Epitaxial La 0.67 Sr 0.33 MnO 3 ͑LSMO͒ / SrRuO 3 ͑SRO͒ ferromagnetic bilayers have been grown on ͑001͒SrTiO 3 ͑STO͒ substrates by pulsed laser deposition with atomic layer control. We observe a shift in the magnetic hysteresis loop of the LSMO layer in the same direction as the applied biasing field (positive exchange bias). The effect is not present above the Curie temperature of the SRO layer ͑T c SRO ͒, and its magnitude increases rapidly as the temperature is lowered below T c SRO . The direction of the shift is consistent with an antiferromagnetic exchange coupling between the ferromagnetic LSMO layer and the ferromagnetic SRO layer. We propose that atomic layer charge transfer modifies the electronic state at the interface, resulting in the observed antiferromagnetic interfacial exchange coupling. © 2004 American Institute Of Physics. [DOI: 10.1063 Interactions at magnetic interfaces are central to the operation of virtually all magnetic heterostructures. When the interface is between two magnetic materials, the exchange interaction between spins at the interface is dominant, and can dramatically change the magnetic response of the overall heterostructure. Interfacial interactions in bilayers of two ferromagnets can couple the layers so strongly that both switch as a single unit. 1 In a bilayer of two ferromagnets with very different coercive fields, an "exchange spring" effect 2 can result, where the magnetization of the soft layer can reversibly "twist" with respect to the hard layer. The interfacial interaction can also shift the magnetic hysteresis loop so that it is no longer symmetric about zero applied field. This exchange bias effect, most commonly implemented by a ferromagnet/antiferromagnet interface, has been extensively used to pin the magnetization in one of the layers of a magnetic spin valve or tunnel junction.Magnetization loop shifts of a ferromagnetic film arising from interfacial exchange interactions with a "pinning layer" have been observed in many systems, including ones in which the pinning layer is ferromagnetic 3 or ferrimagnetic, 4 as well as antiferromagnetic. 5 Although the details of the interfacial spin arrangements are in some cases believed to be quite complicated, in all cases a preferred direction of the pinning layer is induced by the application of a "bias" magnetic field. In the case of an antiferromagnetic ͑AF͒ pinning layer, the dipole interaction with the applied field is usually small, and the preferred direction is determined by interaction of the AF layer with the ferromagnetic layer. An applied field can directly manipulate the magnetic orientation of ferro-and ferrimagnetic pinning layers through the dipole interaction.These interactions are characterized by the exchange field H E , the shift from zero of the magnetization loop center along the field axis. In almost all cases, this shift of the magnetization loop is opposite to the direction of applied bias field. This case is sometimes referred to as negative exchange bias. This amount of shift is the exchange ...