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Register a new userNon-Thermal Emergence of an Orbital-Selective Mott Phase in FeTe$_{1-x}$Se$_x$
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Electronic correlation is of fundamental importance to high temperature superconductivity. Iron-based superconductors are believed to possess moderate correlation strength, which combined with their multi-orbital nature makes them a fascinating platform for the emergence of exotic phenomena. A particularly striking form is the emergence of an orbital selective Mott phase, where the localization of a subset of orbitals leads to a drastically reconstructed Fermi surface. Here, we report spectroscopic evidence of the reorganization of the Fermi surface from FeSe to FeTe as Se is substituted by Te. We uncover a particularly transparent way to visualize the localization of the $d_{xy}$ electron orbital through the suppression of its hybridization with the more coherent $d$ electron orbitals, which leads to a redistribution of the orbital-dependent spectral weight near the Fermi level. These noteworthy features of the Fermi surface are accompanied by a divergent behavior of a band renormalization in the $d_{xy}$ orbital. All of our observations are further supported by our theoretical calculations to be salient spectroscopic signatures of such a non-thermal evolution from a strongly correlated metallic phase towards an orbital-selective Mott phase in FeTe$_{1-x}$Se$_x$ as Se concentration is reduced.
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It has recently been demonstrated that dynamical magnetic correlations measured by neutron scattering in iron chalcogenides can be described with models of short-range correlations characterized by particular {choices of four-spin plaquettes, where the appropriate choice changes as the} parent material is doped towards superconductivity. Here we apply such models to describe measured maps of magnetic scattering as a function of two-dimensional wave vectors obtained for optimally superconducting crystals of FeTe$_{1-x}$Se$_x$. We show that the characteristic antiferromagnetic wave vector evolves from that of the bicollinear structure found in underdoped chalcogenides (at high temperature) to that associated with the stripe structure of antiferromagnetic iron arsenides (at low temperature); {these can both be described with the same local plaquette, but with different inter-plaquette correlations}. While the magnitude of the low-energy magnetic spectral weight is substantial at all temperatures, it actually weakens somewhat at low temperature, where the charge carriers become more itinerant. The observed change in spin correlations is correlated with the dramatic drop in the electronic scattering rate and the growth of the bulk nematic response on cooling. Finally, we also present powder neutron diffraction results for lattice parameters in FeTe$_{1-x}$Se$_x$ indicating that the tetrahedral bond angle tends to increase towards the ideal value on cooling, in agreement with the increased screening of the crystal field by more itinerant electrons and the correspondingly smaller splitting of the Fe $3d$ orbitals.
We present a systematic study of the nematic fluctuations in the iron chalcogenide superconductor Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ ($0 leq x leq 0.53$) using the elastoresistivity technique. Near $x = 0$, in proximity to the double-stripe magnetic order of Fe$_{1+y}$Te, a diverging $B_{1g}$ nematic susceptibility is observed. Upon increasing $x$, despite the absence of magnetic order, the $B_{2g}$ nematic susceptibility increases and becomes dominant, closely following the strength of the $(pi, pi)$ spin fluctuations. Over a wide range of compositions ($0.17 leq x leq 0.53$), while the $B_{2g}$ nematic susceptibility follows a Curie temperature dependence (with zero Weiss temperature) at low temperatures, it shows deviations from Curie-Weiss behavior for temperatures higher than $50K$. This is the opposite of what is observed in typical iron pnictides, where Curie-Weiss deviations are seen at low temperatures. We attribute this unusual temperature dependence to a loss of coherence of the $d_{xy}$ orbital, which is supported by our theoretical calculations. Our results highlight the importance of orbital differentiation on the nematic properties of iron-based materials.
We have fabricated thin films of FeTe$_{1-x}$Se$_x$ using a scotch-tape method. The superconductivities of the thin films are different from each other although these films were fabricated from the same bulk sample. The result clearly presents the inhomogeneous superconductivity in FeTe$_{1-x}$Se$_x$. The difference comes from inhomogeneity due to the excess Fe concentration. The resistivity of a thin film with low excess Fe shows good superconductivity with the sharp superconducting-transition width and more isotropic 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.
In this work, we study the A$_{x}$Fe$_{2-y}$Se$_2$ (A=K, Rb) superconductors using angle-resolved photoemission spectroscopy. In the low temperature state, we observe an orbital-dependent renormalization for the bands near the Fermi level in which the dxy bands are heavily renormliazed compared to the dxz/dyz bands. Upon increasing temperature to above 150K, the system evolves into a state in which the dxy bands have diminished spectral weight while the dxz/dyz bands remain metallic. Combined with theoretical calculations, our observations can be consistently understood as a temperature induced crossover from a metallic state at low temperature to an orbital-selective Mott phase (OSMP) at high temperatures. Furthermore, the fact that the superconducting state of A$_{x}$Fe$_{2-y}$Se$_2$ is near the boundary of such an OSMP constraints the system to have sufficiently strong on-site Coulomb interactions and Hunds coupling, and hence highlight the non-trivial role of electron correlation in this family of iron superconductors.
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