We have performed soft x-ray and ultrahigh-resolution laser-excited photoemission measurements on tetragonal FeSe, which was recently identified as a superconductor. Energy dependent study of valence band is compared to band structure calculations and yields a reasonable assignment of partial densities of states. However, the sharp peak near the Fermi level slightly deviates from the calculated energy position, giving rise to the necessity of self-energy correction. We have also performed ultrahigh-resolution laser photoemission experiment on FeSe and observed the suppression of intensity around the Fermi level upon cooling.
We prepared superconducting and non-superconducting FeSe films on SrTiO3(001) substrates (FeSe/STO) and investigated the superconducting transition induced by charge transfer between organic molecules and FeSe layers by low temperature scanning tunneling microscopy and spectroscopy. At low coverage, donor- and acceptor-type molecules adsorbed preferentially on the non-superconducting and superconducting FeSe layers, respectively. Superconductivity was induced by donor molecules on non-superconducting FeSe layer, while the superconductivity was suppressed near acceptor molecules. The correspond…
The electronic structure of FeSe thin films grown on SrTiO3 substrate is studied by angle-resolved photoemission spectroscopy (ARPES). We reveal the existence of Dirac cone band dispersions in FeSe thin films thicker than 1 Unit Cell below the nematic transition temperature, whose apex are located -10 meV below Fermi energy. The evolution of Dirac cone electronic structure for FeSe thin films as function of temperature, thickness and cobalt doping is systematically studied. The Dirac cones are found to be coexisted with the nematicity in FeSe, disappear when nematicity is suppressed. Our resul…
Iron selenide (FeSe) is an iron-based superconductor which shows unique properties, including strongly anisotropic superconducting gap, paramagnetism in undoped compound and extremely small Fermi pocket size. In this work, we demonstrate that the sizes of electron and hole pockets in FeSe monolayer become much smaller than those in bulk. The Fermi energy is in the order of a few meV and can be fine-tuned by the thickness of graphene layers underneath. Despite the low carrier density, the FeSe monolayers grown on trilayer or multi-layer graphene are superconducting. The superconducting gap size…
The recent observation of replica bands in single-layer FeSe/SrTiO$_3$ by angle-resolved photoemission spectroscopy (ARPES) has triggered intense discussions concerning the potential influence of the FeSe electrons coupling with substrate phonons on the superconducting transition temperature. Here we provide strong evidence that the replica bands observed in the single-layer FeSe/SrTiO$_3$ system and several other cases are largely due to the energy loss processes of the escaping photoelectron, resulted from the well-known strong coupling of external propagating electrons to Fuchs-Kliewer (F-K…
Single crystal synchrotron X-ray diffraction as a function of temperature and pressure has revealed a complex biphase mixture in superconducting FeSe. Based on our experimental results we construct a phase diagram where structural behavior and superconducting properties of FeSe are found to be correlated. We show that below 6 GPa, where pressure promotes the superconducting critical temperature, the FeSe structure is composed of 2D layers of edge-shared FeSe4 tetrahedra, while above 6 GPa the superconductivity is strongly suppressed on formation of a new orthorhombic polymorph characterized by…
In FeSe-derived superconductors, the lack of a systematic and clean control on the carrier concentration prevents the comprehensive understanding on the phase diagram and the interplay between different phases. Here by K dosing and angle resolved photoemission study on thick FeSe films and FeSe$_{0.93}$S$_{0.07}$ bulk crystals, the phase diagram of FeSe as a function of electron doping is established, which is extraordinarily different from other Fe-based superconductors. The correlation strength remarkably increases with increasing doping, while an insulting phase emerges in the heavily overd…
We investigated the microwave conductivity spectrum of FeSe$_{0.5}$Te$_{0.5}$ epitaxial films on CaF$_2$ in the vicinity of the superconducting transition. We observed the critical behavior of the superconducting fluctuations in these films with a dimensional crossover from two-dimensional to three-dimensional as the film thickness increased. From the temperature dependence of the scaling parameters we conclude that the universality class of the superconducting transition in FeSe$_{0.5}$Te$_{0.5}$ is that of the 3D-XY model. The lower limit of the onset temperature of the superconducting fluct…
This work reports studies performed in the superconducting compound FeSe0:5Te0:5 under high pressure. Changes were observed in the transition temperature, superconducting critical fields,anomalous variations in the Meissner fraction, and in Ginzburg Landau parameters. The superconducting properties were calculated and compared using the Werthamer-Helfand-Hohenber approximation and Ginzburg-Landau theory. Hydrostatic pressure was produced from atmospheric to 823 MPa, the increment in the critical temperature was from 14.45 to 20.5 K at a rate of change about 0.0069 K/MPa.
