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Title: Multiple-stage structure transformation of organic-inorganic hybrid perovskite CH3NH3PbI3

In this study, 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 findingsmore » 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.« less
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ;  [4] ;  [3] ;  [2] ;  [1]
  1. The Univ. of North Carolina at Charlotte, Charlotte, NC (United States)
  2. Sungkyunkwan Univ., Suwon (South Korea)
  3. Shaanxi Normal Univ., Xi'an (China)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
OSTI Identifier:
1330000
Report Number(s):
NREL/JA--5900-67314
Journal ID: ISSN 2160-3308; PRXHAE
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Volume: 6; Journal Issue: 3; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society
Research Org:
NREL (National Renewable Energy Laboratory (NREL), Golden, CO (United States))
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE hybrid perovskite; structure; material properties