We measure the electronic structure of FeSe from within individual orthorhombic domains. Enabled by an angle-resolved photoemission spectroscopy beamline with a highly focused beamspot (nano-ARPES), we identify clear stripe-like orthorhombic domains in FeSe with a length scale of approximately 1-5~$μ$m. Our photoemission measurements of the Fermi surface and band structure within individual domains reveal a single electron pocket at the Brillouin zone corner. This result provides clear evidence for a one-electron pocket electronic structure of FeSe, observed without the application of uniaxial strain, and calls for further theoretical insight into this unusual Fermi surface topology. Our results also showcase the potential of nano-ARPES for the study of correlated materials with local domain structures.
Superconductivity originates from pairing of electrons. Pairing channel on Fermi surface and pairing glue are thus two pivotal issues for understanding a superconductor. Recently, high-temperature superconductivity over 40 K was found in electron-doped FeSe superconductors including K$_x$Fe$_{2-y}$Se$_2$, Li$_{0.8}$Fe$_{0.2}$OHFeSe, and 1 monolayer FeSe thin film. However, their pairing mechanism remains controversial. Here, we studied the systematic evolution of electronic structure in potassium-coated FeSe single crystal. The doping level is controlled precisely by in situ evaporating potass…
School of Physics and Astronomy, University of St. Andrews（圣安德鲁斯大学物理与天文学院）；Institute of Physics, University of Greifswald（格赖夫斯瓦尔德大学物理研究所）；Diamond Light Source（钻石光源）
The origin of spontaneous electronic nematic ordering provides important information for understanding iron-based superconductors. Here, we analyze a scenario where the $d_{xy}$ orbital strongly contributes to nematic ordering in FeSe. We show that the addition of $d_{xy}$ nematicity to a pure $d_{xz}/d_{yz}$ order provides a natural explanation for the unusual Fermi surface and correctly reproduces the strongly anisotropic momentum dependence of the superconducting gap. We predict a Lifshitz transition of an electron pocket mediated by temperature and sulphur doping, whose signatures we discu…
High-Tc pairing mechanism absent of hole-pockets in heavily electron-doped FeSe is one of the key unsolved problems in Fe-based superconductors. Here, this problem is attacked by focusing on the higher-order many-body effects neglected in conventional Migdal-Eliashberg formalism. We uncover two significant many-body effects for high-Tc superconductivity: (i) Due to the "vertex correction", the dressed multiorbital Coulomb interaction acquires prominent orbital dependence for low-energy electrons. The dressed Coulomb interaction not only induces the orbital fluctuations, but also magnifies the …
We report high resolution ARPES measurements of detwinned FeSe single crystals. The application of a mechanical strain is used to promote the volume fraction of one of the orthorhombic domains in the sample, which we estimate to be 80$\%$ detwinned. While the full structure of the electron pockets consisting of two crossed ellipses may be observed in the tetragonal phase at temperatures above 90~K, we find that remarkably, only one peanut-shaped electron pocket oriented along the longer $a$ axis contributes to the ARPES measurement at low temperatures in the nematic phase, with the expected po…
We measured the electronic-structure of FeSe_xTe_1-x above and below Tc. In the normal state we find multiple bands with remarkably small values for the Fermi energy, E_F. Yet,below Tc we find a superconducting gap, Delta, that is comparable in size to E_F, leading to a ratio Delta/E_F~0.5 that is much larger than found in any previously studied superconductor. We also observe an anomalous dispersion of the coherence peak which is very similar to the dispersion found in cold Fermi-gas experiments and which is consistent with the predictions of the BCS-BEC crossover theory.
The electronic structure of the enigmatic iron-based superconductor FeSe has puzzled researchers since spectroscopic probes failed to observe the expected electron pocket at the $Y$ point in the 1-Fe Brillouin zone. It has been speculated that this pocket, essential for an understanding of the superconducting state, is either absent or incoherent. Here, we perform a theoretical study of the preferred nematic order originating from nearest-neighbor Coulomb interactions in an electronic model relevant for FeSe. We find that at low temperatures the dominating nematic components are of inter-orbit…
We have studied the structural and superconducting properties of tetragonal FeSe under pressures up to 26GPa using synchrotron radiation and diamond anvil cells. The bulk modulus of the tetragonal phase is 28.5(3)GPa, much smaller than the rest of Fe based superconductors. At 12GPa we observe a phase transition from the tetragonal to an orthorhombic symmetry. The high pressure orthorhombic phase has a higher Tc reaching 34K at 22GPa.
