From Heterostructures to Solid-Solutions: Structural Tunability in Mixed Halide Perovskites

Donghoon Shin, Minliang Lai, Yongjin Shin, Jingshan S. Du, Liban Jibril, James M. Rondinelli, Chad A. Mirkin*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


The stability, reliability, and performance of halide-perovskite-based devices depend upon the structure, composition, and particle size of the device-enabling materials. Indeed, the degree of ion mixing in multicomponent perovskite crystals, although challenging to control, is a key factor in determining properties. Herein, an emerging method termed evaporation–crystallization polymer pen lithography is used to synthesize and systematically study the degree of ionic mixing of Cs0.5FA0.5PbX3 (FA = formamidinium; X = halide anion, ABX3) crystals, as a function of size, temperature, and composition. These experiments have led to the discovery of a heterostructure morphology where the A-site cations, Cs and FA, are segregated into the core and edge layers, respectively. Simulation and experimental results indicate that the heterostructures form as a consequence of a combination of both differences in solubility of the two ions in solution and the enthalpic preference for Cs–FA ion segregation. This preference for segregation can be overcome to form a solid-solution by decreasing crystal size (<60 nm) or increasing temperature. Finally, these tools are utilized to identify and synthesize solid-solution nanocrystals of Cs0.5FA0.5Pb(Br/I)3 that significantly suppress photoinduced anion migration compared to their bulk counterparts, offering a route to deliberately designed photostable optoelectronic materials.

Original languageEnglish (US)
Article number2205923
JournalAdvanced Materials
Issue number11
StatePublished - Mar 16 2023


  • halide perovskites
  • nanolithography
  • robust heterostructures
  • solid-solutions
  • structural tunability
  • suppressed photoinduced phase segregations

ASJC Scopus subject areas

  • Mechanics of Materials
  • Mechanical Engineering
  • Materials Science(all)


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