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The crystallographic and magnetic phase diagram of the n=2 layered manganiteLa2-2xSr1+2xMn2O7 in the region x=>0.5 has been studied using temperaturedependent neutron powder diffraction. The magnetic phase diagram reveals aprogression of ordered magnetic structures generally paralleling that of 3-Dperovskites with similar electronic doping: A (0.5<=x<=0.66) --> C(0.75<=x<=0.90) --> G (0.90<=x<=1.0). However, the quasi-2-D structureamplifies this progression to expose features of manganite physics uniquelyaccessible in the layered systems: (a) a "frustrated" region between the A andC regimes where no long-range magnetic order is observed; (b) magneticpolytypism arising from weak inter-bilayer magnetic exchange in the Type-Cregime; and (c) a tetragonal to orthorhombic phase transition whose temperatureevolution directly measures ordering of d3y2-r2 orbitals in the a-b plane. Thisorbital-ordering transition is precursory to Type-C magnetic ordering, whereferromagnetic rods lie parallel to the b-axis. These observations support thenotion that eg orbital polarisation is the driving force behind magnetic spinordering. Finally, in the crossover region between Type-C and Type-G states, wesee some evidence for the development of local Type-C clusters embedded in aType-G framework, directly addressing proposals of similar short-range magneticordering in highly-doped La1-xCaxMnO3 perovskites.Comment: 32 pages, 13 figures, submitted to Phys. Rev.

physical review. b, condensed matter

Interplay of spin and orbital ordering in the layered colossal magnetoresistance manganite<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">La</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn><mml:mi>−</mml:mi><mml:mn>2</mml:mn><mml:mi>x</mml:mi></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">Sr</mml:mi></mml:mrow><mml:mrow><mml:mn>1</mml:mn><mml:mo>+</mml:mo><mml:mn>2</…

Interplay of spin and orbital ordering in the layered colossal magnetoresistance manganiteLa2−2xSr1+2