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The one-dimensional cobaltate Ca3Co2O6 is an intriguing material having anunconventional magnetic structure, displaying quantum tunneling phenomena inits magnetization. Using a newly developed experimental method, s-core-levelnon-resonant inelastic x-ray scattering (s-NIXS), we were able to image theatomic Co 3d orbital that is responsible for the Ising magnetism in thissystem. We show that we can directly observe that it is the complex d2 orbitaloccupied by the sixth electron at the high-spin Co-trig{3+} (d6) sites thatgenerates this behavior. This is extremely rare in the research field oftransition metal compounds, and is only made possible by the delicatelybalanced prismatic trigonal coordination. The ability to directly relate theorbital occupation with the local crystal structure is essential to model themagnetic properties of this system.

Origin of Ising magnetism in Ca3Co2O6 unveiled by orbital imaging