4.6 Article

Spin frustration and magnetic exchange in cobalt aluminum oxide spinels

Journal

PHYSICAL REVIEW B
Volume 77, Issue 9, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.77.094412

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We report on x-ray diffraction, magnetic susceptibility, electron-spin resonance, and heat-capacity studies of Co[Al1-xCox](2)O-4 for Co concentrations 0 <= x <= 1. In this spinel system only the A-site Co2+ cation is magnetic, while the nonmagnetic B-site Al3+ is substituted by the low-spin nonmagnetic Co3+, and it is possible to investigate the complete phase diagram from Co2+Al23+O4 to Co2+Co23+O4. All samples reveal large negative Curie-Weiss temperatures Theta(CW) of the order of -110 K independent of concentration, which is attributed to a high multiplicity of the superexchange interactions between the A-site Co2+ cations. A pure antiferromagnetic state is found for x=1.0 and 0.9 with Neel temperatures T-N=29.5 and 21.2 K, respectively, as evidenced by lambdalike anomalies in the specific heat. Compositions with 0.3 <= x <= 0.75 show smeared out strongly reduced magnetic ordering temperatures. At low temperatures, a T-2.5 dependence of the specific heat is indicative of a spin-liquid state. For x <= 0.2 a T-2 dependence of the specific heat and a spin-glass-like behavior of the susceptibility below T-f similar to 4.7 K are observed. The high value of the frustration parameter f = vertical bar Theta(CW)vertical bar / T-f > 10 indicates the presence of strong spin frustration at least for x <= 0.6. The frustration mechanism is attributed to competing nearest-neighbor and next-nearest-neighbor superexchange interactions between the A-site Co2+ ions.

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