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Anomalous dependence of the c-axis polarized Fe B$_{1g}$ phonon mode with Fe and Se concentrations in Fe$_{1+y}$Te$_{1-x}$Se$_x$

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 Added by Mathieu Le Tacon
 Publication date 2012
  fields Physics
and research's language is English




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We report an investigation of the lattice dynamical properties in a range of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ compounds, with special emphasis on the c-axis polarized vibration of Fe with B$_{1g}$ symmetry, a Raman active mode common to all families of Fe-based superconductors. We have carried out a systematic study of the temperature dependence of this phonon mode as a function of Se $x$ and excess Fe $y$ concentrations. In parent compound Fe$_{1+y}$Te, we observe an unconventional broadening of the phonon between room temperature and magnetic ordering temperature $T_N$. The situation smoothly evolves towards a regular anharmonic behavior as Te is substituted for Se and long range magnetic order is replaced by superconductivity. Irrespective to Se contents, excess Fe is shown to provide an additional damping channel for the B$_{1g}$ phonon at low temperatures. We performed Density Functional Theory (DFT) ab-initio calculations within the local density approximation (LDA) to calcuate the phonon frequencies including magnetic polarization and Fe non-stoichiometry in the Virtual Crystal Approximation (VCA). We obtained a good agreement with the measured phonon frequencies in the Fe-deficient samples, while the effects of Fe excess are poorly reproduced. This may be due to excess Fe-induced local magnetism and low energy magnetic fluctuations that can not be treated accurately within these approaches. As recently revealed by neutron scattering and $mu$-SR studies, these phenomena occur in the temperature range where anomalous decay of the B$_{1g}$ phonon is observed, and suggests a peculiar coupling of this mode with local moments and spin fluctuations in Fe$_{1+y}$Te$_{1-x}$Se$_{x}$.



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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 report the achieving of depairing current limit along $c$-axis in Fe$_{1+y}$Te$_{1-x}$Se$_x$ single crystals. A series of crystals with $T_{rm{c}}$ ranging from 8.6 K to 13.7 K (different amount of excess Fe, $y$) were fabricated into $c$-axis bridges with a square-micrometer cross-section. The critical current density, $J_{rm{c}}$, was directly estimated from the transport current-voltage measurements. The transport $J_{rm{c}}$ reaches a very large value, which is about one order of magnitude larger than the depinning $J_{rm{c}}$, but comparable to the calculated depairing $J_{rm{c}}$ $sim$ 2 $times$ 10$^6$ A/cm$^2$ at 0 K, based on the Ginzburg-Landau (GL) theory. The temperature dependence of the depairing $J_{rm{c}}$ follows the GL-theory ($propto$ (1-$T/T_{rm{c}}$)$^{3/2}$) down to $sim$ 0.83 $T_{rm{c}}$, then increases with a reduced slope at low temperatures, which can be qualitatively described by the Kupriyanov-Lukichev theory. Our study provides a new route to understand the behavior of depairing $J_{rm{c}}$ in iron-based superconductors in a wide temperature range.
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.
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.
We study Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ multi-band superconductor with $T_c=14$K by polarization-resolved Raman spectroscopy. Deep in the superconducting state, we detect pair-breaking excitation at 45cm$^{-1}$ ($2Delta=5.6$meV) in the $XY$($B_{2g}$) scattering geometry, consistent with twice of the superconducting gap energy (3 meV) revealed by ARPES on the hole-like Fermi pocket with $d_{xz}/d_{yz}$ character. We analyze the superconductivity induced phonon self-energy effects for the $B_{1g}$(Fe) phonon and estimate the electron-phonon coupling constant $lambda^Gamma approx 0.026$, which is insufficient to explain superconductivity with $T_c=14$K.
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