This content will become publicly available on Sat Sep 14 00:00:00 EDT 2024
Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites
Abstract
Triple cation, mixed halide perovskite compositions have been reported to be more thermally stable, exhibit fewer phase impurities, and show higher power conversion efficiency and better reproducibility than single cation perovskites. In this work, we explain the formation of Cs0.05FA0.81MA0.14Pb(I0.85Br0.15)3 via a multimodal in situ study combining structural information from synchrotron grazing-incidence wide-angle X-ray scattering (GIWAXS) and optical properties from photoluminescence (PL) spectroscopy with density functional theory calculations (DFT). The focus here is on the effects of the solvent and antisolvent during crystallization. The predominantly used solvents N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and the antisolvent chlorobenzene (CB) as well as the solvent-antisolvent-precursor interactions are investigated. Given the high elemental complexity and mutual interdependencies between solvent, antisolvent, and perovskite precursors, we found significant differences in the crystallization pathways. DMF-pure precursors show the formation of the DMF-containing intermediate phase and the nucleation of compositionally distinct perovskite phases, while when DMSO is added, only crystalline α- and δ-phases were found. In addition, the presence of DMSO helps the formation of α-perovskite. Coordination energy and bond order (BO) calculations support our experimental findings. Dripping of CB induces nucleation at room temperature, slows the α-phase formation rate, and appears to reduce the nucleation radius. Thesemore »
- Authors:
-
[6];
[3];
[1]
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
- King Fahd University of Petroleum and Minerals (KFUPM) (Saudi Arabia); Interdisciplinary Research Center for Intelligent Manufacturing and Robotics, KFUPM, Dhahran (Saudi Arabia)
- Eindhoven University of Technology (Netherlands)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; University of Nevada, Las Vegas, NV (United States)
- Friedrich-Alexander University Erlangen-Nuremberg, Bamberg (Germany)
- Sorbonne University, Paris (France); Centre National de la Recherche Scientifique (CNRS), Ecole Polytechnique, Palaiseau (France)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- University of Nevada, Las Vegas, NV (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); German Research Foundation (DFG); Bavaria California Technology Center (BaCaTeC); Dutch Research Council (NWO); China Scholarship Council (CSC); France Berkeley Fund (FBF)
- OSTI Identifier:
- 2234038
- Grant/Contract Number:
- AC02-05CH11231; 201808440385; SC0023355
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 35; Journal Issue: 18; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Singh, Mriganka, Abdelsamie, Maged, Li, Qihua, Kodalle, Tim, Lee, Do-Kyoung, Arnold, Simon, Ceratti, Davide R., Slack, Jonathan L., Schwartz, Craig P., Brabec, Christoph J., Tao, Shuxia, and Sutter-Fella, Carolin M. Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites. United States: N. p., 2023.
Web. doi:10.1021/acs.chemmater.3c00799.
Singh, Mriganka, Abdelsamie, Maged, Li, Qihua, Kodalle, Tim, Lee, Do-Kyoung, Arnold, Simon, Ceratti, Davide R., Slack, Jonathan L., Schwartz, Craig P., Brabec, Christoph J., Tao, Shuxia, & Sutter-Fella, Carolin M. Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites. United States. https://doi.org/10.1021/acs.chemmater.3c00799
Singh, Mriganka, Abdelsamie, Maged, Li, Qihua, Kodalle, Tim, Lee, Do-Kyoung, Arnold, Simon, Ceratti, Davide R., Slack, Jonathan L., Schwartz, Craig P., Brabec, Christoph J., Tao, Shuxia, and Sutter-Fella, Carolin M. Thu .
"Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites". United States. https://doi.org/10.1021/acs.chemmater.3c00799.
