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Structural phase transition in cobalt oxyfluoride Co$$_{3}$$Sb$$_{4}$$O$$_{6}$$F$$_{6}$$ observed by high-resolution synchrotron and neutron diffraction

Shimono, Seiya*; Ishibashi, Hiroki*; Nagayoshi, Yusuke*; Ikeno, Hidekazu*; Kawaguchi, Shogo*; Hagihara, Masato ; Torii, Shuki*; Kamiyama, Takashi*; Ichihashi, Katsuya*; Nishihara, Sadafumi*; Inoue, Katsuya*; Ishii, Yui*; Kubota, Yoshiki*

The structural phase transition from cubic ($$Ibar{4}3m$$) to a $$c > a$$ tetragonal ($$Ibar{4}$$) at $$T_{rm S}$$ $$sim$$ 180 K was found in non-centrosymmetric oxyfluoride Co$$_{3}$$Sb$$_{4}$$O$$_{6}$$F$$_{6}$$ by high-resolution neutron and synchrotron powder diffraction. To investigate this phase transition, specific heat, magnetization, and dielectric measurements were performed. Although the specific heat and dielectric constant showed anomalies at $$T_{rm S}$$, a phase transition to ferroelectricity was not observed in the polarization hysteresis loop down to 30 K. The rotation of the CoO$$_{2}$$F$$_{4}$$ octahedron was observed at $$T_{rm S}$$ from the structural analysis using synchrotron and neutron powder diffraction data. It was found that the magnetic phase transition from paramagnetic to G-type antiferromagnetic occurred at $$T_{rm N}$$ $$sim$$ 67 K, at which a peak was observed in the specific heat measurements, via magnetic structure analysis using neutron powder diffraction data. The magnetic moments of Co$$^{2+}$$ were aligned along the tetragonal $$c$$-axis direction with a Co$$^{2+}$$ moment of 2.80(1) $$mu_{rm B}$$ at 13 K.



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