The coupling between superconductivity and othorhombic distortion is studied in vapor-grown FeSe single crystals using high-resolution thermal-expansion measurements. In contrast to the Ba122-based (Ba122) superconductors, we find that superconductivity does not reduce the orthorhombicity below Tc. Instead we find that superconductivity couples strongly to the in-plane area, which explains the large hydrostatic pressure effects. We discuss our results in light of the spinnematic scenario and argue that FeSe has many features quite different from the typical Fe-based superconductors.
FeSe, despite being the structurally simplest compound in the family of iron-based superconductors, shows an astoundingly rich interplay of physical phenomena including nematicity and pressure-induced magnetism. Here, we present a microscopic study of these two phenomena by high-energy x-ray diffraction and time-domain Mössbauer spectroscopy on FeSe single crystals over a wide temperature and pressure range. The topology of the pressure-temperature phase diagram is a surprisingly close parallel to the well-known doping-temperature phase diagram of BaFe2As2 generated through partial Fe/Co and B…
The nature of the tetragonal-to-orthorhombic structural transition at $T_s\approx90$ K in single crystalline FeSe is studied using shear-modulus, heat-capacity, magnetization and NMR measurements. The transition is shown to be accompanied by a large shear-modulus softening, which is practically identical to that of underdoped Ba(Fe,Co)$_2$As$_2$, suggesting very similar strength of the electron-lattice coupling. On the other hand, a spin-fluctuation contribution to the spin-lattice relaxation rate is only observed below $T_s$. This indicates that the structural, or "nematic", phase transition …
To understand the nematicity in Fe-based superconductors, nontrivial $k$-dependence of the orbital polarization ($ΔE_{xz}(k)$, $ΔE_{yz}(k)$) in the nematic phase, such as the sign reversal of the orbital splitting between $Γ$- and X,Y-points in FeSe, provides significant information. To solve this problem, we study the spontaneous symmetry breaking with respect to the orbital polarization and spin susceptibility self-consistently. In FeSe, due to the sign-reversing orbital order, the hole- and electron-pockets are elongated along the $k_y$- and $k_x$-axes respectively, consistently with experi…
In the iron-based superconductors, understanding the relation between superconductivity and electronic structure upon doping is crucial for exploring the pairing mechanism. Recently it was found that in iron selenide (FeSe), enhanced superconductivity (Tc over 40K) can be achieved via electron doping, with the Fermi surface only comprising M-centered electron pockets. Here by utilizing surface potassium dosing, scanning tunneling microscopy/spectroscopy (STM/STS) and angle-resolved photoemission spectroscopy (ARPES), we studied the electronic structure and superconductivity of (Li0.8Fe0.2OH)Fe…
We reproduce the electronic properties of FeSe in the high-temperature phase within an ab initio framework that includes screened Fock exchange and local dynamical correlations. We robustly capture the experimental band structure, as long as the system is in the Hund's metal phase. In particular, we account for the shrinking of the Fermi pockets and the sinking below the Fermi level of the hole pocket with $xy$ orbital character. This entails the elusive correct estimate of the Sommerfeld coefficient, and supports the interpretation of non-compensated Fermi pockets seen in ARPES in terms of su…
Neutron and x-ray total scattering measurements have been performed on powder samples of the iron chalcogenide superconductor FeSe. Using pair distribution function (PDF) analysis of the total scattering data to investigate short-range atomic correlations, we establish the existence of an instantaneous, local orthorhombic structural distortion attributable to nematic fluctuations that persists well into the high-temperature tetragonal phase, at least up to 300 K and likely to significantly higher temperatures. This short-range orthorhombic distortion is correlated over a length scale of about …
The field and temperature dependencies of the longitudinal and Hall resistivity have been measured for FeSe${}_{1-x}$S${}_{x}$ (x=0.04, 0.09 and 0.19) single crystals. The sample FeSe${}_{0.81}$S${}_{0.19}$ does not show a transition to an orthorhombic phase and exhibits at low temperatures the transport properties quite different from those of orthorhombic samples. The behavior of FeSe${}_{0.81}$S${}_{0.19}$ is well described by the simple two band model with comparable values of hole and electron mobility. In particular, at low temperatures the transverse resistance shows a linear field depe…
