By band engineering the iron chalcogenide Fe(Se,Te) via ab-initio calculations, we search for topological surface states and realizations of Majorana bound states. Proposed topological states are expected to occur for non-stoichiometric compositions on a surface Dirac cone where issues like disorder scattering and charge transfer between relevant electronic states have to be addressed. However, this surface Dirac cone is well above the Fermi-level. Our goal is to theoretically design a substituted crystal in which the surface Dirac cone is shifted towards the Fermi-level by modifying the bulk material without disturbing the surface. Going beyond conventional density functional theory (DFT), we apply the coherent potential approximation (BEB-CPA) in a mixed basis pseudo-potential framework to scan the substitutional phase-space of co-substitutions on the Se-sites. We have identified iodine as a promising candidate for intrinsic doping. Our specific proposal is that FeSe$_{0.325}$I$_{0.175}$Te$_{0.5}$ is a very likely candidate to exhibit a Dirac cone right at the Fermi energy without inducing strong disorder scattering.
Our searches for new oxide chalcogenides of rare earths and Fe, Co, Ni, and Zn resulted in preparation of two new compounds Ce2Fe2O3S2 and Pr2Fe2O3S2 which are isostructural to La2Fe2O3Se2 and Sm2Ti2O3Sb2. Crystal structures of the new compounds Ce2Fe2O3S2 and Pr2Fe2O3S2 were determined from powder X-ray diffraction data. Magnetic measurements were performed for Ce2Fe2O3S2 and revealed behavior very similar to that of isostructural oxide chalcogenides of iron and pnictides of titanium. In particular, no superconductivity was observed down to 4 K. Crystal chemical factors determining the stabil…
The interplay between superconductivity, magnetism and crystal structure in iron-based superconductors is a topic of great interest amongst the condensed matter physics community as it is thought to be the key to understanding the mechanisms responsible for high temperature superconductivity. Alkali metal doped iron chalcogenide superconductors exhibit several unique characteristics which are not found in other iron-based superconducting materials such as antiferromagnetic ordering at room temperature, the presence of ordered iron vacancies and high resistivity normal state properties. Detaile…
Using density-functional theory, we calculate the electronic bandstructure of single-layer graphene on top of hexagonal In_2Te_2 monolayers. The geometric configuration with In and Te atoms at centers of carbon hexagons leads to a Kekule' texture with an ensuing bandgap of 20 meV. The alternative structure, nearly degenerate in energy, with the In and Te atoms on top of carbon sites is characterized instead by gapless spectrum with the original Dirac cones of graphene reshaped, depending on the graphene-indium chalcogenide distance, either in the form of an undoubled pseudo-spin one Dirac cone…
We perform realistic first-principles calculations of iron chalcogenides and ruthenate based materials to identify experimental signatures of Hund's coupling induced correlations in these systems. We find that FeTe and K$_x$Fe$_{2-y}$Se$_2$ display unusual orbital dependent fractional powerlaw behavior in their quasiparticle self energy and optical conductivity, a phenomena first identified in SrRuO$_3$. Strong incoherence in the paramagnetic state of these materials results in electronic states hidden to angle-resolved photoemission spectroscopy which reemerge at low temperatures. We identify…
The iron pnictide and chalcogenide compounds are a subject of intensive investigations due to their high temperature superconductivity.\cite{a-LaFeAsO} They all share the same structure, but there is significant variation in their physical properties, such as magnetic ordered moments, effective masses, superconducting gaps and T$_c$. Many theoretical techniques have been applied to individual compounds but no consistent description of the trends is available \cite{np-review}. We carry out a comparative theoretical study of a large number of iron-based compounds in both their magnetic and param…
We report the growth and characterization of single crystals of iron chalcogenide superconductor FeCr$_{0.02}$Se. There is an enhancement of the superconducting transition temperature (T$_{\rm c}$) as compared to the T$_{\rm c}$ of the single crystals of the parent compound Fe$_{1+x}$Se by about 25%. The superconducting parameters such as the critical fields, coherence length, penetration depth and the Ginzburg-Landau parameter have been estimated for these single crystals. Analysis of the critical current data suggests a fluctuation in electronic mean free path induced ($δl$) pinning mechanis…
We calculate the strength of the frequency-dependent on-site electronic interactions in the iron pnictides LaFeAsO, BaFe2As2, BaRu2As2, and LiFeAs and the chalcogenide FeSe from first principles within the constrained random phase approximation. We discuss the accuracy of an atomic-like parametrization of the two-index density-density interaction matrices based on the calculation of an optimal set of three independent Slater integrals, assuming that the angular part of the Fe-d localized orbitals can be described within spherical harmonics as for isolated Fe atoms. We show that its quality dep…