@article{osti_2234038,
title = {Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites},
author = {Singh, Mriganka and Abdelsamie, Maged and Li, Qihua and Kodalle, Tim and Lee, Do-Kyoung and Arnold, Simon and Ceratti, Davide R. and Slack, Jonathan L. and Schwartz, Craig P. and Brabec, Christoph J. and Tao, Shuxia and Sutter-Fella, Carolin M.},
abstractNote = {Triple cation, mixed halide perovskite compositions have been reported to be more thermally stable, exhibit fewer phase impurities, and show higher power conversion efficiency and better reproducibility than single cation perovskites. In this work, we explain the formation of Cs0.05FA0.81MA0.14Pb(I0.85Br0.15)3 via a multimodal in situ study combining structural information from synchrotron grazing-incidence wide-angle X-ray scattering (GIWAXS) and optical properties from photoluminescence (PL) spectroscopy with density functional theory calculations (DFT). The focus here is on the effects of the solvent and antisolvent during crystallization. The predominantly used solvents N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and the antisolvent chlorobenzene (CB) as well as the solvent-antisolvent-precursor interactions are investigated. Given the high elemental complexity and mutual interdependencies between solvent, antisolvent, and perovskite precursors, we found significant differences in the crystallization pathways. DMF-pure precursors show the formation of the DMF-containing intermediate phase and the nucleation of compositionally distinct perovskite phases, while when DMSO is added, only crystalline α- and δ-phases were found. In addition, the presence of DMSO helps the formation of α-perovskite. Coordination energy and bond order (BO) calculations support our experimental findings. Dripping of CB induces nucleation at room temperature, slows the α-phase formation rate, and appears to reduce the nucleation radius. These findings provide novel insights into solvent, antisolvent, and perovskite precursor interactions and their formation pathways. The complexity of interactions between solvents and reagents highlights the importance of understanding these effects to further improve the reproducibility and optimize processing conditions.},
doi = {10.1021/acs.chemmater.3c00799},
journal = {Chemistry of Materials},
number = 18,
volume = 35,
place = {United States},
year = {Thu Sep 14 00:00:00 EDT 2023},
month = {Thu Sep 14 00:00:00 EDT 2023}
}
Free Publicly Available Full Text
This content will become publicly available on September 14, 2024
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Evolution of Iodoplumbate Complexes in Methylammonium Lead Iodide Perovskite Precursor Solutions
journal, January 2017
- Sharenko, Alexander; Mackeen, Cameron; Jewell, Leila
- Chemistry of Materials, Vol. 29, Issue 3
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Highly Efficient and Stable Perovskite Solar Cells Based on Monolithically Grained CH 3 NH 3 PbI 3 Film
journal, December 2016
- Fei, Chengbin; Li, Bo; Zhang, Rong
- Advanced Energy Materials, Vol. 7, Issue 9
Stabilizing Perovskite Structures by Tuning Tolerance Factor: Formation of Formamidinium and Cesium Lead Iodide Solid-State Alloys
journal, December 2015
- Li, Zhen; Yang, Mengjin; Park, Ji-Sang
- Chemistry of Materials, Vol. 28, Issue 1
Progress on Perovskite Materials and Solar Cells with Mixed Cations and Halide Anions
journal, July 2017
- Ono, Luis K.; Juarez-Perez, Emilio J.; Qi, Yabing
- ACS Applied Materials & Interfaces, Vol. 9, Issue 36
Formamidinium Haloplumbate Intermediates: The Missing Link in a Chain of Hybrid Perovskites Crystallization
journal, August 2020
- Petrov, Andrey A.; Fateev, Sergey A.; Khrustalev, Victor N.
- Chemistry of Materials, Vol. 32, Issue 18
Optical Absorption‐Based In Situ Characterization of Halide Perovskites
journal, March 2020
- Babbe, Finn; Sutter‐Fella, Carolin M.
- Advanced Energy Materials
Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films
journal, March 2021
- Abdelsamie, Maged; Li, Tianyang; Babbe, Finn
- ACS Applied Materials & Interfaces, Vol. 13, Issue 11
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Perovskite ink with wide processing window for scalable high-efficiency solar cells
journal, March 2017
- Yang, Mengjin; Li, Zhen; Reese, Matthew O.
