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Crystal structures of highly hole-doped layered perovskite nickelate Pr$$_{2-x}$$Sr$$_{x}$$NiO$$_{4}$$ studied by neutron diffraction

層状ペロブスカイトニッケル酸化物Pr$$_{2-x}$$Sr$$_{x}$$NiO$$_{4}$$の高ホールドープ領域における結晶構造の中性子回折による研究

梶本 亮一 ; 中島 健次 ; 藤田 全基*; 石角 元志*; 鳥居 周輝*; 石川 喜久*; Miao, P.*; 神山 崇*

Kajimoto, Ryoichi; Nakajima, Kenji; Fujita, Masaki*; Ishikado, Motoyuki*; Torii, Shuki*; Ishikawa, Yoshihisa*; Miao, P.*; Kamiyama, Takashi*

A high-resolution time-of-flight powder neutron diffraction study of the layered nickel oxide Pr$$_{2-x}$$Sr$$_{x}$$NiO$$_{4}$$ with $$x = 0.7$$ and $$0.9$$ was performed to characterize the crystal structures of these highly hole-doped nickelates. For the sample with $$x = 0.7$$, the Ni-O bond lengths decrease uniformly with decreasing temperature, and the atomic displacement parameters are similar to those for $$x = 1/3$$. In contrast, for the sample with $$x = 0.9$$, the out-of-plane Ni-O bond length shows a sharp thermal contraction in the high-temperature region, which is suggestive of changes in the orbital occupation accompanied by the development of checkerboard-type charge correlations. Furthermore, the $$x = 0.9$$ sample is characterized by a large atomic displacement parameter for the apical O atoms along the out-of-plane direction, which is interpreted as the existence of two types of Ni$$^{3+}$$ sites with different orbital occupancies. The distinct difference between the $$x = 0.9$$ sample and the lower-concentration compounds should be related to the development of checkerboard-type charge ordering in the metallic matrix and possible orbital ordering at the Ni$$^{3+}$$ sites at $$x sim 1$$ in the hole-doped layered nickel oxides.

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