Cross-correlation based analysis of electron backscatter diffraction (EBSD) patterns and the use of simulated reference patterns has opened up entirely new avenues of insight into local lattice properties within EBSD scans. The benefits of accessing new levels of orientation resolution and multiple types of previously inaccessible data measures are accompanied with new challenges in characterizing microscope geometry and other error previously ignored in EBSD systems. The foremost of these challenges, when using simulated patterns in high resolution EBSD (HR-EBSD), is the determination of pattern center (the location on the sample from which the EBSD pattern originated) with sufficient accuracy to avoid the introduction of phantom lattice rotations and elastic strain into these highly sensitive measures. This dissertation demonstrates how to greatly improve pattern center determination. It also presents a method for the extraction of grain boundary plane information from single two-dimensional surface scans. These are accomplished through the use of previously un-accessed detail within EBSD images, coupled with physical models of the backscattering phenomena. A software algorithm is detailed and applied for the determination of pattern center with an accuracy of ~0.03% of the phosphor screen width, or ~10µm. This resolution makes it possible to apply a simulated pattern method (developed at BYU) in HR-EBSD, with several important benefits over the original HR-EBSD approach developed by Angus Wilkinson. Experimental work is done on epitaxially-grown silicon and germanium in order to gauge the precision of HR-EBSD with simulated reference patterns using the new pattern center calibration approach. It is found that strain resolution with a calibrated pattern center and simulated reference patterns can be as low as 7x10-4. Finally, Monte Carlo-based models of the electron interaction volume are used in conjunction with pattern-mixing-strength curves of line scans crossing grain boundaries in order to recover 3D grain boundary plane information. Validation of the approach is done using 3D serial scan data and coherent twin boundaries in tantalum and copper. The proposed method for recovery of grain boundary plane orientation exhibits an average error of 3 degrees.