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Parallel suppression of superconductivity and Fe moment in the collapsed tetragonal phase of Ca0.67Sr0.33Fe2As2 under pressure

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 Added by Jason Jeffries
 Publication date 2014
  fields Physics
and research's language is English




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Using non-resonant Fe K-beta x-ray emission spectroscopy, we reveal that Sr-doping of CaFe2As2 decouples the Fe moment from the volume collapse transition, yielding a collapsed-tetragonal, paramagnetic normal state out of which superconductivity develops. X-ray diffraction measurements implicate the c-axis lattice parameter as the controlling criterion for the Fe moment, promoting a generic description for the appearance of pressure-induced superconductivity in the alkaline-earth-based 122 ferropnictides (AFe2As2). The evolution of the superconducting critical temperature with pressure lends support to theories for superconductivity involving unconventional pairing mediated by magnetic fluctuations.



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We present high-energy x-ray diffraction data under applied pressures up to p = 29 GPa, neutron diffraction measurements up to p = 1.1 GPa, and electrical resistance measurements up to p = 5.9 GPa, on SrCo2As2. Our x-ray diffraction data demonstrate that there is a first-order transition between the tetragonal (T) and collapsed-tetragonal (cT) phases, with an onset above approximately 6 GPa at T = 7 K. The pressure for the onset of the cT phase and the range of coexistence between the T and cT phases appears to be nearly temperature independent. The compressibility along the a-axis is the same for the T and cT phases whereas, along the c-axis, the cT phase is significantly stiffer, which may be due to the formation of an As-As bond in the cT phase. Our resistivity measurements found no evidence of superconductivity in SrCo2As2 for p <= 5.9 GPa and T >= 1.8 K. The resistivity data also show signatures consistent with a pressure-induced phase transition for p >= 5.5 GPa. Single-crystal neutron diffraction measurements performed up to 1.1 GPa in the T phase found no evidence of stripe-type or A-type antiferromagnetic ordering down to 10 K. Spin-polarized total-energy calculations demonstrate that the cT phase is the stable phase at high pressure with a c/a ratio of 2.54. Furthermore, these calculations indicate that the cT phase of SrCo2As2 should manifest either A-type antiferromagnetic or ferromagnetic order.
Inelastic neutron scattering measurements of CaFe2As2 under applied hydrostatic pressure show that the antiferromagnetic spin fluctuations observed in the ambient pressure, paramagnetic, tetragonal (T) phase are strongly suppressed, if not absent, in the collapsed tetragonal (cT) phase. These results are consistent with a quenched Fe moment in the cT phase and the strong decrease in resistivity observed upon crossing the boundary from the T to cT phase. The suppression or absence of static antiferromagnetic order and dynamic spin fluctuations in the non-superconducting cT phase supports the notion of a coupling between spin fluctuations and superconductivity in the iron arsenides.
The structural properties of EuCo2As2 have been studied up to 35 GPa, through the use of x-ray diffraction in a diamond anvil cell at a synchrotron source. At ambient conditions, EuCo2As2 (I4/mmm) has a tetragonal lattice structure with a bulk modulus of 48 +/-4 GPa. With the application of pressure, the a-axis exhibits negative compressibility with a concurrent sharp decrease in c-axis length. The anomalous compressibility of the a-axis continues until 4.7 GPa, at which point the structure undergoes a second-order phase transition to a collapsed tetragonal (CT) state with a bulk modulus of 111 +/- 2 GPa. We found a strong correlation between the ambient pressure volume of 122 parents of superconductors and the corresponding tetragonal to collapsed tetragonal phase transition pressures
The relationship between antiferromagnetic spin fluctuations and superconductivity has become a central topic of research in studies of superconductivity in the iron pnictides. We present unambiguous evidence of the absence of magnetic fluctuations in the non-superconducting collapsed tetragonal phase of CaFe2As2 via inelastic neutron scattering time-of-flight data, which is consistent with the view that spin fluctuations are a necessary ingredient for unconventional superconductivity in the iron pnictides. We demonstrate that the collapsed tetragonal phase of CaFe2As2 is non-magnetic, and discuss this result in light of recent reports of high-temperature superconductivity in the collapsed tetragonal phase of closely related compounds.
We report the temperature-pressure phase diagram of CaKFe$_4$As$_4$ established using high pressure electrical resistivity, magnetization and high energy x-ray diffraction measurements up to 6 GPa. With increasing pressure, both resistivity and magnetization data show that the bulk superconducting transition of CaKFe$_4$As$_4$ is suppressed and then disappears at $p$ $gtrsim$ 4 GPa. High pressure x-ray data clearly indicate a phase transition to a collapsed tetragonal phase in CaKFe$_4$As$_4$ under pressure that coincides with the abrupt loss of bulk superconductivity near 4 GPa. The x-ray data, combined with resistivity data, indicate that the collapsed tetragonal transition line is essentially vertical, occuring at 4.0(5) GPa for temperatures below 150 K. Band structure calculations also find a sudden transition to a collapsed tetragonal state near 4 GPa, as As-As bonding takes place across the Ca-layer. Bonding across the K-layer only occurs for $p$ $geq$ 12 GPa. These findings demonstrate a new type of collapsed tetragonal phase in CaKFe$_4$As$_4$: a half-collapsed-tetragonal phase.
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