Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites

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.

doi:10.1021/acs.chemmater.3c00799

Effect of the Precursor Chemistry on the Crystallization of Triple Cation Mixed Halide Perovskites

Journal Article · Thu Sep 14 04:00:00 EDT 2023 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.3c00799· OSTI ID:2234038

Singh, Mriganka ^[1]; Abdelsamie, Maged ^[2]; Li, Qihua ^[3]; Kodalle, Tim ^[4]; Lee, Do-Kyoung ^[5]; ^[6]; Ceratti, Davide R. ^[7]; Slack, Jonathan L. ^[8]; Schwartz, Craig P. ^[9]; Brabec, Christoph J. ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: 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)

Grant/Contract Number:: AC02-05CH11231; SC0023355

OSTI ID:: 2234038

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 18 Vol. 35; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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