The ground state of K$_{0.8+x}$Fe$_{1.6+y}$Se$_2$ and other iron-based selenide superconductors are doped antiferromagnetic semiconductors. There are well defined iron local moments whose energies are separated from those of conduction electrons by a large band gap in these materials. We propose that the low energy physics of this system is governed by a model Hamiltonian of interacting electrons with on-site ferromagnetic exchange interactions and inter-site superexchange interactions. We have derived the effective pairing potential of electrons under the linear spin-wave approximation and sh…
We show that electron correlations lead to a bad metallic state in chalcogenides FeSe and FeTe despite the intermediate value of the Hubbard repulsion $U$ and Hund's rule coupling $J$. The evolution of the quasi particle weight $Z$ as a function of the interaction terms reveals a clear crossover at $U \simeq$ 2.5 eV. In the weak coupling limit $Z$ decreases for all correlated $d$ orbitals as a function of $U$ and beyond the crossover coupling they become weakly dependent on $U$ while strongly depend on $J$. A marked orbital dependence of the $Z$'s emerges even if in general the orbital-selecti…
We have investigated several classes of strong spin-orbit chalcogenides related to the (Pb,Sn)Te series studied in connection with the Dirac fermion physics in the 1980s. Our first-principle theoretical calculations suggest that ternary chalcogenides TlBiX$_2$ and TlSbX$_2$ (X=Te, Se, S) series harbor small bandgap topological insulators with single Dirac cone on some selective surfaces whereas the isostructural and isoelectronic silver-based AgBiX$_2$ and AgSbX$_2$ (X=Te, Se, S) series do not. We find that several Tl-compounds are in the vicinity of a topological critical point. We identify t…
We have synthesized tetragonal iron selenide and telluride superconductors through solid state reaction at 450deg.C and 550deg.C respectively. These synthesis temperatures have been established by optimization. Electrical resistivity and magnetic susceptibility measurements (4.2-300 K) confirm superconductivity with Tc of around 8.5 K in all selenide samples of nominal composition Fe1+deltaSe (delta=0.02-0.22). However, Scanning Electron Microscopy/ Energy Dispersive Spectroscopy studies clearly indicate that the actual stoichiometric ratio of Fe : Se for all the samples synthesized is around …
We have performed electrical resistivity measurements of a polycrystalline sample of FeSe$_{0.25}$Te$_{0.75}$, which exhibits superconductivity at $T_{\rm c} \sim 14$ K, in magnetic fields up to 55 T to determine the upper critical field $μ_{0}H_{\rm c2}$. In this compound, very large slopes of $μ_{0}H_{\rm c2}$ at the onset, the mid-point, the zero-resistivity temperatures on superconductivity are determined to be -13.7, -10.1, and -6.9 T/K, respectively. The observed $μ_{0}H_{\rm c2}(T)$s of this compound are considerably smaller than those expected from the Werthamer-Helfand-Hohenberg model…
In this review, we present a summary of the results on single crystal growth of two types of iron-chalcogenide superconductors, Fe(1+y)Te(1-x)Se(x) (11), and A(x)Fe(2-y)Se(2) (A= K, Rb, Cs, Tl, Tl/K, Tl/Rb), using Bridgman, zone-melting, vapor self-transport, and flux techniques. The superconducting and magnetic properties (the latter gained mainly from neutron scattering measurements) of these materials are reviewed to demonstrate the connection between magnetism and superconductivity. It will be shown that for the 11 system, while static magnetic order around the reciprocal lattice position …
Iron-chalcogenide superconductor Fe$_{1.03}$Se$_{0.5}$Te$_{0.5}$ has been investigated under high pressure using synchrotron based x-ray diffraction and mid-infrared reflectance measurements at room temperature. Pressure dependence of the superconducting transition temperature (T$_c$) of the same sample has been determined by temperature-dependent resistance measurements up to 10 GPa. Although the high pressure orthorhombic phase ($\textit{Pbnm}$) starts emerging at 4 GPa, structural transition becomes clearly observable above 10 GPa. A strong correlation is observed between the Fe(Se,Te)$_{4}…
The stability against quench is one of the main issue to be pursued in a superconducting material which should be able to perform at very high levels of current densities. Here we focus on the connection between the critical current $I_c$ and the quenching current $I^*$ associated to the so-called flux-flow instability phenomenon, which sets in as an abrupt transition from the flux flow state to the normal state. To this purpose, we analyze several current-voltage characteristics of three types of iron-based thin films, acquired at different temperature and applied magnetic field values. For t…
Coexistence of phases, characterized by different electronic degrees of freedom, commonly occurs in layered superconductors. Among them, alkaline intercalated chalcogenides are model systems showing microscale coexistence of paramagnetic (PAR) and antiferromagnetic (AFM) phases, however, temporal behavior of different phases is still unknown. Here, we report the first visualization of the atomic motion in the granular phase of K$_{x}$Fe$_{2-y}$Se$_2$ using X-ray photon correlation spectroscopy. Unlike the PAR phase, the AFM texture reveals an intermittent dynamics with avalanches as in martens…
