  In pursuit of rational control of orbital polarization, we present a combined
experimental and theoretical study of single unit cell superlattices of the
correlated metal LaNiO$_3$ and the band insulator LaAlO$_3$. Polarized x-ray
absorption spectra show a distinct asymmetry in the orbital response under
strain. A splitting of orbital energies consistent with octahedral distortions
is found for the case of compressive strain. In sharp contrast, for tensile
strain, no splitting is found although a strong orbital polarization is
present. Density functional theory calculations including a Hubbard U term
reveal that this asymmetry is a result of the interplay of strain and
confinement induces octahedral rotations and distortions and altered covalency
in the bonding across the interfacial Ni-O-Al apical oxygen, leading to a
charge disporportionation at the Ni sites for tensile strain.
