Real‐Space Tilting Method for Atomic Resolution STEM Imaging of Nanocrystalline Materials

Abstract Atomic‐resolution scanning transmission electron microscopy (STEM) characterization requires precise tilting of the specimen to a high symmetric zone axis, which is usually processed in reciprocal space by following the diffraction patterns. However, for small‐sized nanocrystalline materials, their diffraction patterns are often too faint to guide the tilting process. Here, a simple and effective tilting method is developed based on the diffraction contrast change of the shadow image in the Ronchigram. The misorientation angle of the specimen can be calculated and tilted to the zone axis based on the position of the shadow image with lowest intensity. This method requires no prior knowledge of the sample and the maximum misorientation angle that can be corrected is >±6.9° with sub‐mrad accuracy. It operates in real space, without recording the diffraction patterns of the specimens, making it particularly effective for nanocrystalline materials. Combined with the scripting to control the microscope, the sample can be automatically tilted to the zone axis under low dose conditions (<0.17 e − Å − 2 s −1 ), facilitating the imaging of beam sensitive materials such as zeolites or metal‐organic frameworks. This automated tilting method can significantly contribute to the atomic‐scale characterization of the nanocrystalline materials by STEM imaging.