We study the structure of the d-wave orbital order in FeSe in light of recent STM and ARPES data, which detect the shapes of hole and electron pockets in the nematic phase. The geometry of the pockets indicates that the sign of the orbital order $Γ= \langle d^{\dagger}_{xz} d_{xz}- d^{\dagger}_{yz} d_{yz}\rangle$ is different between hole and electron pockets $(Γ_h$ and $Γ_e$). We argue that this sign change cannot be reproduced if one solves for the orbital order within mean-field approximation, as the mean-field analysis yields either no orbital order, or order with the same sign of $Γ_e$ an…
The FeSe nematic phase has been the focus of recent research on iron based superconductors (IBSs) due to its unique properties. A number of electronic structure studies were performed to find the origin of the phase. However, such attempts came out with conflicting results and caused additional controversies. Here, we report results from angle resolved photoemission and X-ray absorption spectroscopy studies on FeSe with detwinning by a piezo stack. We have fully resolved band dispersions with orbital characters near the Brillouin zone corner which reveals absence of a Fermi pocket at the Y poi…
FeSe undergoes a transition from a tetragonal to a slightly orthorhombic phase at 90\,K, and becomes a superconductor below 8\,K. The orthorhombic phase is sometimes called a nematic phase because quantum oscillation, neutron, and other measurements detect a significant asymmetry in $x$ and $y$. How nematicity affects superconductivity has recently become a matter of intense speculation. Here we employ an advanced \emph{ab-initio} Green's function description of superconductivity and show that bulk tetragonal FeSe would, in principle, superconduct with almost the same T$_{c}$ as the nematic ph…
Superconductivity emerges in proximity to a nematic phase in most iron-based superconductors. It is therefore important to understand the impact of nematicity on the electronic structure. Orbital assignment and tracking across the nematic phase transition prove to be challenging due to the multiband nature of iron-based superconductors and twinning effects. Here, we report a detailed study of the electronic structure of fully detwinned FeSe across the nematic phase transition using angle-resolved photoemission spectroscopy. We clearly observe a nematicity-driven band reconstruction involving d…
We study superconducting FeSe (Tc = 9 K) exhibiting the tetragonal-orthorhombic structural transition (Ts = 90 K) without any antiferromagnetic ordering, by utilizing angle-resolved photoemission spectroscopy. In the detwinned orthorhombic state, the energy position of the dyz orbital band at the Brillouin zone corner is 50 meV higher than that of dxz, indicating the orbital order similar to NaFeAs and BaFe2As2 families. Evidence of orbital order also appears in the hole bands at the Brillouin zone center. Precisely measured temperature dependence using strain-free samples shows that the onset…
Single-layer FeSe films with extremely expanded in-plane lattice constant of 3.99A are fabricated by epitaxially growing FeSe/Nb:SrTiO3/KTaO3 heterostructures, and studied by in situ angle-resolved photoemission spectroscopy. Two elliptical electron pockets at the Brillion zone corner are resolved with negligible hybridization between them, indicating the symmetry of the low energy electronic structure remains intact as a free-standing single-layer FeSe, although it is on a substrate. The superconducting gap closes at a record high temperature of 70K for the iron based superconductors. Intrigu…
A rich variety of nematic/smectic orders in Fe-based superconductors is an important unsolved problem in strongly correlated electron systems. A unified understanding of these orders has been investigated for the last decade. In this article, we explain the $B_{1g}$ symmetry nematic transition in FeSe$_{1-x}$Te$_x$, the $B_{2g}$ symmetry nematicity in AFe$_2$As$_2$ (A=Cs, Rb), and the smectic state in BaFe$_2$As$_2$ based on the same framework. We investigate the quantum interference mechanism between spin fluctuations by developing the density wave equation. The observed rich variety of nemat…
The pairing glue of high-$T_{\rm c}$ superconductivity in heavily electron-doped (e-doped) FeSe, in which hole-pockets are absent, has been an important unsolved problem. Here, we focus on a heavily e-doped bulk superconductor Li$_{1-x}$Fe$_x$OHFeSe ($T_{\rm c} \sim 40$K). We construct a multiorbital model beyond the rigid band approximation and analyze the spin and orbital fluctuations by taking both vertex corrections (VCs) and self-energy into consideration. Without e-doping ($x=0$), the ferro-orbital order without magnetism in FeSe is reproduced by the VCs.The orbital order quickly disappe…
