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• W4327720962 abstract "$mathrm{Nd}{}_{2}mathrm{NiO}{}_{4+ensuremath{delta}}$ is a nonstoichiometric oxide, crystallizing in the Ruddlesden-Popper-type framework and exhibiting a wide range of oxygen nonstoichiometry $ensuremath{delta}$ with a complex structural phase diagram. Excess oxygen atoms insert holes, directly influencing the Ni valence state and associated electronic structure. We report here the existence of a correlated incommensurate structural and antiferromagnetic order below $T{}_{N}phantom{rule{4pt}{0ex}}ensuremath{approx}$ 150 K in highly oxygen-doped $mathrm{Nd}{}_{2}mathrm{NiO}{}_{4+ensuremath{delta}}$ with $ensuremath{delta} ensuremath{approx}$ 0.23. The crystal and magnetic structures are investigated by polarized and unpolarized single-crystal neutron diffraction studies together with synchrotron x-ray powder diffraction and macroscopic magnetization measurements. Due to the long-range ordering of excess oxygen atoms, the real structure of the compound is incommensurately modulated, represented by $mathbf{Q}{}_{n}=ifmmodepmelsetextpmfi{}0.813{mathbf{a}}^{*}ifmmodepmelsetextpmfi{}0.519{mathbf{b}}^{*}$ wave vectors. The antiferromagnetic order is characterized by the presence of incommensurate Bragg peaks of type ($hphantom{rule{4pt}{0ex}}ifmmodepmelsetextpmfi{}phantom{rule{4pt}{0ex}}ensuremath{varepsilon}$, 0, $l$/2), with $h$ and $l$ being odd-integer numbers and the magnetic incommensurability $ensuremath{varepsilon}ensuremath{approx}$ 0.36. The in-plane magnetic correlation length is found to be $ensuremath{xi}{}_{ab}$ = 184(1) AA{} but is significantly reduced along the $c$ axis to $ensuremath{xi}{}_{c}$ = 39(2) AA{}, indicating the quasi-two-dimensional nature of the antiferromagnetic correlations. Our study indicates that the excess oxygen atoms nevertheless strongly enhance the magnetic correlations between the ${mathrm{NiO}}_{2}$ planes, resulting in a doubling of the magnetic unit cell along the $c$ axis. In contrast to $mathrm{Nd}{}_{2}mathrm{NiO}{}_{4.1}$, in which the incommensurate periodicity of oxygen and magnetic ordering was found to be identical, the structural and electronic orderings in heavily oxygen-doped ${mathrm{Nd}}_{2}{mathrm{NiO}}_{4.23}$ show two independent modulation vectors. Our study thus unravels a strong correlation between structural and electronic orderings in the highly oxygen-doped $mathrm{Ln}{}_{2}mathrm{NiO}{}_{4+ensuremath{delta}}$ system." @default.
• W4327720962 created "2023-03-18" @default.
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• W4327720962 date "2023-02-21" @default.
• W4327720962 modified "2023-09-25" @default.
• W4327720962 title "Evidence of correlated incommensurate structural and magnetic order in highly oxygen-doped layered nickelate <mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML><mml:msub><mml:mi mathvariant=normal>Nd</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant=normal>NiO</mml:mi><mml:mrow><mml:mn>4.23</mml:mn></mml:mrow></mml:msub></mml:math>" @default.
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• W4327720962 doi "https://doi.org/10.1103/physrevmaterials.7.024412" @default.
• W4327720962 hasPublicationYear "2023" @default.
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