- Nature Energy, Vol. 2, Issue 5
Phase-Pure α-FAPbI3 for Perovskite Solar Cells
journal, February 2022
- Niu, Tingting; Chao, Lingfeng; Dong, Xue
- The Journal of Physical Chemistry Letters, Vol. 13, Issue 7
Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance
journal, October 2020
- Szostak, Rodrigo; Sanchez, Sandy; Marchezi, Paulo E.
- Advanced Functional Materials, Vol. 31, Issue 4
Pseudo-halide anion engineering for α-FAPbI3 perovskite solar cells
journal, April 2021
- Jeong, Jaeki; Kim, Minjin; Seo, Jongdeuk
- Nature, Vol. 592, Issue 7854
Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating
journal, September 2021
- Pratap, Shambhavi; Babbe, Finn; Barchi, Nicola S.
- Nature Communications, Vol. 12, Issue 1
Luminescent Intermediates and Humidity-Dependent Room-Temperature Conversion of the MAPbI 3 Perovskite Precursor
journal, October 2018
- Li, Jun; Dobrovolsky, Alexander; Merdasa, Aboma
- ACS Omega, Vol. 3, Issue 10
Solvent Engineering of the Precursor Solution toward Large‐Area Production of Perovskite Solar Cells
journal, March 2021
- Chao, Lingfeng; Niu, Tingting; Gao, Weiyin
- Advanced Materials, Vol. 33, Issue 14
Die Gesetze der Krystallochemie
journal, May 1926
- Goldschmidt, V. M.
- Die Naturwissenschaften, Vol. 14, Issue 21
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Revealing the Dynamics of Hybrid Metal Halide Perovskite Formation via Multimodal In Situ Probes
journal, December 2019
- Song, Tze‐Bin; Yuan, Zhenghao; Mori, Megumi
- Advanced Functional Materials, Vol. 30, Issue 6
Synthetic Approaches for Halide Perovskite Thin Films
journal, November 2018
- Dunlap-Shohl, Wiley A.; Zhou, Yuanyuan; Padture, Nitin P.
- Chemical Reviews, Vol. 119, Issue 5
Lewis Acid–Base Adduct Approach for High Efficiency Perovskite Solar Cells
journal, January 2016
- Lee, Jin-Wook; Kim, Hui-Seon; Park, Nam-Gyu
- Accounts of Chemical Research, Vol. 49, Issue 2
Crystal Structure of DMF-Intermediate Phases Uncovers the Link Between CH 3 NH 3 PbI 3 Morphology and Precursor Stoichiometry
journal, September 2017
- Petrov, Andrey A.; Sokolova, Iuliia P.; Belich, Nikolai A.
- The Journal of Physical Chemistry C, Vol. 121, Issue 38
Building Blocks of Hybrid Perovskites: A Photoluminescence Study of Lead‐Iodide Solution Species
journal, September 2020
- Shargaieva, Oleksandra; Kuske, Lena; Rappich, Jörg
- ChemPhysChem, Vol. 21, Issue 20
Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells
journal, July 2014
- Jeon, Nam Joong; Noh, Jun Hong; Kim, Young Chan
- Nature Materials, Vol. 13, Issue 9, p. 897-903
Growth modes and quantum confinement in ultrathin vapour-deposited MAPbI 3 films
journal, January 2019
- Parrott, Elizabeth S.; Patel, Jay B.; Haghighirad, Amir-Abbas
- Nanoscale, Vol. 11, Issue 30
The role of solvents in the formation of methylammonium lead triiodide perovskite
journal, May 2022
- Jiang, Junke; Vicent-Luna, José Manuel; Tao, Shuxia
- Journal of Energy Chemistry, Vol. 68
Long-Distance Charge Carrier Funneling in Perovskite Nanowires Enabled by Built-in Halide Gradient
journal, January 2017
- Tian, Wenming; Leng, Jing; Zhao, Chunyi
- Journal of the American Chemical Society, Vol. 139, Issue 2
Introducing DDEC6 atomic population analysis: part 2. Computed results for a wide range of periodic and nonperiodic materials
journal, January 2016
- Limas, Nidia Gabaldon; Manz, Thomas A.