The discovery of superconductivity in alkali-ammonia co-intercalated FeSe has generated intensive interest because of their highest Tc (~ 45 K) among iron-chalcogenide superconductors with bulk form. Here, we report the phase diagrams of two series of Li/Na-ammonia co-intercalated FeSe1-zTez. When superconductivity is suppressed by Te doping, the magnetic ordering states are emergent. Moreover, a novel phase Lix(NH3)yFe2-δTe2 with possible antiferromagnetism is discovered. This strongly indicates the intimate relation between superconductivity and magnetism in these materials, like in other ir…
The response of the worldwide scientific community to the discovery in 2008 of superconductivity at Tc = 26 K in the Fe-based compound LaFeAsO_{1-x}F_x has been very enthusiastic. In short order, other Fe-based superconductors with the same or related crystal structures were discovered with Tc up to 56 K. Many experiments were carried out and theories formulated to try to understand the basic properties of these new materials and the mechanism for Tc. In this selective critical review of the experimental literature, we distill some of this extensive body of work, and discuss relationships betw…
Interface-Induced Superconductivity in Magnetic Topological Insulator-Iron Chalcogenide Heterostructures
The Pennsylvania State University（宾夕法尼亚州立大学）；Rutgers University（罗格斯大学）；University of Washington（华盛顿大学）；Chinese Academy of Sciences（中国科学院）；Materials Research Institute, The Pennsylvania State University（宾夕法尼亚州立大学材料研究所）；National High Magnetic Field Laboratory（国家高磁场实验室）；Paul Scherrer Institute（保罗谢尔研究所）；National Institute of Standards and Technology（美国国家标准与技术研究院）
An SDW antiferromagnetic (SDW-AF) low temperature phase transition is generally observe and the AF spin fluctuations are considered to play an important role for the superconductivity paring mechanism in FeAs superconductors. However, a similar magnetic phase transition is not observed in FeSe superconductors, which has caused considerable discussion. We report on the intrinsic electronic states of FeSe as elucidated by transport measurements under magnetic fields using a high quality single crystal. A mobility spectrum analysis, an ab initio method that does not make assumptions on the transp…
Here, we theoretically predict that the series of Pb-based layered chalcogenides, Pb$_n$Bi$_2$Se$_{n+3}$ and Pb$_n$Sb$_2$Te$_{n+3}$, are possible new candidates for topological insulators. As $n$ increases, the phase transition from a topological insulator to a band insulator is found to occur between $n=2$ and 3 for both series. Significantly, among the new topological insulators, we found a bulk band gap of 0.40eV in PbBi$_2$Se$_4$ which is one of the largest gap topological insulators, and that Pb$_2$Sb$_2$Te$_5$ is located in the immediate vicinity of the topological phase boundary, making…
Rock-salt chalcogenide SnTe represents the simplest realization of a topological insulator where a crystal symmetry allows for the appearence of topologically protected metallic states with an even number of Dirac cones on high-symmetry crystal surfaces. Related rock-salt lead chalcogenides have been predicted as well to undergo a phase-transition to a topological crystalline insulating phase after band inversion induced by alloying and pressure. Here we theoretically predict that strain, as realized in thin films grown on (001) substrates, may induce such topological phase-transitions. Furthe…
Drastic field-induced resistivity upturns as signatures of unconventional magnetism in superconducting iron chalcogenides
University of Oxford（牛津大学）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Institute of High-Pressure Physics, Polish Academy of Sciences（波兰科学院高压物理研究所）；Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院量子材料与技术研究所）
Based on density functional theory (DFT), we investigate the electronic properties of bulk and single-layer ZrTe$_4$Se. The band structure of bulk ZrTe$_4$Se can produce a semimetal-to-topological insulator (TI) phase transition under uniaxial strain. The maximum global band gap is 0.189 eV at the 7\% tensile strain. Meanwhile, the Z$_2$ invariants (0; 110) demonstrate conclusively it is a weak topological insulator (WTI). The two Dirac cones for the (001) surface further confirm the nontrivial topological nature. The single-layer ZrTe$_4$Se is a quantum spin Hall (QSH) insulator with a band g…
By first-principles calculation based on the density functional theory (DFT) with the modified Becke-Johnson local density approximation plus Hubbard U (MBJLDA+U), we studied the band structures of the Yb chalcogenides YbO and YbS under ambient and high pressures. It was revealed that both YbO and YbS have a trivial band topology under ambient pressure, and a nontrivial band topology under high pressure. The topological phase transition is reduced by the pressure-driven single-band inversion between 5d- and 4f -orbitals at the time-reversal invariant momentum (TRIM) point X. A bulk Dirac cone …
