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Matthew J. Cabral

Publications and source records attributed to Matthew J. Cabral.

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Accounting for Location Measurement Error in Imaging Data with Application to Atomic Resolution Images of Crystalline Materials

Scientists use imaging to identify objects of interest and infer properties of these objects. The locations of these objects are often measured with error, which when ignored leads to biased parameter estimates and inflated variance. Current measurement error methods require an estimate or knowledge of the measurement error variance to correct these estimates, which may not be available. Instead, we create a spatial Bayesian hierarchical model that treats the locations as parameters, it using the image itself to incorporate positional uncertainty. We lower the computational burden by approximating the likelihood using a non-contiguous block design around the object locations. We apply this model in a materials science setting to study the relationship between the chemistry and displacement of hundreds of atom columns in crystal structures directly imaged via scanning transmission electron microscopy. Greater knowledge of this relationship can lead to engineering materials with improved properties of interest. We find strong evidence of a negative relationship between atom column displacement and the intensity of neighboring atom columns, which is related to the local chemistry. A simulation study shows our method corrects the bias in the parameter of interest and drastically improves coverage in high noise scenarios compared to non-measurement error models.

stat.AP

Decoding the complexities of lead-based relaxor ferroelectrics

Relaxor ferroelectrics, which can exhibit exceptional electromechanical coupling are some of the most important functional materials with applications ranging from ultrasound imaging to actuators and sensors in microelectromechanical devices. Since their discovery nearly 60 years ago, the complexity of nanoscale chemical and structural heterogeneity in these systems has made understanding the origins of their unique electromechanical properties a seemingly intractable problem. A full accounting of the mechanisms that connect local structure and chemistry with nanoscale fluctuations in polarization has, however, remained a need and a challenge. Here, we employ aberration-corrected scanning transmission electron microscopy (STEM) to quantify various types of nanoscale heterogeneity and their connection to local polarization in the prototypical relaxor ferroelectric system Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$-PbTiO3 (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. Specifically, these heterogeneities lead to nanoscale domain formation and the relaxor response. We further locate nanoscale regions of monoclinic distortion that correlate directly with Ti content and the electromechanical performance. Through this approach, the elusive connection between chemical heterogeneity, structural heterogeneity and local polarization is revealed, and the results validate models needed to develop the next generation of relaxor ferroelectric materials.

cond-mat.mtrl-sci