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Exploration for multipole order in 5$$d$$-electron systems; X-ray magnetic circular dichroism study of Ba$$_2$$CaOsO$$_6$$

Shibata, Goro ; Hayashi, Hiroaki*; Kawamura, Naomi*; Okamoto, Jun*; Huang, D. J.*; Tanaka, Arata*; Streltsov, S.*; Yamaura, Kazunari*; Fujimori, Atsushi*

The double perovskite-type (DP) oxide Ba$$_2$$CaOsO$$_6$$ with $$(5d)^2$$ electron configuration is one of the candidates for magnetic octupole order. In the present study, we investigated the Os 5$$d$$ electronic structure of Ba$$_2$$CaOsO$$_6$$ polycrystals under magnetic fields via Os $$L_{2,3}$$-edge hard X-ray magnetic circular dichroism (XMCD). In contrast to conventional XMCD spectra of 3$$d$$ and 4$$d$$ electron systems, relatively large ($$sim 1$$%) XMCD signal was observed at the $$L_2$$-edge, whereas it is weak ($$sim 0.1$$%) at the $$L_3$$ edge, suggesting a large orbital magnetic moment due to the strong SOI of Os 5$$d$$ electrons. The overall line shapes of the XAS and XMCD spectra can be simulated by atomic multiplet calculations with cubic symmetry. The calculations show that Coulomb interaction is weak compared to Os 5$$d$$ SOI, suggesting that SOI plays an importance role in the electronic structure of Ba$$_2$$CaOsO$$_6$$.

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