One of central issues in iron-based superconductors is the role of structural change to the superconducting transition temperature (T_c). It was found in FeSe that the lattice strain leads to a drastic increase in T_c, accompanied by suppression of nematic order. By angle-resolved photoemission spectroscopy on tensile- or compressive-strained and strain-free FeSe, we experimentally show that the in-plane strain causes a marked change in the energy overlap (DeltaE_{h-e}) between the hole and electron pockets in the normal state. The change in DeltaE_{h-e} modifies the Fermi-surface volume, lead…
The presumably unconventional superconductor Beta-FeSe was deposited by radio frequency sputtering and molecular beam epitaxy (MBE) from two elementary sources. Superconducting thin films were grown in (001)-orientation on MgO(100) and YAlO3(010) substrates. The morphology of the samples was studied and directly related to the superconducting properties of the Beta-FeSe thin films. The MBE grown thin films show microcracks down to the substrate and a roughness of about 100~nm. In contrast, sputter deposited superconducting thin films show a smooth surface with almost no precipitates. In both c…
Solvothermal intercalation of ethylenediamine molecules into FeSe separates the layers by 1078 pm and creates a different stacking. FeSe(en)0.3 is not superconducting although each layer exhibits the stripe-type crystal structure and the Fermi surface topology of superconducting FeSe. FeSe(en)0.3 requires electron-doping for high-Tc similar to monolayers of FeSe@SrTiO3, whose much higher Tc may arise from the proximity of the oxide surface.
We report comprehensive angle-resolved photoemission investigations on the electronic structure of single crystal multiple-layer FeSe films grown on CaF2 substrate by pulsed laser deposition (PLD) method. Measurements on FeSe/CaF2 samples with different superconducting transition temperatures Tc of 4 K, 9 K and 14 K reveal electronic difference in their Fermi surface and band structure. Indication of the nematic phase transition is observed from temperature-dependent measurements of these samples; the nematic transition temperature is 140-160 K, much higher than 90 K for the bulk FeSe. Potassi…
We study the consequences of an electron-phonon ($e$-$ph$) interaction that is strongly peaked in the forward scattering ($\mathbf{q} = 0$) direction in a two-dimensional superconductor using Migdal-Eliashberg theory. We find that strong forward scattering results in an enhanced $T_c$ that is linearly proportional to the strength of the dimensionless $e$-$ph$ coupling constant $λ_m$ in the weak coupling limit. This interaction also produces distinct replica bands in the single-particle spectral function, similar to those observed in recent angle-resolved photoemission experiments on FeSe monol…
Planar tunneling junctions of the presumably unconventional superconductor FeSe were prepared and investigated. The junctions consisted of FeSe/AlOx/Ag multilayers patterned lithographically into mesa structures. Bias voltage dependent differential conductivities dI/dV(V) of junctions in the tunneling, intermediate barrier strength, and metallic regimes were investigated. Depending on the barrier type between two and four features of the conductivity were obtained, which are discussed in the framework of multiple superconducting energy gaps. Specifically we reproduced with all barrier types an…
We present a systematic angle-resolved photoemission spectroscopy study of the superconducting gap in FeSe. The gap function is determined in a full Brillouin zone including all Fermi surfaces and kz-dependence. We find significant anisotropy of the superconducting gap in all momentum directions. While the in-plane anisotropy can be explained by both, nematicity-induced pairing anisotropy and orbital-selective pairing, the kz-anisotropy requires additional refinement of theoretical approaches.
