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Register a new userEffects of Pnictogen Atmosphere Annealing in Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$
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It has been clarified that bulk superconductivity in Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ can be induced by annealing in an appropriate atmosphere to remove the harmful effects of excess iron. In order to clarify the details of the annealing process, we studied the changes in the physical properties and reaction products of Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ annealed in pnictogen (P, As, Sb) atmospheres. Crystals annealed in a pnictogen atmosphere show bulk superconductivity and the values of $T_{c}$ and $J_{c}$ are about $14~$K and 2-4 $times 10{^5}~$A/cm$^2$ ($2~$K, self-field), respectively. It is also found that the reaction rate increases with the increase in the saturated vapor pressure of the pnictogen. Unexpectedly, the reaction products of Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ after annealing in a P atmosphere mainly consist of FeTe$_2$. In addition, the amount of P required to obtain the optimal $T_{c}$ is much smaller than the amount of excess iron, which is similar to the case of oxygen annealing. P, oxygen, and to some extent As could serve as catalysts to form FeTe$_2$ to remove excess iron.
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Iron chalcogenide Fe(Te,Se) attracted much attention due to its simple structure, which is favorable for probing the superconducting mechanism. Its less toxic nature compared with iron arsenides is also advantageous for applications of iron-based superconductors. By intercalating spacer layers, superconducting transition temperature has been raised over 40 K. On the other hand, the presence of excess Fe is almost unavoidable in Fe(Te,Se) single crystals, which hinders the appearance of bulk superconductivity and causes strong controversies over its fundamental properties. Here we report a systematical study of O$_2$-annealing dynamics in Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ by controlling the amount of O$_2$, annealing temperature, and time. Bulk superconductivity can be gradually induced by increasing the amount of O$_2$ and annealing time at suitable temperatures. The optimally annealed crystals can be easily obtained by annealing with ~ 1.5% molar ratio of oxygen at 400 $^{circ}$C for more than 1 hour. Superconductivity was witnessed to evolve mainly from the edge of the crystal to the central part. After the optimal annealing, the complete removal of excess Fe was demonstrated via STM measurements. Some fundamental properties were recharacterized and compared with those of as-grown crystals to discuss the influence of excess Fe.
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.
We present a study of the Seebeck and Nernst coefficients of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ extended up to 28 T. The large magnitude of the Seebeck coefficient in the optimally doped sample tracks a remarkably low normalized Fermi temperature, which, like other correlated superconductors, is only one order of magnitude larger than T$_c$. We combine our data with other experimentally measured coefficients of the system to extract a set of self-consistent parameters, which identify Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ as a low-density correlated superconductor barely in the clean limit. The system is subject to strong superconducting fluctuations with a sizeable vortex Nernst signal in a wide temperature window.
We report a systematic study of the superconducting (SC) and normal-state anisotropy of Fe$_{1+y}$Te$_{0.6}$Se$_{0.4}$ single crystals with controlled amounts of excess Fe ($y$ = 0, 0.07, and 0.14). The SC state anisotropy $gamma_{H}$ was obtained by measuring the upper critical fields under high magnetic fields over 50 T for both $Hparallel ab$ and $Hparallel c$. On the other hand, the normal state anisotropy $gamma_{rho}$ was obtained by measuring the resistivity with current flowing in the $ab$ plane ($rho_{ab}$) and along the $c$ axis ($rho_c$). To precisely measure $rho_{ab}$ and $rho_c$ in the same part of a specimen avoiding the variation dependent on pieces or parts, we adopt a new method using a micro-fabricated bridge with an additional neck part along $c$ axis. The $gamma_{H}$ decreases from a value dependent on the amount of excess Fe at $T_{rm{c}}$ to a common value $sim$ 1 at 2 K. The different $gamma_{H}$ at $T_{rm{c}}$ ($sim$1.5 for $y$ = 0, and 2.5 for $y$ = 0.14) suggests that the anisotropy of effective mass $m_c^*/m_{ab}^*$ increases from $sim$ 2.25 ($y$ = 0) to 6.25 ($y$ = 0.14) with the excess Fe. The almost isotropic $gamma_{H}$ at low temperatures is due to the strong spin paramagnetic effect at $Hparallel ab$. By contrast, the $gamma_{rho}$ shows a much larger value of $sim$ 17 ($y$ = 0) to $sim$ 50 ($y$ = 0.14) at the temperature just above $T_{rm{c}}$. Combined the results of $gamma_{H}$ and $gamma_{rho}$ near $T_{rm{c}}$, we found out that the discrepant anisotropies between the SC and normal states originates from a large anisotropy of scattering time $tau_{ab}$/$tau_c$ $sim$ 7.8. The $tau_{ab}$/$tau_c$ is found to be independent of the excess Fe.
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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