Multiple-Stage Structure Transformation of Organic-Inorganic Hybrid Perovskite CH3NH3PbI3

Mengjin Yang, Kai Zhu, Qiong Chen, Henan Liu, Hui-Seon Kim, Yucheng Liu, Naili Yue, Gang Ren, Shengzhong Liu, Nam-Gyu Park, Yong Zhang

Research output: Contribution to journalArticlepeer-review

24 Scopus Citations


By performing spatially resolved Raman and photoluminescence spectroscopy with varying excitation wavelength, density, and data acquisition parameters, we achieve a unified understanding towards the spectroscopy signatures of the organic-inorganic hybrid perovskite, transforming from the pristine state (CH3NH3PbI3) to the fully degraded state (i.e., PbI2) for samples with varying crystalline domain size from mesoscopic scale (approximately 100 nm) to macroscopic size (centimeters), synthesized by three different techniques. We show that the hybrid perovskite exhibits multiple stages of structure transformation occurring either spontaneously or under light illumination, with exceptionally high sensitivity to the illumination conditions (e.g., power, illumination time, and interruption pattern). We highlight four transformation stages (stages I-IV, with stage I being the pristine state) along either the spontaneous or photoinduced degradation path exhibiting distinctly different Raman spectroscopy features at each stage, and point out that previously reported Raman spectra in the literature reflect highly degraded structures of either stage III or stage IV. Additional characteristic optical features of partially degraded materials under the joint action of spontaneous and photodegradation are also given. This study offers reliable benchmark results for understanding the intrinsic material properties and structure transformation of this unique category of hybrid materials, and the findings are pertinently important to a wide range of potential applications where the hybrid material is expected to function in greatly different environment and light-matter interaction conditions.

Original languageAmerican English
Article number31042
Number of pages20
JournalPhysical Review X
Issue number3
StatePublished - 2016

Bibliographical note

Publisher Copyright:
© American Physical Society.

NREL Publication Number

  • NREL/JA-5900-67314


  • hybrid perovskite
  • material properties
  • structure


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