The transition from insulator to superconductor was achieved in the non-superconducting FeSe ultrathin film via simple Mg coating technique in present work. It was found that in non-superconducting FeSe ultrathin film without Mg coating, insulating \b{eta}-Fe1-xSe phase with iron-vacancy disorders is the main phase and more likely to be the parent phase of FeSe superconducting system. Proper Mg coating on the surface of FeSe films can lead to Mg entering FeSe crystal lattice to fill up these Fe vacancies rather than replace Fe. Simultaneously, additional electron doping is introduced and the e…
We investigated the magnetization and crystal structure of FeSe polycrystalline samples with various grain sizes. For the samples with large grains, a large magnetic critical current density Jc was observed. For the samples with small grains, superconductivity signals were not observed; instead, magnetization hysteresis, which is not a result of superconductivity, was observed. In the X-ray diffraction pattern for the samples with small grains, broad additional peaks were observed, corresponding to the formation of the non-superconducting (monoclinic) Fe-Se phase at the FeSe grain surface. The…
Synthesis of monolayer FeSe on SrTiO3, with greatly enhanced superconductivity compared to bulk FeSe, remains difficult. Lengthy annealing within a certain temperature window is always required to achieve superconducting samples as reported by different groups around the world, but the mechanism of annealing in inducing superconductivity has not been elucidated. We grow FeSe films on SrTiO3 by molecular beam epitaxy and adjust the stoichiometry by depositing additional small amounts of Fe atoms. The monolayer films become superconducting after the Fe deposition without any annealing, and show …
A flux-free solution to the growth of large and composition homogeneous superconducting FeSe crystal is reported for the first time, which is based on the traveling-solvent floating-zone technique. The size of the crystal samples prepared by this approach is up to 15x6x2 mm3, being far bigger than previously reported in all dimensions, and the main phase of the crystals is of a single preferred orientation along the tetragonal (101) plane. X-ray diffraction analysis identifies the main phase to be the superconducting tetragonal \b{eta}-FeSe. The superconducting transition temperature (TC) is d…
Hexagonal FeSe thin films were grown on SrTiO3 substrates and the temperature and thickness dependence of their electronic structures were studied. The hexagonal FeSe is found to be metallic and electron doped, whose Fermi surface consists of six elliptical electron pockets. With decreased temperature, parts of the bands shift downward to high binding energy while some bands shift upwards to EF. The shifts of these bands begin around 300 K and saturate at low temperature, indicating a magnetic phase transition temperature of about 300 K. With increased film thickness, the Fermi surface topolog…
Point contact Andreev reflection studies have been conducted on FeSe single crystals by lowering the temperatures down to 0.5 K. The point contact Andreev reflection spectra were analyzed in the framework of the two-band model. As a result, the presence of two anisotropic superconducting gaps in FeSe were certainly established and their BCS-like temperature dependencies were obtained. The weights of each gap have been determined and the anisotropy parameter has been calculated. It is shown, that sub-kelvin temperatures are necessary to ascertain details of the superconducting gap structure, es…
Temperature (12K $\le$ T $\le$ 300K) dependent extended X-ray absorption fine structure (EXAFS) studies at the Fe K edge in FeSe$_{1-x}$Te$_x$ (x = 0, 0.5 and 1.0) compounds have been carried out to understand the reasons for increase in T$_C$ upon Te doping in FeSe. While local distortions are present near superconducting onset in FeSe and FeSe$_{0.5}$Te$_{0.5}$, they seem to be absent in non superconducting FeTe. Of crucial importance is the variation of anion height. In FeSe$_{0.5}$Te$_{0.5}$, near superconducting onset, the two heights, $h_{Fe-Se}$ and $h_{Fe-Te}$ show a nearly opposite be…
