<p>Although edges and defects constitute only a small fraction of crystalline materials, they exert an outsized impact on a material′s properties. Organic–inorganic halide perovskites are promising next-generation semiconductor materials with superior cost effectiveness and interesting optoelectronic properties<sup><CitationRef AdditionalCitationIDS="CR2" CitationID="CR1">1</CitationRef>–<CitationRef CitationID="CR3">3</CitationRef></sup>. However, clear images of their edges have remained challenging to obtain owing to their extreme sensitivity<sup><CitationRef CitationID="CR4">4</CitationRef>,<CitationRef CitationID="CR5">5</CitationRef></sup>. Using truly high-speed ultralow-dose four-dimensional scanning transmission electron microscopy with dose fractionation, we perform ptychography at, to our knowledge, the lowest-dose atomic resolution to date, revealing not only the detailed atomic structure of the edges of a halide perovskite but also their structural dynamics. A majority methylammonium (MA) and iodine (I) edge termination is observed in methylammonium lead iodide (MAPbI<sub>3</sub>), and the damage rate of its edges and internal defects is found to depend on the concentration and type of vacancies present, with a preponderance of I vacancies in particular correlating with higher rates of damage.</p>

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Atomically resolved edges and defects in lead halide perovskites

  • Biao Yuan,
  • Zeyu Wang,
  • Shuchen Zhang,
  • Christoph Hofer,
  • Chuang Gao,
  • Tamazouzt Chennit,
  • Hongsheng Shi,
  • Xiaoyan Wu,
  • Yu Han,
  • Letian Dou,
  • Yi Yu,
  • Timothy J. Pennycook

摘要

Although edges and defects constitute only a small fraction of crystalline materials, they exert an outsized impact on a material′s properties. Organic–inorganic halide perovskites are promising next-generation semiconductor materials with superior cost effectiveness and interesting optoelectronic properties13. However, clear images of their edges have remained challenging to obtain owing to their extreme sensitivity4,5. Using truly high-speed ultralow-dose four-dimensional scanning transmission electron microscopy with dose fractionation, we perform ptychography at, to our knowledge, the lowest-dose atomic resolution to date, revealing not only the detailed atomic structure of the edges of a halide perovskite but also their structural dynamics. A majority methylammonium (MA) and iodine (I) edge termination is observed in methylammonium lead iodide (MAPbI3), and the damage rate of its edges and internal defects is found to depend on the concentration and type of vacancies present, with a preponderance of I vacancies in particular correlating with higher rates of damage.