Strong orbital polarization in orthorhombicDyMnO3: A combined x-ray linear dichroism andab initioelectronic structure study

We present a combined experimental and theoretical study on the $\text{Mn}\text{ }3d$ orbital occupation in orthorhombic ${\text{DyMnO}}_{3}$ single crystals. We have observed a very strong polarization dependence in the $\text{Mn}\text{ }{L}_{2,3}$ x-ray absorption spectra, indicative for a distinct anisotropic orbital occupation. Ab initio electronic-structure calculations clearly infer the existence of a strong orbital polarization in the ${e}_{g}$ band with a staggered ${d}_{3{x}^{2}\ensuremath{-}{r}^{2}}/{d}_{3{y}^{2}\ensuremath{-}{r}^{2}}$-type ordering pattern in the $ab$ plane. This finding is in excellent agreement with a quantitative analyis of the spectra using the atomic multiplet cluster approach.