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Register a new userMagnetic hour-glass dispersion and its relation to high-temperature superconductivity in iron-tuned Fe$_{1+y}$Te$_{0.7}$Se$_{0.3}$
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High-temperature superconductivity remains arguably the largest outstanding enigma of condensed matter physics. The discovery of iron-based high-temperature superconductors has renewed the importance of understanding superconductivity in materials susceptible to magnetic order and fluctuations. Intriguingly they show magnetic fluctuations reminiscent of the superconducting (SC) cuprates, including a resonance and an hour-glass shaped dispersion, which provide an opportunity to new insight to the coupling between spin fluctuations and superconductivity. Here we report inelastic neutron scattering data on Fe$_{1+y}$Te$_{0.7}$Se$_{0.3}$ using excess iron concentration to tune between a SC ($y=0.02$) and a non-SC ($y=0.05$) ground states. We find incommensurate spectra in both samples but discover that in the one that becomes SC, a constriction towards a commensurate hourglass shape develop well above $T_c$. Conversely a spin-gap and concomitant spectral weight shift happen below $T_c$. Our results imply that the hourglass shaped dispersion is most likely a pre-requisite for superconductivity, whereas the spin-gap and shift of spectral weight are consequences of superconductivity. We explain this observation by pointing out that an inwards dispersion towards the commensurate wave-vector is needed for the opening of a spin gap to lower the magnetic exchange energy and hence provide the necessary condensation energy for the SC state to emerge.
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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.
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 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 compare the superconducting phase-diagram under high magnetic fields (up to $H = 45$ T) of Fe$_{1+y}$Se$_{0.4}$Te$_{0.6}$ single crystals originally grown by the Bridgman-Stockbarger (BRST) technique, which were annealed to display narrow superconducting transitions and the optimal transition temperature $T_c gtrsim 14$ K, with the diagram for samples of similar stoichiometry grown by the traveling-solvent floating-zone technique as well as with the phase-diagram reported for crystals grown by a self-flux method. We find that the so-annealed samples tend to display higher ratios $H_{c2}/T_c$, particularly for fields applied along the inter-planar direction, where the upper critical field $H_{c2}(T)$ exhibits a pronounced downward curvature followed by saturation at lower temperatures $T$. This last observation is consistent with previous studies indicating that this system is Pauli limited. An analysis of our $H_{c2}(T)$ data using a multiband theory suggests the emergence of the Farrel-Fulde-Larkin-Ovchnikov state at low temperatures. A detailed structural x-ray analysis, reveals no impurity phases but an appreciable degree of mosaicity in as-grown BRST single-crystals which remains unaffected by the annealing process. Energy-dispersive x-ray analysis showed that the annealed samples have a more homogeneous stoichiometric distribution of both Fe and Se with virtually the same content of interstitial Fe as the non-annealed ones. Thus, we conclude that stoichiometric disorder, in contrast to structural disorder, is detrimental to the superconducting phase diagram of this series under high magnetic fields. Finally, a scaling analysis of the fluctuation conductivity in the superconducting critical regime, suggests that the superconducting fluctuations have a two-dimensional character in this system.
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.
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