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Spin and orbital disordering by hole doping in Pr1-xCaxVO3

Reehuis, M.
•
Ulrich, C.
•
Abdala, P. M.
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2016
Physical Review B

High-resolution powder x-ray diffraction and single-crystal neutron diffraction were used to investigate the crystal structure and magnetic ordering of the compound Pr1-xCax VO3 (0 <= x <= 0.3), which undergoes an insulator-to-metal transition for x similar to 0.23. Since the ionic radii of Pr3+ and Ca2+ are almost identical and structural disorder is minimal, Pr1-xCaxVO3 is a good model system for the influence of hole doping on the spin and orbital correlations in transition metal oxides. The end member PrVO3 is a Mott-Hubbard insulator, which exhibits a structural phase transition at T-S = 180 K from an orthorhombic to a monoclinic structure with space groups Pbnm and P2(1)/b, respectively. This transition is associated with the onset of orbital ordering and strong Jahn-Teller distortions of the VO6 octahedra. Antiferromagnetic C-type order with vanadium moments oriented in the ab plane is observed below T-N = 140 K. Upon cooling, the vanadium moments induce a progressive magnetic polarization of the praseodymium sublattice, resulting in a ferrimagnetic structure with coexisting modes (C-x, F-y) and (F-x, C-y). In the insulating range of the Pr1-xCaxVO3 phase diagram, Ca doping reduces both the orbital and magnetic transition temperatures so that T-S = 108 K and T-N = 95 K for x = 0.20. The Jahn-Teller distortions and ordered vanadium moments also decrease upon doping. In a metallic sample with x = 0.30, Jahn-Teller distortions and long-range orbital ordering are no longer observable, and the average crystal structure remains orthorhombic down to low temperature. However, broadening of some lattice Bragg reflections indicate a significant increase in lattice strain. Antiferromagnetic short-range order with a weak ordered moment of 0.14(3) mu(B) per vanadium atom could still be observed on the vanadium site below T similar to 60 K. We discuss these observations in terms of doping-induced spin-orbital polaron formation.

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PhysRevB.94.104436.pdf

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