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We have performed non-resonant x-ray diffraction, resonant soft and hardx-ray magnetic diffraction, soft x-ray absorption and x-ray magnetic circulardichroism measurements to clarify the electronic and magnetic states of theCo3+ ions in GdBaCo2O5.5. Our data are consistent with a 3+ Py Co HS state atthe pyramidal sites and a 3+ Oc Co LS state at the octahedral sites. Thestructural distortion, with a doubling of the a axis (2ap x 2ap x 2ap cell),shows alternating elongations and contractions of the pyramids and indicatesthat the metal-insulator transition is associated with orbital order in the t2gorbitals of the 3+ Py Co HS state. This distortion corresponds to analternating ordering of xz and yz orbitals along the a and c axes for the 3+ PyCo . The orbital ordering and pyramidal distortion lead to deformation of theoctahedra, but the 3+ Oc Co LS state does not allow an orbital order to occurfor the 3+ Oc Co ions. The soft x-ray magnetic diffraction results indicatethat the magnetic moments are aligned in the ab plane but are not parallel tothe crystallographic a or b axes. The orbital order and the doubling of themagnetic unit cell along the c axis support a non-collinear magnetic structure.The x-ray magnetic circular dichroism data indicate that there is a largeorbital magnetic contribution to the total ordered Co moment.

Magnetic and electronic Co states in layered cobaltate GdBaCo2O5.5-x