Cyanamide Passivation Enables Robust Elemental Imaging of Metal Halide Perovskites at Atomic Resolution

Abstract

Lead halide perovskites (LHPs) have attracted a tremendous amount of attention because of their applications in solar cells, lighting, and optoelectronics. However, the atomistic principles underlying their decomposition processes remain in large part obscure, likely due to the lack of precise information about their local structures and composition along regions with dimensions on the angstrom scale, such as crystal interfaces. Aberration-corrected scanning transmission electron microscopy combined with X-ray energy dispersive spectroscopy (EDS) is an ideal tool, in principle, for probing such information. However, atomic-resolution EDS has not been achieved for LHPs because of their instability under electron-beam irradiation. We report the fabrication of CsPbBr₃ nanoplates with high beam stability through an interface-assisted regrowth strategy using cyanamide. The ultrahigh stability of the nanoplates primarily stems from two contributions: defect-healing self-assembly/regrowth processes and surface modulation by strong electron-withdrawing cyanamide molecules. The ultrahigh stability of as-prepared CsPbBr₃ nanoplates enabled atomic-resolution EDS elemental mapping, which revealed atomically and elementally resolved details of the LHP nanostructures at an unprecedented level. While improving the stability of LHPs is critical for device applications, this work illustrates how improving the beam stability of LHPs is essential for addressing fundamental questions on structure–property relations in LHPs.