Controlling the electronic properties via bandstructure engineering is at the heart of modern semiconductor devices. Here, we extend this concept to semimetals where, utilizing LuSb as a model system, we show that quantum confinement lifts carrier compensation and differentially affects the mobility of the electron and hole-like carriers resulting in a strong modification in its large, non-saturating magnetoresistance behavior. Bonding mismatch at the heteroepitaxial interface of a semimetal (LuSb) and a semiconductor (GaSb) leads to the emergence of a novel, two-dimensional, interfacial hole gas and is accompanied by a charge transfer across the interface that provides another avenue to modify the electronic structure and magnetotransport properties in the ultra-thin limit. Our work lays out a general strategy of utilizing confined thin film geometries and heteroepitaxial interfaces to engineer electronic structure in semimetallic systems, which allows control over their magnetoresistance behavior and simultaneously, provides insights into its origin.
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