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Oxygen-defect control has long been considered an influential tuning knob forproducing various property responses in complex oxide films. In addition tophysical property changes, modification to the lattice structure, specificallylattice expansion, with increasing oxygen vacancy concentrations has beenreported often and has become the convention for oxide materials. However, thecurrent understanding of the lattice behavior in oxygen-deficient films becomesdisputable when considering compounds containing different bonding environmentsor atomic layering. Moreover, tensile strain has recently been discovered tostabilize oxygen vacancies in epitaxial films, which further complicates theinterpretation of lattice behavior resulting from their appearance. Here, wereport on the selective strain control of oxygen vacancy formation andresulting lattice responses in the layered, Ruddlesden-Popper phases,La1.85Sr0.15CuO4. We found that a drastically reduced Gibbs free energy foroxygen vacancy formation near the typical growth temperature fortensile-strained epitaxial LSCO accounts for the large oxygennon-stoichiometry. Additionally, oxygen vacancies form preferentially in theequatorial position of the CuO2 plane, leading to a lattice contraction, ratherthan the expected expansion, observed with apical oxygen vacancies. Sinceoxygen stoichiometry plays a key role in determining the physical properties ofmany complex oxides, the strong strain coupling of oxygen nonstoichiometry andthe unusual structural response reported here can provide new perspectives andunderstanding to the structure and property relationships of many otherfunctional oxide materials.

Selective control of oxygen sublattice stability by epitaxial strain in Ruddlesden-Popper films