Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides

<p>La<sub><em>x</em></sub>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>6</sub>, La<sub><em>x</em></sub>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>8</sub>, and La<sub>...

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Autores principales: Xu, Z, Jin, L, Backhaus, J-K, Green, F, Hayward, MA
Formato: Journal article
Lenguaje:English
Publicado: American Chemical Society 2021
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author Xu, Z
Jin, L
Backhaus, J-K
Green, F
Hayward, MA
author_facet Xu, Z
Jin, L
Backhaus, J-K
Green, F
Hayward, MA
author_sort Xu, Z
collection OXFORD
description <p>La<sub><em>x</em></sub>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>6</sub>, La<sub><em>x</em></sub>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>8</sub>, and La<sub><em>x</em></sub>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>7</sub>&nbsp;are, respectively, the&nbsp;<em>n</em>&nbsp;= &infin;, 1, and 2 members of the (La<sub><em>x</em>/2</sub>Sr<sub>1&ndash;(<em>x</em>/2)</sub>)<sub><em>n</em></sub>Sr(Ni<sub>0.5</sub>Ru<sub>0.5</sub>)<sub><em>n</em></sub>O<sub>3<em>n</em>+1</sub>&nbsp;compositional series. Reaction with CaH<sub>2</sub>, in the case of the La<em><sub>x</sub></em>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>6</sub>&nbsp;perovskite phases, or Zr oxygen getters in the case of the La<em><sub>x</sub></em>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>8</sub>&nbsp;and La<em><sub>x</sub></em>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>7</sub>&nbsp;Ruddlesden&ndash;Popper phases, yields the corresponding topochemically reduced (La<sub><em>x</em>/2</sub>Sr<sub>1&ndash;(<em>x</em>/2)</sub>)<sub><em>n</em></sub>Sr(Ni<sub>0.5</sub>Ru<sub>0.5</sub>)<sub><em>n</em></sub>O<sub>3<em>n</em>&ndash;1</sub>&nbsp;compounds (La<sub><em>x</em></sub>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>4</sub>, La<sub><em>x</em></sub>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>6</sub>, and La<sub><em>x</em></sub>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>5</sub>), which contain Ni and Ru cations in square-planar coordination sites. The&nbsp;<em>x</em>&nbsp;= 1 members of each series (LaSrNiRuO<sub>4</sub>, LaSr<sub>3</sub>NiRuO<sub>6</sub>, and LaSr<sub>2</sub>NiRuO<sub>5</sub>) exhibit insulating ferromagnetic behavior at low temperature, attributable to exchange couplings between the Ni<sup>1+</sup>&nbsp;and Ru<sup>2+</sup>&nbsp;centers they contain. Increasing the La<sup>3+</sup>&nbsp;concentration (<em>x</em>&nbsp;&gt; 1) leads to a reduction of some of the Ru<sup>2+</sup>&nbsp;centers to Ru<sup>1+</sup>&nbsp;centers and a suppression of the ferromagnetic state (lower&nbsp;<em>T</em><sub>c</sub>, reduced saturated ferromagnet moment). In contrast, increasing the Sr<sup>2+</sup>&nbsp;concentration (<em>x</em>&nbsp;&lt; 1) oxidizes some of the Ru<sup>2+</sup>&nbsp;centers to Ru<sup>3+</sup>&nbsp;centers and enhances the ferromagnetic coupling (increased&nbsp;<em>T</em><sub>c</sub>, increased saturated ferromagnet moment) for the&nbsp;<em>n</em>&nbsp;= &infin; and&nbsp;<em>n</em>&nbsp;= 2 samples but appears to have no influence on the magnetic ordering temperature of the&nbsp;<em>n</em>&nbsp;= 1 samples. The magnetic couplings and influence of doping are discussed on the basis of superexchange and direct exchange couplings between the square-planar Ni and Ru centers.</p>
