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First-order magnetic and structural phase transitions in Fe$_{1+y}$Se$_x$Te$_{1-x}$

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 Added by Shiliang Li
 Publication date 2008
  fields Physics
and research's language is English




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We use bulk magnetic susceptibility, electronic specific heat, and neutron scattering to study structural and magnetic phase transitions in Fe$_{1+y}$Se% $_x$Te$_{1-x}$. Fe$_{1.068}$Te exhibits a first order phase transition near 67 K with a tetragonal to monoclinic structural transition and simultaneously develops a collinear antiferromagnetic (AF) order responsible for the entropy change across the transition. Systematic studies of FeSe$%_{1-x}$Te$_x$ system reveal that the AF structure and lattice distortion in these materials are different from those of FeAs-based pnictides. These results call into question the conclusions of present density functional calculations, where FeSe$_{1-x}$Te$_x$ and FeAs-based pnictides are expected to have similar Fermi surfaces and therefore the same spin-density-wave AF order.



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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.
Single crystals of Fe(1+x)Te(1-y)Se(y) have been grown with a controlled Fe excess and Se doping, and the crystal structure has been refined for various compositions. The systematic investigation of magnetic and superconducting properties as a function of the structural parameters shows how the material can be driven into various ground states, depending on doping and the structural modifications. Our results prove that the occupation of the additional Fe site, Fe2, enhances the spin localization. By reducing the excess Fe, the antiferromagnetic ordering is weakened, and the superconducting ground state is favored. We have found that both Fe excess and Se doping in synergy determine the properties of the material and an improved 3-dimensional phase diagram is proposed.
Using angle-resolved photoemission spectroscopy we have studied the low-energy electronic structure and the Fermi surface topology of Fe$_{1+y}$Te$_{1-x}$Se$_x$ superconductors. Similar to the known iron pnictides we observe hole pockets at the center and electron pockets at the corner of the Brillouin zone (BZ). However, on a finer level, the electronic structure around the $Gamma$- and $Z$-points in $k$-space is substantially different from other iron pnictides, in that we observe two hole pockets at the $Gamma$-point, and more interestingly only one hole pocket is seen at the $Z$-point, whereas in $1111$-, $111$-, and $122$-type compounds, three hole pockets could be readily found at the zone center. Another major difference noted in the Fe$_{1+y}$Te$_{1-x}$Se$_x$ superconductors is that the top of innermost hole-like band moves away from the Fermi level to higher binding energy on going from $Gamma$ to $Z$, quite opposite to the iron pnictides. The polarization dependence of the observed features was used to aid the attribution of the orbital character of the observed bands. Photon energy dependent measurements suggest a weak $k_z$ dispersion for the outer hole pocket and a moderate $k_z$ dispersion for the inner hole pocket. By evaluating the momentum and energy dependent spectral widths, the single-particle self-energy was extracted and interestingly this shows a pronounced non-Fermi liquid behaviour for these compounds. The experimental observations are discussed in context of electronic band structure calculations and models for the self-energy such as the spin-fermion model and the marginal-Fermi liquid.
Superconductivity (SC) with the suppression of long-range antiferromagnetic (AFM) order is observed in the parent compounds of both iron-based and cuprate superconductors. The AFM wave vectors are bicollinear ($pi$, 0) in the parent compound FeTe different from the collinear AFM order ($pi$, $pi$) in most iron pnictides. Study of the phase diagram of Fe$_{1+y}$Te$_{1-x}$Se$_x$ is the most direct way to investigate the competition between bicollinear AFM and SC. However, presence of interstitial Fe affects both magnetism and SC of Fe$_{1+y}$Te$_{1-x}$Se$_x$, which hinders the establishment of the real phase diagram. Here, we report the comparison of doping-temperature ($x$-$T$) phase diagrams for Fe$_{1+y}$Te$_{1-x}$Se$_x$ (0 $leq$ $x$ $leq$ 0.43) single crystals before and after removing interstitial Fe. Without interstitial Fe, the AFM state survives only for $x$ $<$ 0.05, and bulk SC emerges from $x$ = 0.05, and does not coexist with the AFM state. The previously reported spin glass state, and the coexistence of AFM and SC may be originated from the effect of the interstitial Fe. The phase diagram of Fe$_{1+y}$Te$_{1-x}$Se$_x$ is found to be similar to the case of the 1111 system such as LaFeAsO$_{1-x}$F$_x$, and is different from that of the 122 system.
The idea of employing non-Abelian statistics for error-free quantum computing ignited interest in recent reports of topological surface superconductivity and Majorana zero modes (MZMs) in FeTe$_{0.55}$Se$_{0.45}$. An associated puzzle is that the topological features and superconducting properties are not observed uniformly across the sample surface. Understanding and practical control of these electronic inhomogeneities present a prominent challenge for potential applications. Here, we combine neutron scattering, scanning angle-resolved photoemission spectroscopy (ARPES), and microprobe composition and resistivity measurements to characterize the electronic state of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$. We establish a phase diagram in which the superconductivity is observed only at sufficiently low Fe concentration, in association with distinct antiferromagnetic correlations, while the coexisting topological surface state occurs only at sufficiently high Te concentration. We find that FeTe$_{0.55}$Se$_{0.45}$ is located very close to both phase boundaries, which explains the inhomogeneity of superconducting and topological states. Our results demonstrate the compositional control required for use of topological MZMs in practical applications.
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