Atomic-scale imaging of CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> structure and its decomposition pathway.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 34535678.
- Also identified by DOI 10.1038/s41467-021-25832-9 and PMC identifier 8448763.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
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 CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> (MAPbI<sub>3</sub>) 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<sup>+</sup> followed by the collapse of perovskite structure into 6H-PbI<sub>2</sub> with their critical threshold doses also determined. Interestingly, an intermediate phase (MA<sub>0.5</sub>PbI<sub>3</sub>) 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<sub>3</sub> and HI and leaving hydrocarbons. These findings enhance our understanding of the photoelectric properties and failure mechanism of MAPbI<sub>3</sub>, providing potential strategies into material optimization.