Origin of Ising magnetism in Ca3Co2O6 unveiled by orbital imaging

Brett Leedahl, Martin Sundermann, Andrea Amorese, Andrea Severing, Hlynur Gretarsson, Lunyong Zhang, Alexander C. Komarek, Antoine Maignan, Maurits W. Haverkort and Liu Hao Tjeng ()
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Brett Leedahl: Max Planck Institute for Chemical Physics of Solids
Martin Sundermann: Max Planck Institute for Chemical Physics of Solids
Andrea Amorese: Max Planck Institute for Chemical Physics of Solids
Andrea Severing: Max Planck Institute for Chemical Physics of Solids
Hlynur Gretarsson: Max Planck Institute for Chemical Physics of Solids
Lunyong Zhang: Max Planck Institute for Chemical Physics of Solids
Alexander C. Komarek: Max Planck Institute for Chemical Physics of Solids
Antoine Maignan: UMR 6508 CNRS-ENSICAEN
Maurits W. Haverkort: Heidelberg University
Liu Hao Tjeng: Max Planck Institute for Chemical Physics of Solids

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract The one-dimensional cobaltate Ca$${}_{3}$$3Co$${}_{2}$$2O$${}_{6}$$6 is an intriguing material having an unconventional magnetic structure, displaying quantum tunneling phenomena in its magnetization. Using a newly developed experimental method, $$s$$s-core-level non-resonant inelastic x-ray scattering ($$s$$s-NIXS), we were able to image the atomic Co $$3d$$3d orbital that is responsible for the Ising magnetism in this system. We can directly observe that corrections to the commonly accepted ideal prismatic trigonal crystal field scheme occur in Ca$${}_{3}$$3Co$${}_{2}$$2O$${}_{6}$$6, and it is the complex $${d}_{2}$$d2 orbital occupied by the sixth electron at the high-spin Co$${}_{\,\text{trig}\,}^{3+}$$trig3+ ($${d}^{6}$$d6) sites that generates the Ising-like behavior. The ability to directly relate the orbital occupation with the local crystal structure is essential to model the magnetic properties of this system.

Date: 2019
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DOI: 10.1038/s41467-019-13273-4

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