Orientation mapping via dictionary indexing of AC-STEM Kikuchi patterns using open-source software

The properties of polycrystalline materials are strongly influenced by the spatial arrangement and orientations of individual grains within the microstructure, making nanoscale characterization of grain orientation essential. This is also often the case for small grains in the nm regime explored using scanning transmission electron microscopy (STEM). Automated crystal orientation mapping (ACOM) is traditionally performed using spot-like diffraction patterns. In contrast, orientation mapping based on transmission Kikuchi diffraction (TKD) using an aberration-corrected (AC) convergent STEM probe remains relatively underexplored, despite its superior orientation sensitivity and higher spatial resolution. In this work, we present an open-source software-based template-matching approach for orientation mapping using AC-STEM TKD. A master pattern (a simulated angular distribution of Kikuchi band intensities on the unit sphere) is first generated through a dynamical simulation implemented in open-source software. This resulting pattern is subsequently imported into another open-source package for geometric simulations and orientation indexing. We demonstrate the capability of the proposed method by applying it to orientation mapping in BaZr_0.4Ce_0.4Y_0.1Yb_0.1O_3-δ (BZCYYb4411) fuel-cell material and LiNiO₂ (LNO) lithium-ion battery cathode material. The best-matched simulated patterns exhibit strong agreement with experimental data, even under the challenging conditions with limited diffraction space available for matching.