Crystal Structure of DMF-Intermediate Phases Uncovers the Link between CH3NH3PbI3 Morphology and Precursor Stoichiometry

We found for the first time a new origin of selection of perovskite crystallization pathways from DMF solutions containing MAI and PbI2 to present here a comprehensive study of a full set of essential intermediate phases determining the perovskite's morphology. For all three discovered structurally different intermediate phases forming at a given precursor ratio, we refined their crystal structures by synchrotron X-ray radiation and investigated dynamics and phase assemblage in the course of decomposition. As a result, we revealed a clear correlation between the composition of the intermediate phases, peculiarities of their crystal structure, and the morphology of the final perovskite films. Using the DFT method we calculated formation enthalpies of these intermediate phases and explained the preferential precipitation of DMSO-adduct rather than DMF-adduct in an antisolvent approach. This finding opens up a possibility of design-on-demand of perovskite materials using simple soft chemistry approaches. © 2017 American Chemical Society.

Petrov A.A. 1 , Sokolova I.P.1 , Belich N.A.1 , Peters G.S.2 , Dorovatovskii P.V.2 , Zubavichus Y.V.2 , Khrustalev V.N. 3 , Petrov A.V.4 , Grätzel M.5 , Goodilin E.A.1, 6 , Tarasov A.B.1, 6
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  • 1 Laboratory of New Materials for Solar Energetics, Department of Materials Science, Lomonosov Moscow State University, Lenin Hills, Moscow, 119991, Russian Federation
  • 2 National Research Center, Kurchatov Unstitute, Moscow, 123182, Russian Federation
  • 3 Department of Inorganic Chemistry, Peoples' Friendship University of Russia, RUDN University, Moscow, 117198, Russian Federation
  • 4 Institute of Chemistry, Saint-Petersburg State University, 26 Universitetskii prospect, Saint-Petersburg, 198504, Russian Federation
  • 5 Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Station 6, Lausanne, CH-1015, Switzerland
  • 6 Laboratory of Inorganic Materials, Department of Chemistry, Lomonosov Moscow State University, Lenin Hills, Moscow, 119991, Russian Federation
Ключевые слова
Design for testability; Morphology; Perovskite; Crystallization pathway; Formation enthalpy; Intermediate phasis; Perovskite films; Phase assemblages; Precursor ratios; Soft Chemistry; Synchrotron x-ray radiation; Crystal structure
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