Control of electronic properties by lanthanide size and manganese oxidation state in the MnIII/MnIV Ruddlesden–Popper phases Ln2-xSr1+xMn2O7

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Peter D. Battle, Mark A. Green, N. Scott Laskey, Nicholas Kasmir, Julie E. Millburn, Lauren E. Spring, Stuart P. Sullivan, Matthew J. Rosseinsky and Jaap F. Vente


Abstract

The magnetic behaviour of then=2 Ruddlesden–Popper phases Sr2LnMn2O7 is very sensitive to the Ln3+ lanthanide cation. In samples with larger, more basic lanthanide cations (Ln=Nd, Pr) antiferromagnetic phases with ordering temperatures in the region of 130 K co-exist with phases showing a magnetic response suggestive of superparamagnetism or the development of small ferromagnetic clusters at high temperature. The magnetic transition temperature drops to 20 K in samples containing smaller, acidic cations (Ln=Gd–Er, Y). In the latter group of compounds, the transition is from a Curie–Weiss paramagnet to a spin-glass; there is no evidence for long-range magnetic order. This change in behaviour can be explained by considering the variation in the relative strength of superexchange and double exchange interactions as a function of the lanthanide cation. The influence of manganese oxidation state on magnetic response is investigated in the Sr2-xLn1+x Mn2O7 composition range (0.0≤x≤0.7) for Ln=Nd, Tb.


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