Magnetic properties and interfacial phenomena of epitaxial perovskite oxides depend sensitively on parameters such as film thickness and strain state. In this work, epitaxial La0.67Sr0.33CoO3 (LSCO)/La0.67Sr0.33MnO3 (LSMO) bilayers were grown on NdGaO3 (NGO) and LaAlO3 (LAO) substrates with a fixed LSMO thickness of 6 nm, and LSCO thickness (tLSCO) varying from 2 to 10 nm. Soft x-ray magnetic spectroscopy revealed that magnetically active Co2+ ions that strongly coupled to the LSMO layer were observed below a critical tLSCO for bilayers grown on both substrates. On LAO substrates, this critical thickness was 2 nm, above which the formation of Co2+ ions was quickly suppressed leaving only a soft LSCO layer with mixed valence Co3+/Co4+ ions. The magnetic properties of both LSCO and LSMO layers displayed strong tLSCO dependence. This critical tLSCO increased to 4 nm on NGO substrates, and the magnetic properties of only the LSCO layer displayed tLSCO dependence. A non-magnetic layer characterized by Co3+ ions and with a thickness below 2 nm exists at the LSCO/substrate interface for both substrates. The results contribute to the understanding of interfacial exchange spring behavior needed for applications in next generation spintronic and magnetic memory devices.

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