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Epitaxial strain imposed in complex oxide thin films by heteroepitaxy isrecognized as a powerful tool for identifying new properties and exploring thevast potential of materials performance. A particular example is LaCoO3, a zerospin, nonmagnetic material in the bulk, whose strong ferromagnetism in a thinfilm remains enigmatic despite a decade of intense research. Here, we usescanning transmission electron microscopy complemented by X-ray and opticalspectroscopy to study LaCoO3 epitaxial thin films under different strainstates. We observed an unconventional strain relaxation behavior resulting instripe-like, lattice modulated patterns, which did not involve uncontrolledmisfit dislocations or other defects. The modulation entails the formation offerromagnetically ordered sheets comprising intermediate or high spin Co3+,thus offering an unambiguous description for the exotic magnetism found inepitaxially strained LaCoO3 films. This observation provides a novel route totailoring the electronic and magnetic properties of functional oxideheterostructures.

Strain-Induced Spin States in Atomically Ordered Cobaltites