We predict a new class of three dimensional topological insulators in thallium-based III-V-VI$_2$ ternary chalcogenides, including TlBiQ$_2$ and TlSbQ$_2$ (Q = Te, Se and S). These topological insulators have robust and simple surface states consisting of a single Dirac cone at the $Γ$ point. The mechanism for topological insulating behavior is elucidated using both first principle calculations and effective field theory models. Remarkably, one topological insulator in this class, TlBiTe$_2$ is also a superconductor when doped with $p$-type carriers. We discuss the possibility that this materi…
CaFeAs2 is a parent compound of recently discovered 112-type iron-based superconductors. It is predicted to be a staggered intercalation compound that naturally integrates both quantum spin Hall insulating and superconducting layers and an ideal system for the realization of Majorana modes. We performed a systematical angle-resolved photoemission spectroscopy and first-principle calculation study of the slightly electron-doped CaFeAs2. We found that the zigzag As chain of 112-type iron-based superconductors play a considerable role in the low-energy electronic structure, resulting in the chara…
The remarkable properties of graphene stem from its two-dimensional (2D) structure, with a linear dispersion of the electronic states at the corners of the Brillouin zone (BZ) forming a Dirac cone. Since then, other 2D materials have been suggested based on boron, silicon, germanium, phosphorus, tin, and metal di-chalcogenides. Here, we present an experimental investigation of a single silicon layer on Au(111) using low energy electron diffraction (LEED), high resolution angle-resolved photoemission spectroscopy (HR-ARPES), and scanning tunneling microscopy (STM). The HR-ARPES data show compel…
Binary bismuth chalcogenides Bi$_2$Se$_3$, Bi$_2$Te$_3$, and related materials are currently being extensively investigated as the reference topological insulators (TIs) due to their simple surface-state band dispersion (single Dirac cone) and relatively large bulk band gaps. Nanostructures of TIs are of particular interest as an increased surface-to-volume ratio enhances the contribution of surfaces states, meaning they are promising candidates for potential device applications. So far, the vast majority of research efforts have focused on the low-energy (0001) surfaces, which correspond to n…
A possible superconducting gap signature with filling temperature around 40 K in hexagonal iron telluride islands
Peking University（北京大学）；ShanghaiTech University（上海科技大学）；Quantum Science Center of Guangdong–Hong Kong–Macao Greater Bay Area (Guangdong)（粤港澳大湾区量子科学中心（广东））；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）；Hefei National Laboratory（合肥国家实验室）
The electronic structure of iron pnictides is topologically nontrivial, leading to the appearance of Dirac cones in the band structure for the antiferromagnetic phase. Motivated by the analogy with Dirac cones in graphene, we explore the possible existence of topologically protected surface states. Surprisingly, bands of surface states exist even in the paramagnetic state. A realistic five-orbital model predicts two such bands. In the antiferromagnetic phase, these surface bands survive but split. We obtain the bulk and surface dispersion from exact diagonalization of two- and five-orbital mod…
While in strongly correlated materials one often focuses on local electronic correlations, the influence of non-local exchange and correlation effects beyond band-theory can be pertinent in systems with more extended orbitals. Thus in many compounds an adequate theoretical description requires the joint treatment of local and non-local self-energies. Here, I will argue that this is the case for the iron pnictide and chalcogenide superconductors. As an approach to tackle their electronic structure, I will detail the implementation of the recently proposed scheme that combines the quasi-particle…
We have investigated several strong spin-orbit coupling ternary chalcogenides related to the (Pb,Sn)Te series of compounds. Our first-principles calculations predict the low temperature rhombohedral ordered phase in TlBiTe2, TlBiSe2, and TlSbX2 (X=Te, Se, S) to be topologically Kane-Mele Z2 = -1 nontrivial. We identify the specific surface termination that realizes the single Dirac cone through first-principles surface state computations. This termination minimizes effects of dangling bonds making it favorable for photoemission (ARPES) experiments. Our analysis predicts that thin films of thes…
The effect of Mn substitution, acting as a magnetic impurity for Fe, on the Dirac cone was investigated in Ba(Fe$_{1-x}$Mn$_x$As)$_2$. Both magnetoresistance and Hall resistivity studies clearly indicate that the cyclotron effective mass ($m^{\ast}$) of the Dirac cone is anomalously enhanced at low temperatures by the impurity, although its evolution as a function of carrier number proceeds in a conventional manner at higher temperatures. Kondo-like band renormalization induced by the magnetic impurity scattering is suggested as an explanation for this, and the anomalous mass enhancement of th…