We use density functional theory to study the structure and the band structure of the monolayer FeSe deposited on the SrTiO$_3$ substrate with the additional layer of Se between them. Top of the SrTiO$_3$ is formed by the double TiO layer with and without oxygen vacancies. Several structures with different arrangements of the additional Se atoms above the double TiO layer is considered. Equilibrium structures were found and the band structures for them were obtained. Near the $Γ=(0,0,0)$ point of the Brillouin zone, the hole Fermi surface pockets persist and, additionally, an electron pocket a…
We study the crystal structure of the tetragonal iron selenide FeSe and its nematic phase transition to the low-temperature orthorhombic structure using synchrotron x-ray and neutron scattering analyzed in both real and reciprocal space. We show that in the local structure the orthorhombic distortion associated with the electronically driven nematic order is more pronounced at short length scales. It also survives up to temperatures above 90 K where reciprocal-space analysis suggests tetragonal symmetry. Additionally, the real-space pair distribution function analysis of the synchrotron x-ray …
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…
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…
Simultaneous high pressure x-ray diffraction and electrical resistance measurements have been carried out on a PbO type α-FeSe0.92 compound to a pressure of 44 GPa and temperatures down to 4 K using designer diamond anvils at synchrotron source. At ambient temperature, a structural phase transition from a tetragonal (P4/nmm) phase to an orthorhombic (Pbnm) phase is observed at 11 GPa and the Pbnm phase persists up to 74 GPa. The superconducting transition temperature (TC) increases rapidly with pressure reaching a maximum of ~28 K at ~ 6 GPa and decreases at higher pressures, disappearing comp…
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…
Magnetoresistivity \r{ho}xx and Hall resistivity \r{ho}xy in ultra high magnetic fields up to 88T are measured down to 0.15K to clarify the multiband electronic structure in high-quality single crystals of superconducting FeSe. At low temperatures and high fields we observe quantum oscillations in both resistivity and Hall effect, confirming the multiband Fermi surface with small volumes. We propose a novel and independent approach to identify the sign of corresponding cyclotron orbit in a compensated metal from magnetotransport measurements. The observed significant differences in the relativ…
An exact particle-hole transformation is discovered in a local-moment model for a single layer of heavily electron-doped FeSe. The model harbors hidden magnetic order between the iron d_xz and d_yz orbitals at the wavenumber (pi,pi). It potentially is tied to the magnetic resonances about the very same Neel ordering vector that have been recently discovered in intercalated FeSe. Upon electron doping, the local-moment model successfully accounts for the electron-pocket Fermi surfaces observed experimentally at the corner of the two-iron Brillouin zone in electron-doped FeSe, as well as for isot…
We report pair distribution function measurements of the iron-based superconductor FeSe above and below the structural transition temperature. Structural analysis reveals a local orthorhombic distortion with a correlation length of about 4 nm at temperatures where an average tetragonal symmetry is observed. The analysis further demonstrates that the local distortion is larger than the distortion at temperatures where the average observed symmetry is orthorhombic. Our results suggest that the low-temperature macroscopic nematic state in FeSe forms from an imperfect ordering of orbital-degenerac…
There is growing evidence that the superconducting semimetal FeSe ($T_c\sim8$ K) is in the crossover regime between weak-coupling Bardeen-Cooper-Schrieffer (BCS) and strong-coupling Bose-Einstein-condensate (BEC) limits. We report on longitudinal and transverse thermal conductivities, $κ_{xx}$ and $κ_{xy}$, respectively, in magnetic fields up to 20 T. The field dependences of $κ_{xx}$ and $κ_{xy}$ imply that a highly anisotropic small superconducting gap forms at the electron Fermi-surface pocket whereas a more isotropic and larger gap forms at the hole pocket. Below $\sim1.0$ K, both $κ_{xx}$…
