Evidence for negative thermal expansion in the superconducting precursor phase SmFeAsO
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The fluorine-doped rare-earth iron oxypnictide series SmFeAsO<sub>1-x</sub>F<sub>x</sub> (0 ≤ x ≤ 0.10) was investigated with high resolution powder x-ray scattering. In agreement with previous studies, the parent compound SmFeAsO exhibits a tetragonal-to-orthorhombic structural distortion at T<sub>S</sub>= 130 K which is rapidly suppressed by x ∼ 0.10 deep within the superconducting dome. The change in unit cell symmetry is followed by a previously unreported magnetoelastic distortion at 120 K. The temperature dependence of the thermal expansion coefficient α<sub>V</sub> reveals a rich phase diagram for SmFeAsO: (i) a global minimum at 125 K corresponds to the opening of a spin-density wave instability as measured by pump-probe femtosecond spectroscopy whilst (ii) a global maximum at 110 K corresponds to magnetic ordering of the Sm and Fe sublattices as measured by magnetic x-ray scattering. At much lower temperatures than T<sub>N</sub>, SmFeAsO exhibits a significant negative thermal expansion on the order of -20 ppm·K<sup>-1</sup> in contrast to the behavior of other rare-earth oxypnictides such as PrFeAsO and the actinide oxypnictide NpFeAsO where the onset of α < 0 only appears in the vicinity of magnetic ordering. Correlating this feature with the temperature and doping dependence of the resistivity and the unit cell parameters, we interpret this result as being due to the condensation of itinerant electrons caused by the opening of a SDW gap, consistent with transport measurements.
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