Influence of oxygen content on the structural, magnetotransport, and magnetic properties of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">LaMnO</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn><mml:mo>+</mml:mo><mml:mi mathvariant="normal">δ</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math>

Abstract

A systematic study of the effect of oxygen content on the structural, magnetotransport, and magnetic properties has been undertaken on a series of ${\mathrm{LaMnO}}_{3+\mathrm{\ensuremath{\delta}}}$ samples, with $\ensuremath{\delta}=0,$ 0.025, 0.07, 0.1, and 0.15. Measurements of the ac initial magnetic susceptibility, magnetization, magnetoresistance, and neutron diffraction, including small-angle neutron scattering (SANS), were performed in the temperature range 1--320 K using high magnetic fields up to 12 T. The antiferromagnetic order found in ${\mathrm{LaMnO}}_{3}$ evolves towards a ferromagnetic order as \ensuremath{\delta} increases. This behavior is accompanied by a drastic reduction of the static Jahn-Teller distortion of the ${\mathrm{MnO}}_{6}$ octahedra. The ferromagnetic coupling weakens for $\ensuremath{\delta}&gt;~0.1.$ The magnetic behavior is interpreted by taking into account two effects caused by the increase in \ensuremath{\delta}: cation vacancies and ${\mathrm{Mn}}^{4+}{/\mathrm{M}\mathrm{n}}^{3+}$ ratio enhancement. The orthorhombic crystallographic structure becomes unstable at room temperature for $\ensuremath{\delta}&gt;~0.1.$ The sample $\ensuremath{\delta}=0.1$ shows a structural transition from rhombohedral to orthorhombic below ${T}_{S}\ensuremath{\approx}300\mathrm{K}$ with a huge change in the cell volume. All the studied compounds were found to be insulating at low temperatures with no appreciable magnetoresistance, except for $\ensuremath{\delta}=0.15,$ in which we observed a large value for the magnetoresistance. The SANS results indicate that magnetic clustering effects are important below ${T}_{C}$ for $\ensuremath{\delta}&gt;~0.07,$ which could explain the intriguing ferromagnetic insulator state. In the $\ensuremath{\delta}=0.07$ and $\ensuremath{\delta}=0.10$ samples we found at temperatures below ${T}_{C}$ magnetic and structural anomalies that are characteristic of charge ordering.