We report the results of our in-depth analysis of spectroscopic and thermodynamic properties of a multi-orbital metal, like FeSe, which first develops a nematic order and then undergoes a transition into a superconducting state, which co-exists with nematicity. We analyze the angular dependence of the gap function and specific heat $C_V (T)$ of such nematic superconductor. We specifically address three issues: (i) angular dependence of the gap in light of the competition between nematicity-induced $s$-$d$ mixture and orbital transmutation of low-energy excitations in the nematic state, (ii) th…
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 …
We compute the compressibility of the conduction electrons in both bulk orthorhombic FeSe and monolayer FeSe on SrTiO$_3$ substrate, including dynamical electronic correlations within slave-spin mean-field + density-functional theory. Results show a zone of enhancement of the electronic compressibility crossing the interaction-doping phase diagram of these compounds in accord with previous simulations on iron pnictides and in general with the phenomenology of Hund's metals. Interestingly at ambient pressure FeSe is found slightly away from the zone with enhanced compressibility but moved right…
We use scanning tunneling spectroscopy to investigate the filled and empty electronic states of superconducting single-unit-cell FeSe deposited on SrTiO$_3$(001). We map the momentum-space band structure by combining quasiparticle interference imaging with decay length spectroscopy. In addition to quantifying the filled-state bands, we discover a $Γ$-centered electron pocket 75 meV above the Fermi energy. Our density functional theory calculations show the orbital nature of empty states at $Γ$ and suggest that the Se height is a key tuning parameter of their energies, with broad implications f…
We use high-resolution angle-resolved photoemission spectroscopy to map the three-dimensional momentum dependence of the superconducting gap in FeSe. We find that on both the hole and electron Fermi surfaces, the magnitude of the gap follows the distribution of $d_{yz}$ orbital weight. Furthermore, we theoretically determine the momentum dependence of the superconducting gap by solving the linearized gap equation using a tight binding model which quantitatively describes both the experimental band dispersions and orbital characters. By considering a Fermi surface only including one electron po…
We have performed high-resolution angle-resolved photoemission spectroscopy on FeSe superconductor (Tc ~ 8 K), which exhibits a tetragonal-to-orthorhombic structural transition at Ts ~ 90 K. At low temperature we found splitting of the energy bands as large as 50 meV at the M point in the Brillouin zone, likely caused by the formation of electronically driven nematic states. This band splitting persists up to T ~ 110 K, slightly above Ts, suggesting that the structural transition is triggered by the electronic nematicity. We have also revealed that at low temperature the band splitting gives r…
Iron chalcogenide superconductors are multi-band systems with strong electron correlations. Here we use angle-resolved photoemission spectroscopy to study band dependent correlation effects in single-layer FeSe/Nb:BaTiO3/KTaO3, a new iron chalcogenide superconductor with non-degenerate electron pockets and interface-enhanced superconductivity. The non-degeneracy of the electron bands helps to resolve the temperature dependent evolution of different bands. With increasing temperature, the single layer FeSe undergoes a band-selective localization, in which the coherent spectral weight of one ele…
The origin of enhanced superconductivity over 50 K in the recently discovered FeSe monolayer films grown on SrTiO$_{3}$ (STO), as compared to 8 K in bulk FeSe, is intensely debated. As with the ferrochalcogenides A$_{x}$Fe$_{2-y}$Se$_{2}$ and potassium doped FeSe, which also have a relatively high superconducting critical temperature ($T_c$), the Fermi surface (FS) of the FeSe/STO monolayer films is free of hole-like FS, suggesting that a Lifshitz transition by which these hole FSs vanish may help increasing $T_c$. However, the fundamental reasons explaining this increase of $T_c$ remain uncle…
Strain is a powerful experimental tool to explore new electronic states and understand unconventional superconductivity. Here, we investigate the effect of uniaxial strain on the nematic and superconducting phase of single crystal FeSe using magnetotransport measurements. We find that the resistivity response to the strain is strongly temperature dependent and it correlates with the sign change in the Hall coefficient being driven by scattering, coupling with the lattice and multiband phenomena. Band structure calculations suggest that under strain the electron pockets develop a large in-plane…
