Relaxor ferroelectrics, which can exhibit exceptional electromechanical coupling, are some of the most important functional materials with applications ranging from ultrasound imaging to actuators. Since their discovery, their complexity of nanoscale chemical and structural heterogeneity has made understanding the origins of their electromechanical properties a seemingly intractable problem. Here, we employ aberration-corrected scanning transmission electron microscopy (STEM) to quantify various types of nanoscale heterogeneities and their connection to local polarization in the prototypical relaxor ferroelectric system Pb(Mg 1/3 Nb 2/3)O 3-PbTiO 3 (PMN-PT). We identify three main contributions that each depend on Ti content: chemical order, oxygen octahedral tilt, and oxygen octahedral distortion. These heterogeneities are found to be spatially correlated with low angle polar domain walls, indicating their role in disrupting long-range polarization and leading to nanoscale domain formation and the relaxor response. We further locate nanoscale regions of monoclinic-like distortion that correlate directly with Ti content and electromechanical performance. Through this approach, the connection between chemical heterogeneity, structural heterogeneity and local polariza

Controllable n-type doping over wide ranges of carrier concentrations in AlN, or Al-rich AlGaN, is critical to realizing next-generation applications in high-power electronics and deep UV light sources. Silicon is not a hydrogenic donor in AlN as it is in GaN; despite this, the carrier concentration should be controllable, albeit less efficiently, by increasing the donor concentration during growth. At low doping levels, an increase in the Si content leads to a commensurate increase in free electrons. Problematically, this trend does not persist to higher doping levels. In fact, a further increase in the Si concentration leads to a decrease in free electron concentration; this is commonly referred to as the compensation knee. While the nature of this decrease has been attributed to a variety of compensating defects, the mechanism and identity of the predominant defects associated with the knee have not been conclusively determined. Density functional theory calculations using hybrid exchange-correlation functionals have identified VAl+nSiAl complexes as central to mechanistically understanding compensation in the high Si limit in AlN, while secondary impurities and vacancies tend to dominate compensation in the low Si limit. The formation energies and optical signatures of these defects in AlN are calculated and utilized in a grand canonical charge balance solver to identify carrier concentrations as a function of Si content. The results were found to qualitatively reproduce the experimentally observed compensation knee. Furthermore, these calculations predict a shift in the optical emissions present in the high and low doping limits, which is confirmed with detailed photoluminescence measurements.

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To understand the underlying defect mechanisms governing the coloration of Fe-doped SrTiO3 (Fe:STO), density functional theory calculations were used to determine defect formation energies and to interpret optical absorption spectra. A grand canonical defect equilibrium model was developed using the calculated formation energies, which enabled connection to annealing experiments. It was found that FeTi0 is stable in oxidizing conditions and leads to the optical absorption signatures in oxidized Fe:STO, consistent with experiment. Fe:STO was found to transition from brown to transparent as PO2 was reduced during annealing. The defect equilibrium model reproduces a consistent PO2 of this coloration transition. Most critical to reproducing the PO2 of the coloration transition was inclusion of a FeTi-VO first nearest neighbor complex, which was found to be strongly interacting. The coloration transition PO2 was found to be insensitive to the presence of minority background impurities, slightly sensitive to Fe content, and more sensitive to annealing temperature.