Atomic-scale imaging of CH3NH3PbI3 structure and its decomposition pathway

Chen，Shulin1,2; Wu，Changwei3; Han，Bo1; Liu，Zhetong1; Mi，Zhou4; Hao，Weizhong4; Zhao，Jinjin4; Wang，Xiao3,5; Zhang，Qing6; Liu，Kaihui7,8; Qi，Junlei2; Cao，Jian2; Feng，Jicai2; Yu，Dapeng9; Li，Jiangyu3,5,10; Gao，Peng1,8,11

2021-12-01

10.1038/s41467-021-25832-9

Nature Communications   影响因子和分区

2041-1723

Understanding the atomic structure and structural instability of organic-inorganic hybrid perovskites is the key to appreciate their remarkable photoelectric properties and understand failure mechanism. Here, using low-dose imaging technique by direct-detection electron-counting camera in a transmission electron microscope, we investigate the atomic structure and decomposition pathway of CHNHPbI (MAPbI) at the atomic scale. We successfully image the atomic structure of perovskite in real space under ultra-low electron dose condition, and observe a two-step decomposition process, i.e., initial loss of MA followed by the collapse of perovskite structure into 6H-PbI with their critical threshold doses also determined. Interestingly, an intermediate phase (MAPbI) with locally ordered vacancies can robustly exist before perovskite collapses, enlightening strategies for prevention and recovery of perovskite structure during the degradation. Associated with the structure evolution, the bandgap gradually increases from ~1.6 eV to ~2.1 eV. In addition, it is found that C-N bonds can be readily destroyed under irradiation, releasing NH and HI and leaving hydrocarbons. These findings enhance our understanding of the photoelectric properties and failure mechanism of MAPbI, providing potential strategies into material optimization.

SCI

英语

NI期刊

其他

WOS:000697033200024

2-s2.0-85115426351

Scopus

1.Electron Microscopy Laboratory,International Center for Quantum Materials,School of Physics,Peking University,Beijing,China
2.State Key Laboratory of Advanced Welding and Joining,Harbin Institute of Technology,Harbin,China
3.Shenzhen Key Laboratory of Nanobiomechanics,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen,China
4.School of Materials Science and Engineering,School of Mechanical Engineering,Shijiazhuang Tiedao University,Shijiazhuang,China
5.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,China
6.Department of Materials Science and Engineering,College of Engineering,Peking University,Beijing,China
7.State Key Laboratory for Mesoscopic Physics,School of Physics,Peking University,Beijing,China
8.Collaborative Innovation Center of Quantum Matter,Beijing,China
9.Department of Physics,South University of Science and Technology,Shenzhen,China
10.Guangdong Provisional Key Laboratory of Functional Oxide Materials and Devices,Southern University of Science and Technology,Shenzhen,China
11.Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced Materials,Peking University,Beijing,China

Chen，Shulin,Wu，Changwei,Han，Bo,et al. Atomic-scale imaging of CH3NH3PbI3 structure and its decomposition pathway[J]. Nature Communications,2021,12(1).

Chen，Shulin.,Wu，Changwei.,Han，Bo.,Liu，Zhetong.,Mi，Zhou.,...&Gao，Peng.(2021).Atomic-scale imaging of CH3NH3PbI3 structure and its decomposition pathway.Nature Communications,12(1).

Chen，Shulin,et al."Atomic-scale imaging of CH3NH3PbI3 structure and its decomposition pathway".Nature Communications 12.1(2021).