The microscopic mechanism governing the zero-resistance flow of current in some iron-based, high-temperature superconducting materials is not well understood up to now. A central issue concerning the investigation of these materials is their superconducting gap symmetry and structure. Here we present a combined study of low-temperature specific heat and scanning tunnelling microscopy measurements on single crystalline FeSe. The results reveal the existence of at least two superconducting gaps which can be represented by a phenomenological two-band model. The analysis of the specific heat sugge…
Our recent year's studies of the prototypal FeSe and molecule-intercalated (Li,Fe)OHFeSe superconductor systems are briefly reviewed here, with emphasis on experimental observations of the link between the superconductivity and normal-state electronic property in the single crystals and films. These samples were successfully synthesized by our recently developed soft-chemical hydrothermal methods, which are also briefly described. Particularly in the Mn-doped high-Tc (Li,Fe)OHFeSe film, a strong enhancement of the superconducting critical current density was achieved, which is promising for pr…
We report the successful growth of epitaxial thin films of FeSe$_{1-x}$S$_x$ with $x \leq 0.43$ via pulsed laser deposition. As S content increases, the nematic transition temperature, $T_{\mathrm s}$, decreases systematically and the superconducting transition temperature, $T_{\mathrm c}$, shows a gradual decrease even when $x$ exceeds the nematic end point (NEP), similar to bulk samples. A new kink anomaly was observed in the $ρ$-$T$ curves for films with large $x$, which is likely due to a magnetic transition. The obtained phase diagram of FeSe$_{1-x}$S$_x$ thin films is in contrast to that…
Using the self-consistent approximation we calculate conductivity in an anisotropic heterogeneous media with superconducting inclusions and compare the results with those obtained previously using the Maxwell approximation and with available experimental data on excess conductivity above $ T_c= $~8K in FeSe. Advantages and drawbacks of these two approximations are discussed. The obtained analytical formulas can be applied to various other anisotropic heterogeneous superconductors, including high-Tc layered superconductors.
High-resolution time- and angle-resolved photoemission measurements were made on FeSe superconductors. With ultrafast photoexcitation, two critical excitation fluences that correspond to two ultrafast electronic phase transitions were found only in the $d_{yz}$-orbit-derived band near the Brillouin-zone center within our time and energy resolution. Upon comparison to the detailed temperature dependent measurements, we conclude that there are two equilibrium electronic phase transitions (at approximately 90 and 120 K) above the superconducting transition temperature, and an anomalous contributi…
Systematic Comparison of Eight Substrates in the Growth of FeSe$_{0.5}$Te$_{0.5}$ Superconducting Thin Films
本文研究了在八种不同衬底上生长的FeSe $_{0.5}$ Te $_{0.5}$薄膜的晶体结构和超导性质。超导性与晶格失配无关，而是与面内取向程度和晶格参数比$c/a$相关。在MgO和LaAlOPDMATHABMO（$T_\mathrm{c}^\mathrm{zero}$为9.5 K）上的薄膜中观察到最好的超导性能。TEM观察表明，在衬底表面的非晶类层的存在或不存在起着关键作用，在确定的结构和超导性能的生长薄膜。
We investigated the influence of different Ag additions (up to 10 wt %) on the superconducting properties of FeSe0.94. The structural investigations (XRD and SEM) indicated that Ag is present in three different forms. Ag at grain boundaries supports the excellent intergrain connections and reduces superconducting transition width to values smaller than 1K at B=0 and smaller than 2.74 K at B=14 T. Ag insertion in the crystal lattice unit cell provides additional carriers and changes the electron hole imbalance in FeSe0.94. This results in an increase in the magnetoresistive effect (MR) and crit…
We present direct measurements of the superconducting order parameter in nearly optimal FeSe$_{0.5}$Te$_{0.5}$ single crystals with critical temperature $T_C \approx 14$ K. Using intrinsic multiple Andreev reflection effect (IMARE) spectroscopy and measurements of lower critical field, we directly determined two superconducting gaps, $Δ_L \approx 3.3 - 3.4$ meV and $Δ_S \approx 1$ meV, and their temperature dependences. We show that a two-band model fits well the experimental data. The estimated electron-boson coupling constants indicate a strong intraband and a moderate interband interaction.
