No Arabic abstract
The (Li$_{1-x}$Fe$_{x}$OH)FeSe superconductor has been suspected to exhibit long-range magnetic ordering due to Fe substitution in the LiOH layer. However, no direct observation such as magnetic reflection from neutron diffraction has be reported. Here, we use a chemical design strategy to manipulate the doping level of transition metals in the LiOH layer to tune the magnetic properties of the (Li$_{1-x-y}$Fe$_{x}$Mn$_{y}$OD)FeSe system. We find Mn doping exclusively replaces Li in the hydroxide layer resulting in enhanced magnetization in the (Li$_{0.876}$Fe$_{0.062}$Mn$_{0.062}$OD)FeSe superconductor without significantly altering the superconducting behavior as resolved by magnetic susceptibility and electrical/thermal transport measurements. As a result, long-range magnetic ordering was observed below 12 K with neutron diffraction measurements. This work has implications for the design of magnetic superconductors for the fundamental understanding of superconductivity and magnetism in the iron chalcogenide system as well as exploitation as functional materials for next generation devices.
We report the phase diagram for the superconducting system (${^{7}}$Li${_{1-x}}$Fe${_{x}}$OD)FeSe and contrast it with that of (Li${_{1-x}}$Fe${_{x}}$OH)FeSe both in single crystal and powder forms. Samples were prepared via hydrothermal methods and characterized with laboratory and synchrotron X-ray diffraction, high-resolution neutron powder diffraction (NPD), and high intensity NPD. We find a correlation between the tetragonality of the unit cell parameters and the critical temperature, $T_{c}$, which is indicative of the effects of charge doping on the lattice and formation of iron vacancies in the FeSe layer. We observe no appreciable isotope effect on the maximum $T_{c}$ in substituting H by by D. The NPD measurements definitively rule out an antiferromagnetic ordering in the non-superconducting (Li${_{1-x}}$Fe${_{x}}$OD)FeSe samples below 120 K, which has been reported in non-superconducting (Li${_{1-x}}$Fe${_{x}}$OH)FeSe.$^{1}$ A likely explanation for the observed antiferromagnetic transition in (Li${_{1-x}}$Fe${_{x}}$OH)FeSe samples is the formation of impurities during their preparation such as Fe${_{3}}$O${_{4}}$ and LixFeO2, which express a charge ordering transition known as the Verwey transition near 120 K. The concentration of these oxide impurities is found to be dependent on the concentration of the lithium hydroxide reagent and the use of H${_{2}}$O vs. D${_{2}}$O as the solvent during synthesis. We also describe the reaction conditions that lead to some of our superconducting samples to exhibit ferromagnetism below $T_{c}$.
We used angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations to study the electronic structure of Ba(Fe1-x-yCoxMny)2As2 for x=0.06 and 0<=y <=0.07. From ARPES we derive that the substitution of Fe by Mn does not lead to hole doping, indicating a localization of the induced holes. An evaluation of the measured spectral function does not indicate a diverging effective mass or scattering rate near optimal doping. Thus the present ARPES results indicate a continuous evolution of the quasiparticle interaction and therefore question previous quantum critical scenarios.
We develop a local spin model to explain the rich magnetic structures in the iron-based superconductors $Fe_{1+y}Te_{1-x}Se_x$. We show that our model exhibits both commensurate antiferromagnetic and incommensurate magnetic order along the crystal a-axis. The transition from the commensurate to the incommensurate phase is induced when the concentration of excess $Fe$ atoms is larger than a critical value. Experimentally measurable spin-wave features are calculated, and the mean-field phase diagram of the model is obtained. Our model also suggests the existence of a large quantum critical region due to strong spin frustration upon increasing $Se$ concentration.
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.
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.