 W 205th Street, The Bronx, New York 10468, USA
3
Department of Chemistry, Fordham University
, 441 E. Fordham Road, The Bronx, New York 10458, USA
4
Massachusetts Institute of Technology
, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
5
Department of Chemistry, Haverford College
, 370 Lancaster Avenue, Haverford, Pennsylvania 19041, USA
a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the APL Special Collection on New Solution-processed Perovskites and Perovskite-inspired Optoelectronic Materials and Devices.
Appl. Phys. Lett. 119, 041903 (2021)
Article history
Received:
June 11 2021
Accepted:
July 14 2021
Citation
Philip W. Nega, Zhi Li, Victor Ghosh, Janak Thapa, Shijing Sun, Noor Titan Putri Hartono, Mansoor Ani Najeeb Nellikkal, Alexander J. Norquist, Tonio Buonassisi, Emory M. Chan, Joshua Schrier; Using automated serendipity to discover how trace water promotes and inhibits lead halide perovskite crystal formation. Appl. Phys. Lett. 26 July 2021; 119 (4): 041903. https://doi.org/10.1063/5.0059767
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