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We combine state-of-the-art oxide epitaxial growth by hybrid molecular beam epitaxy with transport, x-ray photoemission, and surface diffraction, along with classical and first-principles quantum mechanical modeling to investigate the nuances of insulating layer formation in otherwise high-mobility homoepitaxial n-SrTiO 3 (001) films. Our analysis points to charge immobilization at the buried n-SrTiO 3 /undoped SrTiO 3 (001) interface as well as within the surface contamination layer resulting from air exposure as the drivers of electronic dead-layer formation. As Fermi level equilibration occurs at the surface and the buried interface, charge trapping reduces the sheet carrier density ( n 2 D ) and renders the n-STO film insulating if n 2 D falls below the critical value for the metal-to-insulator transition. 

We report charge transfer and built-in electric fields across the epitaxial SrNbxTi1−xO3−δ=Sið001Þ interface. Electrical transport measurements indicate the formation of a hole gas in the Si and the presence of built-in fields. Hard x-ray photoelectron measurements reveal pronounced asymmetries in core-level spectra that arise from these built-in fields. Theoretical analysis of core-level spectra enables built-in fields and the resulting band bending to be spatially mapped across the heterojunction. The demonstration of tunable charge transfer, built-in fields, and the spatial mapping of the latter, lays the groundwork for the development of electrically coupled, functional heterojunctions. 

Complex oxides and semiconductors exhibit distinct yet complementary properties owing to their respective ionic and covalent natures. By electrically coupling oxides to semiconductors within epitaxial heterostructures, enhanced or novel functionalities beyond those of the constituent materials can potentially be realized. Key to electrically coupling oxides to semiconductors is controlling the physical and electronic structure of semiconductor – crystalline oxide heterostructures. Here we discuss how composition of the oxide can be manipulated to control physical and electronic structure in Ba1-xSrxTiO3/ Ge and SrZrxTi1-xO3/Ge heterostructures. In the case of the former we discuss how strain can be engineered through composition to enable the re-orientable ferroelectric polarization to be coupled to carriers in the semiconductor. In the case of the latter we discuss how composition can be exploited to control the band offset at the semiconductor - oxide interface. The ability to control the band offset, i.e. band-gap engineering, provides a pathway to electrically couple crystalline oxides to semiconductors to realize a host of functionalities.