We provide a band structure with low-energy properties consistent with recent photoemission and quantum oscillations measurements on FeSe, assuming mean-field like s and/or d-wave orbital ordering at the structural transition. We show how the resulting model provides a consistent explanation of the temperature dependence of the measured Knight shift and the spin-relaxation rate. Furthermore, the superconducting gap structure obtained from spin fluctuation theory exhibits nodes on the electron pockets, consistent with the 'V'-shaped density of states obtained by tunneling spectroscopy on this m…
We report on the structural phase transitions in the S doped FeSe superconductor by powder synchrotron X ray diffraction at high pressures up to 18.5 GPa under compression and decompression modes. In order to create high quasi hydrostatic pressures, diamond anvil cells filled with helium as a pressure transmitting medium were used. It was found that at ambient pressure and room temperature, S doped FeSe has a tetragonal structure. Under compression, in the region of 10 GPa, a phase transition from the tetragonal into the orthorhombic structure is observed, which persists up to 18.5 GPa. Our re…
FeSe is a fascinating superconducting material at the frontier of research in condensed matter physics. Here we provide an overview on the current understanding of the electronic structure of FeSe, focusing in particular on its low energy electronic structure as determined from angular resolved photoemission spectroscopy, quantum oscillations and magnetotransport measurements of single crystal samples. We discuss the unique place of FeSe amongst iron-based superconductors, being a multi-band system exhibiting strong orbitally-dependent electronic correlations and unusually small Fermi surfaces…
Superconductivity in FeSe has recently attracted a great deal of attention because it emerges out of an electronic nematic state of elusive character. Here we study both the electronic normal state and the superconducting gap structure using heat-capacity measurements on high-quality single crystals. The specific-heat curve, from 0.4 K to Tc = 9.1 K, is found to be consistent with a recent gap determination using Bogoliubov quasiparticle interference [P. O. Sprau et al., Science 357, 75 (2017)], however only if nodes are introduced on either the electron or the hole Fermi-surface sheets. Our a…
We report on the synthesis of superconducting single crystals of FeSe, and their characterization by X-ray diffraction, magnetization and resistivity. We have performed ac susceptibility measurements under high pressure in a hydrostatic liquid argon medium up to 14 GPa and we find that TC increases up to 33-36 K in all samples, but with slightly different pressure dependences on different samples. Above 12 GPa no traces of superconductivity are found in any sample. We have also performed a room temperature high pressure X-ray diffraction study up to 12 GPa on a powder sample, and we find that …
We review a variety of theoretical and experimental results concerning electronic band structure of superconducting materials based on FeSe monolayers. Three type of systems are analyzed: intercalated FeSe systems A_xFe_2Se_{2-x}S_x and [Li_{1-x}Fe_xOH]FeSe as well as the single FeSe layer films on SrTiO_3 substrate. We present the results of detailed first principle electronic band structure calculations for these systems together with comparison with some experimental ARPES data. The electronic structure of these systems is rather different from that of typical FeAs superconductors, which is…
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…
We report the evolution of the electronic nematic susceptibility in FeSe via Raman scattering as a function of hydrostatic pressure up to 5.8 GPa where the superconducting transition temperature $T_{c}$ reaches its maximum. The critical nematic fluctuations observed at low pressure vanish above 1.6 GPa, indicating they play a marginal role in the four-fold enhancement of $T_{c}$ at higher pressures. The collapse of nematic fluctuations appears to be linked to a suppression of low energy electronic excitations which manifests itself by optical phonon anomalies at around 2 GPa, in agreement with…
