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Coexistence of 3d-ferromagnetism and superconductivity in [(Li(1-x)Fex)OH](Fe(1-y)Liy)Se

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 Added by Dirk Johrendt
 Publication date 2014
  fields Physics
and research's language is English




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Superconducting [(Li(1-x)Fex)OH](Fe(1-y)Liy)Se (x ~ 0.2, y ~ 0.08) was synthesized by hydrothermal methods and structurally characterized by single crystal X-ray diffraction. The crystal structure contains anti-PbO type (Fe(1-y)Liy)Se layers separated by layers of (Li(1-x)Fex)OH. Electrical resistivity and magnetic susceptibility measurements reveal superconductivity at 43 K. An anomaly in the diamagnetic shielding indicates ferromagnetic ordering near 10 K while superconductivity is retained. The ferromagnetism emerges from the iron atoms in the (Li(1-x)Fex)OH layer. Isothermal magnetization measurements confirm the superposition of ferromagnetic with superconducting hysteresis. The internal ferromagnetic field is larger than the lower, but smaller than the upper critical field of the superconductor, which gives evidence for a spontaneous vortex phase where both orders coexist. 57Fe-Mossbauer spectra, 7Li-NMR spectra, and muSR experiments consistently support this rare situation, especially in a bulk material where magnetism emerges from a 3d-element.



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Neutron scattering has played a significant role in characterizing magnetic and structural correlations in Fe$_{1+y}$Te$_{1-x}$Se$_x$ and their connections with superconductivity. Here we review several key aspects of the physics of iron chalcogenide superconductors where neutron studies played a key role. These topics include the phase diagram of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$, where the doping-dependence of structural transitions can be understood from a mapping to the anisotropic random field Ising model. We then discuss orbital-selective Mott physics in the Fe chalcogenide series, where temperature-dependent magnetism in the parent material provided one of the earliest cases for orbital-selective correlation effects in a Hunds metal. Finally, we elaborate on the character of local magnetic correlations revealed by neutron scattering, its dependence on temperature and composition, and the connections to nematicity and superconductivity.
The magnetic properties attributed to the hydroxide layer of Li1-xFex(OH)Fe1-ySe have been elucidated by the study of superconducting and nonsuperconducting members of this family. Both ac magnetometry and muon spin relaxation measurements of nonsuperconductors find a magnetic state existing below approximately 10 K which exhibits slow relaxation of magnetization. This magnetic state is accompanied by a low-temperature heat capacity anomaly present in both superconducting and nonsuperconducting variants suggesting that the magnetism persists into the superconducting state. The estimated value of magnetic moment present within the hydroxide layer supports a picture of a glassy magnetic state, probably comprising clusters of iron ions of varying cluster sizes distributed within the lithium hydroxide layer.
The iron chalcogenide Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ on the Te-rich side is known to exhibit the strongest electron correlations among the Fe-based superconductors, and is non-superconducting for $x$ < 0.1. In order to understand the origin of such behaviors, we have performed ARPES studies of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ ($x$ = 0, 0.1, 0.2, and 0.4). The obtained mass renormalization factors for different energy bands are qualitatively consistent with DFT + DMFT calculations. Our results provide evidence for strong orbital dependence of mass renormalization, and systematic data which help us to resolve inconsistencies with other experimental data. The unusually strong orbital dependence of mass renormalization in Te-rich Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ arises from the dominant contribution to the Fermi surface of the $d_{xy}$ band, which is the most strongly correlated and may contribute to the suppression of superconductivity.
We have performed inelastic neutron scattering measurements on a powder sample of the superconductor lithium iron selenide hydroxide Li$_{1-x}$Fe$_{x}$ODFe$_{1-y}$Se ($x simeq 0.16, y simeq 0.02$, $T_{rm c} = 41$,K). The spectrum shows an enhanced intensity below $T_{rm c}$ over an energy range $0.64times2Delta < E < 2Delta$, where $Delta$ is the superconducting gap, with maxima at the wave vectors $Q_1 simeq 1.46$,AA$^{-1}$ and $Q_2 simeq 1.97$,AA$^{-1}$. The behavior of this feature is consistent with the spin resonance mode found in other unconventional superconductors, and strongly resembles the spin resonance observed in the spectrum of the molecular-intercalated iron selenide, Li$_{0.6}$(ND$_{2}$)$_{0.2}$(ND$_{3}$)$_{0.8}$Fe$_{2}$Se$_{2}$. The signal can be described with a characteristic two-dimensional wave vector $(pi, 0.67pi)$ in the Brillouin zone of the iron square lattice, consistent with the nesting vector between electron Fermi sheets.
The ground state of the parent compounds of many high temperature superconductors is an antiferromagnetically (AFM) ordered phase, where superconductivity emerges when the AFM phase transition is suppressed by doping or application of pressure. This behaviour implies a close relation between the two orders. Understanding the interplay between them promises a better understanding of how the superconducting condensate forms from the AFM ordered background. Here we explore this relation in real space at the atomic scale using low temperature spin-polarized scanning tunneling microscopy (SP-STM) and spectroscopy. We investigate the transition from antiferromagnetically ordered $mathrm{Fe}_{1+y}mathrm{Te}$ via the spin glass phase in $mathrm{Fe}_{1+y}mathrm{Se}_{0.1}mathrm{Te}_{0.9}$ to superconducting $mathrm{Fe}_{1+y}mathrm{Se}_{0.15}mathrm{Te}_{0.85}$. In $mathrm{Fe}_{1+y}mathrm{Se}_{0.1}mathrm{Te}_{0.9}$ we observe an atomic-scale coexistence of superconductivity and short-ranged bicollinear antiferromagnetic order.
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