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Interlayer excitons in solid‐state systems have emerged as candidates for realizing novel platforms ranging from excitonic transistors and optical qubits to exciton condensates. Interlayer excitons have been discovered in 2D transition metal dichalcogenides, with large exciton binding energies and the ability to form various van der Waals heterostructures. Here, an oxide system consisting of a single unit cell of Mg₂TiO₄on MgO (001) is proposed as a platform for hosting interlayer excitons. Using a combination of density functional theory (DFT) calculations, molecular beam epitaxy growth, and in situ crystal truncation rod measurements, it is shown that the Mg₂TiO₄‐MgO interface can be precisely controlled to yield an internal electric field suitable for hosting interlayer excitons. The atoms in the polar Mg₂TiO₄layers are observed to be displaced to reduce polarity at the interface with the non‐polar MgO (001) surface. Such polarity‐driven atomic displacements strongly affect electrostatics of the film and the interface, resulting in localization of filled and empty band‐edge states in different layers of the Mg₂TiO₄film. The DFT calculations suggest that the electronic structure is favorable for localization of photoexcited electrons in the bottom layer and holes in the top layer, which may bind to form interlayer exciton states.

Topological crystalline insulators (TCIs) are new materials with metallic surface states protected by crystal symmetry. The properties of molecular beam epitaxy grown SnTe TCI on SrTiO₃(001) are investigated using scanning tunneling microscopy (STM), noncontact atomic force microscopy, low‐energy and reflection high‐energy electron diffraction, X‐ray diffraction, Auger electron spectroscopy, and density functional theory. Initially, SnTe (111) and (001) surfaces are observed; however, the (001) surface dominates with increasing film thickness. The films grow island‐by‐island with the [011] direction of SnTe (001) islands rotated up to 7.5° from SrTiO₃[010]. Microscopy reveals that this growth mechanism induces defects on different length scales and dimensions that affect the electronic properties, including point defects (0D); step edges (1D); grain boundaries between islands rotated up to several degrees; edge‐dislocation arrays (2D out‐of‐plane) that serve as periodic nucleation sites for pit growth (2D in‐plane); and screw dislocations (3D). These features cause variations in the surface electronic structure that appear in STM images as standing wave patterns and a nonuniform background superimposed on atomic features. The results indicate that both the growth process and the scanning probe tip can be used to induce symmetry breaking defects that may disrupt the topological states in a controlled way.