We report charge-transfer up to a single electron per interfacial unit cell across non-polar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and tri-layer systems grown using pulsed laser deposition, soft X-ray absorption, dichroism and STEM-EELS are used to probe the cobalt 3d-electron count and provide an element-specific investigation of the magnetic properties. The experiments prove a deterministically-tunable charge transfer process acting in the LaCoO3 within three unit cells of the heterointerface, able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3 / LaCoO3 interfaces, the thickness of an additional break layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in tri-layers provide a trio of sensitive control knobs for the charge transfer process, illustrating the efficacy of O2p-band alignment as a guiding principle for property design in complex oxide heterointerfaces.
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