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spelling oxford-uuid:c0a7e46c-47e4-48f6-815a-93489c00e76f2022-09-13T08:19:59ZHole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxidesJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:c0a7e46c-47e4-48f6-815a-93489c00e76fEnglishSymplectic ElementsAmerican Chemical Society2021Xu, ZJin, LBackhaus, J-KGreen, FHayward, MA<p>La<sub><em>x</em></sub>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>6</sub>, La<sub><em>x</em></sub>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>8</sub>, and La<sub><em>x</em></sub>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>7</sub>&nbsp;are, respectively, the&nbsp;<em>n</em>&nbsp;= &infin;, 1, and 2 members of the (La<sub><em>x</em>/2</sub>Sr<sub>1&ndash;(<em>x</em>/2)</sub>)<sub><em>n</em></sub>Sr(Ni<sub>0.5</sub>Ru<sub>0.5</sub>)<sub><em>n</em></sub>O<sub>3<em>n</em>+1</sub>&nbsp;compositional series. Reaction with CaH<sub>2</sub>, in the case of the La<em><sub>x</sub></em>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>6</sub>&nbsp;perovskite phases, or Zr oxygen getters in the case of the La<em><sub>x</sub></em>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>8</sub>&nbsp;and La<em><sub>x</sub></em>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>7</sub>&nbsp;Ruddlesden&ndash;Popper phases, yields the corresponding topochemically reduced (La<sub><em>x</em>/2</sub>Sr<sub>1&ndash;(<em>x</em>/2)</sub>)<sub><em>n</em></sub>Sr(Ni<sub>0.5</sub>Ru<sub>0.5</sub>)<sub><em>n</em></sub>O<sub>3<em>n</em>&ndash;1</sub>&nbsp;compounds (La<sub><em>x</em></sub>Sr<sub>2&ndash;<em>x</em></sub>NiRuO<sub>4</sub>, La<sub><em>x</em></sub>Sr<sub>4&ndash;<em>x</em></sub>NiRuO<sub>6</sub>, and La<sub><em>x</em></sub>Sr<sub>3&ndash;<em>x</em></sub>NiRuO<sub>5</sub>), which contain Ni and Ru cations in square-planar coordination sites. The&nbsp;<em>x</em>&nbsp;= 1 members of each series (LaSrNiRuO<sub>4</sub>, LaSr<sub>3</sub>NiRuO<sub>6</sub>, and LaSr<sub>2</sub>NiRuO<sub>5</sub>) exhibit insulating ferromagnetic behavior at low temperature, attributable to exchange couplings between the Ni<sup>1+</sup>&nbsp;and Ru<sup>2+</sup>&nbsp;centers they contain. Increasing the La<sup>3+</sup>&nbsp;concentration (<em>x</em>&nbsp;&gt; 1) leads to a reduction of some of the Ru<sup>2+</sup>&nbsp;centers to Ru<sup>1+</sup>&nbsp;centers and a suppression of the ferromagnetic state (lower&nbsp;<em>T</em><sub>c</sub>, reduced saturated ferromagnet moment). In contrast, increasing the Sr<sup>2+</sup>&nbsp;concentration (<em>x</em>&nbsp;&lt; 1) oxidizes some of the Ru<sup>2+</sup>&nbsp;centers to Ru<sup>3+</sup>&nbsp;centers and enhances the ferromagnetic coupling (increased&nbsp;<em>T</em><sub>c</sub>, increased saturated ferromagnet moment) for the&nbsp;<em>n</em>&nbsp;= &infin; and&nbsp;<em>n</em>&nbsp;= 2 samples but appears to have no influence on the magnetic ordering temperature of the&nbsp;<em>n</em>&nbsp;= 1 samples. The magnetic couplings and influence of doping are discussed on the basis of superexchange and direct exchange couplings between the square-planar Ni and Ru centers.</p>
spellingShingle Xu, Z
Jin, L
Backhaus, J-K
Green, F
Hayward, MA
Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title_full Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title_fullStr Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title_full_unstemmed Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title_short Hole and electron doping of topochemically reduced Ni(I)/Ru(II) insulating ferromagnetic oxides
title_sort hole and electron doping of topochemically reduced ni i ru ii insulating ferromagnetic oxides
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AT jinl holeandelectrondopingoftopochemicallyreducedniiruiiinsulatingferromagneticoxides
AT backhausjk holeandelectrondopingoftopochemicallyreducedniiruiiinsulatingferromagneticoxides
AT greenf holeandelectrondopingoftopochemicallyreducedniiruiiinsulatingferromagneticoxides
AT haywardma holeandelectrondopingoftopochemicallyreducedniiruiiinsulatingferromagneticoxides