- RSC Advances, Vol. 6, Issue 51
Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction
journal, December 2020
- Al-Ashouri, Amran; Köhnen, Eike; Li, Bor
- Science, Vol. 370, Issue 6522
Performance-limiting formation dynamics in mixed-halide perovskites
journal, November 2021
- Huang, Tianyi; Tan, Shaun; Nuryyeva, Selbi
- Science Advances, Vol. 7, Issue 46
Influence of Solvent Coordination on Hybrid Organic–Inorganic Perovskite Formation
journal, November 2017
- Hamill, J. Clay; Schwartz, Jeffrey; Loo, Yueh-Lin
- ACS Energy Letters, Vol. 3, Issue 1
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
An open-access database and analysis tool for perovskite solar cells based on the FAIR data principles
journal, December 2021
- Jacobsson, T. Jesper; Hultqvist, Adam; García-Fernández, Alberto
- Nature Energy, Vol. 7, Issue 1
Optical in situ monitoring during the synthesis of halide perovskite solar cells reveals formation kinetics and evolution of optoelectronic properties
journal, January 2020
- Suchan, Klara; Just, Justus; Becker, Pascal
- Journal of Materials Chemistry A, Vol. 8, Issue 20
Cation and anion immobilization through chemical bonding enhancement with fluorides for stable halide perovskite solar cells
journal, May 2019
- Li, Nengxu; Tao, Shuxia; Chen, Yihua
- Nature Energy, Vol. 4, Issue 5
A Systematic Review of Metal Halide Perovskite Crystallization and Film Formation Mechanism Unveiled by In Situ GIWAXS
journal, October 2021
- Qin, Minchao; Chan, Pok Fung; Lu, Xinhui
- Advanced Materials, Vol. 33, Issue 51
Perovskite Photovoltaics: The Significant Role of Ligands in Film Formation, Passivation, and Stability
journal, January 2019
- Zhang, Hong; Nazeeruddin, Mohammad Khaja; Choy, Wallace C. H.
- Advanced Materials, Vol. 31, Issue 8
Introducing DDEC6 atomic population analysis: part 3. Comprehensive method to compute bond orders
journal, January 2017
- Manz, Thomas A.
- RSC Adv., Vol. 7, Issue 72
Recent Progress in Halide Perovskite Radiation Detectors for Gamma-Ray Spectroscopy
journal, February 2022
- Liu, Fangze; Wu, Rong; Wei, Jing
- ACS Energy Letters, Vol. 7, Issue 3
Impact of Processing on Structural and Compositional Evolution in Mixed Metal Halide Perovskites during Film Formation
journal, July 2020
- Abdelsamie, Maged; Xu, Junwei; Bruening, Karsten
- Advanced Functional Materials, Vol. 30, Issue 38
Accelerated formation of iodine vacancies in CH3NH3PbI3 perovskites: The impact of oxygen and charges
journal, December 2022
- Li, Qihua; Gaastra‐Nedea, Silvia; Smeulders, David
- EcoMat, Vol. 5, Issue 4
Nanocrystalline Polymorphic Energy Funnels for Efficient and Stable Perovskite Light-Emitting Diodes
journal, April 2021
- Lee, Do-Kyoung; Shin, Yunseop; Jang, Ho Jin
- ACS Energy Letters, Vol. 6, Issue 5
Hybrid Halide Perovskite Solar Cell Precursors: Colloidal Chemistry and Coordination Engineering behind Device Processing for High Efficiency
journal, March 2015
- Yan, Keyou; Long, Mingzhu; Zhang, Tiankai
- Journal of the American Chemical Society, Vol. 137, Issue 13
Perovskite-Inspired Photovoltaic Materials: Toward Best Practices in Materials Characterization and Calculations
journal, February 2017
- Hoye, Robert L. Z.; Schulz, Philip; Schelhas, Laura T.
- Chemistry of Materials, Vol. 29, Issue 5
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
journal, February 2015
- Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I.
- Nano Letters, Vol. 15, Issue 6
Compositional effect on water adsorption on metal halide perovskites
journal, February 2021
- Li, Qihua; Chen, Zehua; Tranca, Ionut
- Applied Surface Science, Vol. 538