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Register a new userMagnetic Ordering and Negative Thermal Expansion in PrFeAsO
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We report the structure and magnetism of PrOFeAs, one of the parent phases of the newly discovered Fe-As superconductors, as measured by neutron powder diffraction. In common with other REOFeAs materials, a tetragonal-orthorhombic phase transition is found on cooling below 136 K and striped Fe magnetism with $k =$(1,0,1) is detected below $sim$ 85 K. Our magnetic order parameter measurements show that the ordered Fe moment along the a axis reaches a maximum at $sim$ 40 K, below which an anomalous expansion of the c axis sets in, which results in a negative thermal volume expansion of 0.015 % at 2 K. We propose that this effect, which is suppressed in superconducting samples, is driven by a delicate interplay between Fe and Pr ordered moments.
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A neptunium analogue of the LaFeAsO tetragonal layered compound has been synthesized and characterized by a variety of experimental techniques. The occurrence of long-range magnetic order below a critical temperature T_N = 57 K is suggested by anomalies in the temperature-dependent magnetic susceptibility, electrical resistivity, Hall coefficient, and specific heat curves. Below T_N, powder neutron diffraction measurements reveal an antiferromagnetic structure of the Np sublattice, with an ordered magnetic moment of 1.70(0.07) mu_B aligned along the crystallographic c-axis. No magnetic order has been observed on the Fe sublattice, setting an upper limit of about 0.3 mu_B for the ordered magnetic moment on the iron. High resolution x-ray powder diffraction measurements exclude the occurrence of lattice transformations down to 5 K, in sharp contrast to the observation of a tetragonal-to-orthorhombic distortion in the rare-earth analogues, which has been associated with the stabilization of a spin density wave on the iron sublattice. Instead, a significant expansion of the NpFeAsO lattice parameters is observed with decreasing temperature below T_N, corresponding to a relative volume change of about 0.2% and to an invar behavior between 5 and 20 K. First-principle electronic structure calculations based on the local-spin density plus Coulomb interaction and the local density plus Hubbard-I approximations provide results in good agreement with the experimental findings.
The fluorine-doped rare-earth iron oxypnictide series SmFeAsO$_{1-x}$F$_x$ (0 $leq x leq$ 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$rm{_{S}}$~=~130~K which is rapidly suppressed by $x simeq$ 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 $alpha_{V}$ 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$rm{_{N}}$, SmFeAsO exhibits a significant negative thermal expansion on the order of -40~ppm~$cdot$~K$^{-1}$ in contrast to the behavior of other rare-earth oxypnictides such as PrFeAsO and the actinide oxypnictide NpFeAsO where the onset of $alpha <$ 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 the negative thermal expansion as being indicative of the possible condensation of itinerant electrons accompanying the opening of a SDW gap, consistent with transport measurements.
We use powder neutron diffraction to study the spin and lattice structures of polycrystalline samples of nonsuperconducting PrFeAsO and superconducting PrFeAsO0.85F0.15 and PrFeAsO0.85. We find that PrFeAsO exhibits an abrupt structural phase transitions at 153 K, followed by static long range antiferromagnetic order at 127 K. Both the structural distortion and magnetic order are identical to other rare-earth oxypnictides. Electron-doping the system with either Fluorine or oxygen deficiency suppresses the structural distortion and static long range antiferromagnetic order, therefore placing these materials into the same class of FeAs-based superconductors.
Neutron powder diffraction has been used to investigate the structural and magnetic behavior of the isoelectronically doped Fe pnictide material PrFe1-xRuxAsO. Substitution of Ru for Fe suppresses the structural and magnetic phase transitions that occur in the undoped compound PrFeAsO. Contrary to the behavior usually observed in 1111 pnictide materials, the suppression of both the structural and magnetic transitions does not result in the emergence of superconductivity or any other new ground state. Interestingly, PrFeAsO itself shows an unusual negative thermal expansion (NTE) along the c-axis, from 60K down to at least 4K; this does not occur in superconducting samples such as those formed by doping with fluorine on the oxygen site. We find that NTE is present for all concentrations of PrFe1-xRuxAsO with x ranging from 0.05 to 0.75. These results suggest that the absence of superconductivity in these materials could be related to the presence of NTE.
The thermal expansion at constant pressure of solid CD$_4$ III is calculated for the low temperature region where only the rotational tunneling modes are essential and the effect of phonons and librons can be neglected. It is found that in mK region there is a giant peak of the negative thermal expansion. The height of this peak is comparable or even exceeds the thermal expansion of solid N$_2$, CO, O$_2$ or CH$_4$ in their triple points. It is shown that like in the case of light methane, the effect of pressure is quite unusual: as evidenced from the pressure dependence of the thermodynamic Gr{u}neisen parameter (which is negative and large in the absolute value), solid CD$_4$ becomes increasingly quantum with rising pressure.
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