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We investigate the effect of strain and film thickness on the orbital andmagnetic properties of LaSrCrO$_3$ (LSCO)/LaSrMnO$_3$ (LSMO) heterostructuresusing bulk magnetometry, soft X-ray magnetic spectroscopy, first-principlesdensity functional theory, high-resolution electron microscopy and X-raydiffraction. We observe an anti-parallel ordering of the magnetic momentsbetween the ferromagnetic LSMO layers and the LSCO spacers leading to astrain-independent ferromagnetic ground state of the LSCO/LSMO heterostructuresfor LSMO layers as thin as 2 unit cells. As the LSMO thickness is increased, anet ferromagnetic state is maintained, however, the average magnetic moment perMn is found to be dependent on the magnitude of the substrate-induced strain.The differences in the magnetic responses are related to preferentialoccupation of the Mn $x^2-y^2$ (in-plane) d-orbitals for tensile strain and$3z^2-r^2$ (out-of-plane) orbitals under compressive strain leading tocompeting ferromagnetic and anti-ferromagnetic exchange interactions within theLSMO layers. These results underscore the relative contributions of orbital,structural and spin degree of freedom and their tunability in atomically-thincrystalline complex oxide layers.

Effect of strain on magnetic and orbital ordering of LaSrCrO$_3$/LaSrMnO$_3$ heterostructures