A polycrystalline sample of FeSe, which adopts the tetragonal PbO-type structure (P4/nmm) at room temperature, has been prepared using solid state reaction. We have investigated pressure-induced structural changes in tetragonal FeSe at varying hydrostatic pressures up to 0.6 GPa in the orthorhombic (T = 50 K) and tetragonal (T = 190 K) phases using high resolution neutron powder diffraction. We report that the structure is quite compressible with a Bulk modulus around 31 GPa to 33 GPa and that the pressure response is anisotropic with a larger compressibility along the c-axis. Key bond angles …
Iron pnictides are the only known family of unconventional high-temperature superconductors besides cuprates. Until recently, it was widely accepted that superconductivity is spin-fluctuation driven and intimately related to their fermiology, specifically, hole and electron pockets separated by the same wave vector that characterizes the dominant spin fluctuations, and supporting order parameters (OP) of opposite signs. This picture was questioned after the discovery of a new family, based on the FeSe layers, either intercalated or in the monolayer form. The critical temperatures there reach ~…
The accurate theoretical description of the underlying electronic structures is essential for understanding the superconducting mechanism of iron-based superconductors. Compared to bulk FeSe, the superconducting single-layer FeSe/SrTiO3 films exhibit a distinct electronic structure consisting of only electron Fermi pockets, due to the formation of a new band gap at the Brillouin zone (BZ) corners and an indirect band gap between the BZ center and corners. Although intensive studies have been carried out, the origin of such a distinct electronic structure and its connection to bulk FeSe remain …
To understand the rich electronic phase diagram in FeSe under pressure that vividly demonstrates the strong interplay between the nematicity, magnetism and superconductivity, we analyze the electronic states by including the higher-order many-body effects called the vertex correction (VC). We predict the pressure-induced emergence of xy-orbital hole-pocket based on the first-principles analysis. Due to this pressure-induced Lifshitz transition, the spin fluctuations on the xy orbital are enhanced, whereas those on xz,yz orbitals are gradually reduced. For this reason, nonmagnetic orbital order…
The band structure and the Fermi surface of the recently discovered superconductor (EMIM)$_x$FeSe are studied within the density functional theory in the generalized gradient approximation. We show that the bands near the Fermi level are formed primarily by Fe-$d$ orbitals. Although there is no direct contribution of EMIM orbitals to the near-Fermi level states, the presence of organic cations leads to a shift of the chemical potential. It results in the appearance of small electron pockets in the quasi-two-dimensional Fermi surface of (EMIM)$_x$FeSe.
The electronic structure and magnetism of a new magnetic intercalation compound (Li0.8Fe0.2)OHFeSe are investigated theoretically. The electronic structure calculations predict that the Fe in the (Li,Fe)OH intercalated layer is in +2 valence state, i.e. there is electron doping to the FeSe layer, resulting in the shrinking of the Fermi surface (FS) pocket around Gamma and a strong suppression of dynamical spin susceptibility at M in comparison with the bulk FeSe compound. The ground state of the FeSe layer is a striped antiferromagnetic (SAFM) metal, while the (Li,Fe)OH layer displays a very w…
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…
We present temperature-dependent in-plane resistivity measurements on FeSe single crystals under He-gas pressure up to 800 MPa and magnetic fields $B \leq$ 10 T. A sharp phase transition anomaly is revealed at the tetragonal-to-orthorhombic transition at $T_s$ slightly below 90 K. $T_s$ becomes reduced with increasing pressure in a linear fashion at a rate d$T_{s}$/d$P$ $\simeq$ -31 K/GPa. This is accompanied by a $P$-linear increase of the superconducting transition temperature at $T_c \sim$ 8.6 K with d$T_{c}$/d$P$ $\simeq$ +5.8 K/GPa. Pressure studies of the normal-state resistivity highlig…
We report a high-resolution angle-resolved photo-emission spectroscopy study of the evolution of the electronic structure of FeSe1-xSx single crystals. Isovalent S substitution onto the Se site constitutes a chemical pressure which subtly modifies the electronic structure of FeSe at high temperatures and induces a suppression of the tetragonal-symmetry-breaking structural transition temperature from 87K to 58K for x=0.15. With increasing S substitution, we find smaller splitting between bands with dyz and dxz orbital character and weaker anisotropic distortions of the low temperature Fermi sur…