We report the superconductivity evolution of one unit cell (1-UC) and 2-UC FeSe films on SrTiO3(001) substrates with potassium (K) adsorption. By in situ scanning tunneling spectroscopy measurement, we find that the superconductivity in 1-UC FeSe films is continuously suppressed with increasing K coverage, whereas non-superconducting 2-UC FeSe films become superconducting with a gap of ~17 meV or ~11 meV depending on whether the underlying 1-UC films are superconducting or not. This work explicitly reveals that the interface electron-phonon coupling is strongly related to the charge transfer a…
We investigate the local density of states in the vicinity of a native dumbbell defect arising from an Fe vacancy in FeSe single crystals. The tunneling spectra close to the impurity display two bound states inside the superconducting gap, equally spaced with respect to zero energy but asymmetric in amplitude. Using spin-polarized density functional theory (DFT) calculations on realistic slab models with Fe vacancy, we show that such a defect does not induce a local magnetic moment. Therefore, the dumbbell defect is considered as non-magnetic. Thus, the in-gap bound states emerging from a non-…
We report on the emergence of two disconnected superconducting domes in alkali-metal potassium (K)-doped FeSe ultra-thin films grown on graphitized SiC(0001). The superconductivity exhibits hypersensitivity to K dosage in the lower-Tc dome, whereas in the heavily electron-doped higher-Tc dome it becomes spatially homogeneous and robust against disorder, supportive of a conventional Cooper-pairing mechanism. Furthermore, the heavily K-doped multilayer FeSe films all reveal a large superconducting gap of ~ 14 meV, irrespective of film thickness, verifying the higher-Tc superconductivity only in …
We investigated the superconducting fluctuation in FeSe, which is assumed to be located in the BCS--BEC crossover region, via magnetic torque measurements. In our method, the absolute cantilever displacement is measured by detecting the interference intensity of the Fabry--Perot cavity formed between the cantilever and optical fiber. Our findings are totally different from the results of the previous torque magnetometry using a piezoresistive cantilever; the "giant" fluctuation diamagnetism related to the BCS--BEC crossover does not exist. Instead, a considerably smaller fluctuation signal ori…
In this study, we investigated the gate voltage dependence of $T_{\mathrm c}$ in electrochemically etched FeSe films with an electric-double layer transistor structure. The $T_{\mathrm c}^{\mathrm {zero}}$ value of the etched FeSe films with a lower gate voltage ($V_{\mathrm g}$ = 2.5 and 3.3 V) reaches 46 K, which is the highest value among almost all reported values from the resistivity measurements except for the data by Ge et al. This enhanced $T_{\mathrm c}$ remains unchanged even after the discharge process, unlike the results for electrostatic doping without an etching process. Our resu…
Tetragonal beta-FeSe obtained by hydrothermal reaction is not superconducting and transforms to a triclinic structure at 60 K unlike superconducting FeSe from solid state synthesis, which becomes orthorhombic at 90 K. In contrast, tetragonal iron sulphide FeS from hydrothermal synthesis is superconducting at 4.8 K but undergoes no structural transition. Our results suggest that the absence of superconductivity in hydrothermally synthesized FeSe may be associated to the low-temperature structure with zigzag chains of iron atoms, which is different from the known orthorhombic Cmme structure of s…
We investigate the electronic reconstruction across the tetragonal-orthorhombic structural transition in FeSe by employing polarization-dependent angle-resolved photoemission spectroscopy (ARPES) on detwinned single crystals. Across the structural transition, the electronic structures around the G and M points are modified from four-fold to two-fold symmetry due to the lifting of degeneracy in dxz/dyz orbitals. The dxz band shifts upward at the G point while it moves downward at the M point, suggesting that the electronic structure of orthorhombic FeSe is characterized by a momentum-dependent …
