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We report charge-transfer up to a single electron per interfacial unit cellacross non-polar heterointerfaces from the Mott insulator LaTiO3 to the chargetransfer insulator LaCoO3. In high-quality bi- and tri-layer systems grownusing pulsed laser deposition, soft X-ray absorption, dichroism and STEM-EELSare used to probe the cobalt 3d-electron count and provide an element-specificinvestigation of the magnetic properties. The experiments prove adeterministically-tunable charge transfer process acting in the LaCoO3 withinthree unit cells of the heterointerface, able to generate full conversion to3d7 divalent Co, which displays a paramagnetic ground state. The number ofLaTiO3 / LaCoO3 interfaces, the thickness of an additional "break" layerbetween the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself intri-layers provide a trio of sensitive control knobs for the charge transferprocess, illustrating the efficacy of O2p-band alignment as a guiding principlefor property design in complex oxide heterointerfaces.

Full control of Co valence in isopolar LaCoO3 / LaTiO3 perovskite heterostructures via interfacial engineering