Abstract
Understanding the interplay between crystal engineering and the coupled electronic-ionic charge transport properties of metal halide perovskites remains a critical issue in the field. In this work, we developed an experimental approach to tune the crystallite orientation of methylammonium lead iodide (CH(3)NH(3)PbI(3)) while maintaining their overall crystal structure. This approach allows us to selectively manipulate crystallite orientations to control out-of-plane ion migration and mitigate voltage bias stress effects in CH(3)NH(3)PbI(3) thin films. By employing advanced diffraction and spectroscopic techniques, we achieved a comprehensive characterization of the anisotropic crystallite properties in CH(3)NH(3)PbI(3) thin films with distinct preferred orientations. Our findings reveal that specific crystallite orientations, particularly those that limit halide ion migration pathways along the (200) crystallographic plane, significantly suppress out-of-plane ion migration. This suppression reduces hysteresis and alleviates voltage bias stress effects in CH(3)NH(3)PbI(3) solar cells, ultimately enhancing device stability and performance. These insights not only deepen our understanding of the relationship between crystallite orientation and device functionality but also highlight a promising strategy for regulating ion migration in MHP-based devices. This approach holds significant potential for advancing the stability and efficiency of perovskite solar cells and extending its applicability to other optoelectronic devices.