Predictability as a probe of manifest and latent physics: The case of atomic scale structural, chemical, and polarization behaviors in multiferroic Sm-doped BiFeO3

The predictability of a certain effect or phenomenon is often equated with the knowledge of relevant physical laws, typically understood as a functional or numerically derived relationship between the observations and known states of the system. Correspondingly, observations inconsistent with prior knowledge can be used to derive new knowledge on the nature of the system or indicate the presence of yet unknown mechanisms. Here, we explore the applicability of Gaussian processes (GP) to establish predictability and uncertainty of local behaviors from multimodal observations, providing an alternative to this classical paradigm. Using atomic resolution scanning transmission electron microscopy (STEM) of multiferroic Sm-doped BiFeO3 across a broad composition range, we directly visualize the atomic structure and structural, physical, and chemical order parameter fields for the material. GP regression is used to establish the predictability of the local polarization field from different groups of parameters, including the adjacent polarization values and several combinations of physical and chemical descriptors, including lattice parameters, column intensities, etc. We observe that certain elements of microstructure, including charged and uncharged domain walls and interfaces with the substrate, are best predicted with specific combinations of descriptors, and this predictability and associated uncertainties are consistent across the composition series. The associated generative physical mechanisms are discussed. It is also found that certain parameter combinations tend to predict the orthorhombic phase in the cases where rhombohedral phase is observed, suggesting a potential role of clamping and confinement phenomena in phase equilibrium in Sm-BiFeO3 system close to morphotropic phase boundary. We argue that predictability and uncertainty in observational data offer a new pathway to probe the physics of condensed matter systems from multimodal local observations.

Automated summary

The predictability of certain effects or phenomena is closely related to the understanding of physical laws and the relationship between observations and known states of the system. Inconsistencies in observations can lead to new knowledge about the system. Gaussian processes are explored as an alternative to establish predictability and uncertainty of local behaviors. Different parameter combinations are used to establish predictability of local polarization fields.